TW201004993A - Modified resin composition, method for producing same and curable resin composition containing same - Google Patents

Abstract

The present invention provides a modified resin composition obtained by reacting an epoxy resin (A) and an alkoxysilane compound represented by the following formula (1): (R1)n-Si-(OR2)4-n (1)The alkoxysilane compound contains the following (B) and (C): (B) at least one alkoxysilane compound having at least one cyclic ether group for R1, wherein n = 1 or 2; (C) at least one alkoxysilane compound having at least one aromatic organic group for R1, wherein n=1 or 2. The mixed index α of the alkoxysilane compound represented by the following formula (2) is equal to or more than 0. 001 and equal to or less than 19; and the remaining amount of alkoxyl group in the modified resin composition is equal to or less than 5%. The mixed index α = (α c)/(α b) (2)

Description

201004993 6. Technical Field of the Invention The present invention relates to a modified resin composition obtained by reacting an epoxy resin with an alkoxylated compound, and a method for producing the same, and relates to a composition containing the same A curable resin composition and its use. [Prior Art] - The epoxy resin composition using an acid anhydride-based hardener provides a transparent cured product, and is suitable for use as a light-emitting diode because of its high heat resistance and adhesion. : Sealing of optical semiconductors such as exposure diodes (Ph«e) === In recent years, the performance of optical semiconductors has been increasing. Therefore, as a resin for LED sealing, in addition to the high heat and adhesion required in the past, In the case of the heat, the light resistance, and the hardening of the cracking (the ckiness) in the case of the heat cycle, the surface is viscous. The stone oxime oxygen regulation ^ is a review of the study of the aerobic (Xianzhan) resin of the Xuxi. The work of the compound stone is excellent for lightness or heat resistance, but then the stone is used for the moon. Peeling, and sometimes the hardness of the hardened material has a non-satisfactory performance, so in fact, it is still necessary to add more J, etc., and on the other hand, many are being carried out to repeat the stone (4) 321346 4 2010049 93 Research on the modified resin composition containing an epoxy group in the mono- and t-organic groups. The composition of the modified resin is not only provided with an excellent transparent heat of epoxy resin and a non-adhesive surface. In addition, it is expected that the cured product has the light resistance and oxidation resistance possessed by oxygen, and further has flexibility. For example, Patent Document 1 proposes a modified resin composition containing a T structure. It is necessary to repeat the unit, and the content of the organic group containing an epoxy group is in the range of Ο" to 40 mol% with respect to the combination of the φ 原子 atom and the ρ organic group in one molecule. A molecular weight having a specific range: a composition of a polyoxo compound having at least two epoxy groups in = and a utilization of the (four) material in an optical semiconductor sealing material. Condensation: to 5 is disclosed in relation to epoxy resin and A resin composition obtained by mixing a 'oxygen resin'. In Patent Documents 6 to η, it is disclosed that the stone is sintered or its partial heart pa η* and the base lipid composition. Dehydration reaction The number is a resin composition of a modified phenoxy tree in which the number of alkoxy groups contained in the molecule is twice that of the S! atomic group. [Patent Document] (Patent Document 1) Japanese Patent Laid-Open No. Hei. No. Hei. No. Hei. No. 2006-225515 (Patent Document 3). Japanese Patent Laid-Open Publication No. Hei. No. Hei. No. 2006-225515 No. 321346 5 201004993 (Patent Document 4) (Patent Document 5) (Patent Document 6) (Patent Document 7) (Patent Document 8) (Patent Document 9) (Patent Document 10) (Patent Document 11) (Patent Document 12) [Summary of the Invention]

曰本特开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开开Japanese Patent Application Laid-Open No. Hei. No. Hei. No. Hei. No. Hei. No. Hei. Resin composition, lack of obscurity's about crack resistance and adhesion have not yet reached a satisfactory level. Further, the above-mentioned modified resin composition tends to have low storage stability, and the viscosity of the resin tends to increase remarkably during storage, and it can be said that it has sufficient resilience. + In addition, in the absence of the epoxy resin described in Patent Documents 3 to 5, the composition of the pre-condensed material Oxygen and the Wei tree m AM is stored in Angulow, in the storage towel_丝There will be a significant increase in the degree of ^ ^ 'sometimes 'epoxy resin and poly-resin resin will not be able to evenly mix and so on, can not be said to have sufficient practicality. The de-alcoholization reaction of Putian to 'have a tendency to remain in the polyoxanium when it is agglomerated with oxygen." For example, it is dedicated to the hardening of the tree containing the alkaloids (10). The hardened material is vaporized by the hydrolysis of the organic solvent at the time of 321346 6 201004993, so that the crack resistance or the adhesion property during the thermal cycle tends to decrease. In view of the above facts, an object of the present invention is to provide a modified resin composition having good storage stability, which can be formed to have good transparency, and has excellent heat resistance, heat discoloration resistance, light resistance, and heat cycle. A hardened material that is resistant to cracking. Further, an object of the present invention is to provide an excellent LED or the like which is excellent in adhesion to an element or a packaging material, which does not cause cracking, and which has a small decrease in brightness over a long period of time, or can be injection molded and hardened. Then, it is an optical lens which is hard, has excellent dimensional stability, and has light resistance, and a semiconductor device using the above-described light-emitting component and/or optical lens. Further, an object of the present invention is to provide a photosensitive composition which is excellent in adhesiveness which can suppress polymerization inhibition by oxygen, a coating agent containing the composition, and a coating film obtained by curing the coating agent. . Further, an object of the present invention is to provide a fluorescent resin composition excellent in dispersion stability of a phosphor and a light-storing material using the fluorescent resin composition. Further, an object of the present invention is to provide a conductive resin composition which is excellent in fluidity, electrical conductivity, and adhesion and which does not generate voids. Further, an object of the present invention is to provide an insulating resin composition which is excellent in fluidity, insulation, and adhesion and which does not cause voids. (Means for Solving the Problem) The inventors of the present invention have found that the epoxy resin and the specific alkoxydecane compound are reacted at a specific ratio of 7 321 346 201004993 in order to solve the above problems. The present invention can be solved by adjusting the amount of residual activating oxygen in the active fat composition to a specific level. That is, the present invention is as follows: [1] A modified resin composition obtained by reacting an epoxy resin with a non-alkoxydecane compound of the following general formula (1) to form a modified fat composition , ❹

(R)n~ Si — (OR2)4-11 (1) (wherein η represents an integer of 3 or more in 〇; further, R1 independently represents a hydrogen atom, and is selected from the following &) to C) At least one or more organic groups in a group: a) an aliphatic hydrocarbon having one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, and cyclic groups And an organic group having a cyclic ether group composed of a carbon number of 4 or more and 24 or less and an oxygen atom number of 1 or more and 5 or less; b) having a chain-like or branched shape selected from unsubstituted or substituted And an aliphatic tobacco unit composed of one or more types of structures in a ring-shaped structure, and a monovalent aliphatic organic group having a carbon number of 1 or more and 24 or less and an oxygen atom number of 5 or more; c) An unsubstituted or substituted aromatic hydrocarbon unit, and if desired, an aliphatic group composed of one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, and cyclic groups a monovalent aromatic organic group having a carbon number of 6 or more and 24 or less and an oxygen atom number of 5 or more; 321346 8 2010049 On the other hand, R2 each independently represents a hydrogen atom and one or more organic groups selected from the group consisting of d) below: d) having a chain-like or branched form selected from unsubstituted or substituted groups And an aliphatic hydrocarbon unit which has one or more types of structures in a cyclic structure, and a monovalent organic group having a carbon number of 1 or more and 8 or less; the alkoxydecane compound contains the following (β) and (c): (Β) η = 1 or 2 and having at least one cyclic ether group as at least one alkoxydecane compound of R1, and

(C) n=l "2 and at least one aromatic organic group as at least one alkoxydecane compound; the following general formula (2) shows that the mixing index α of the previous oxy (tetra) compound is 0. 〇〇1 or more 19 or less. Mixed index 〇: =( α c) / ( α b) (2) (In the formula (2), ab represents the content of the above-mentioned (8) component in the alkoxydecane compound represented by the general formula (1) -he represents a general The content (mol%) of the above-mentioned component (6) in the oxy-xanthene compound represented by the formula (1); and the residual amount of the residual oxy group in the modified resin composition is [2] modified as described above. In the resin composition, the viscosity of the modified resin composition at 25 ° C is i〇〇〇pa · 卜 卜. The modified tree assay of the above (1) or [2], wherein the modified resin composition has an epoxy equivalent of from 100 g/eq to 7 or less. The modified resin composition of any one of the above-mentioned items (1) to [3] wherein the alkoxydecane compound has a condensation ratio of 8% by mass or more. [5] : On! The modified resin composition according to any one of (1) to (4) wherein the epoxy resin (4) has a viscosity of 5 〇〇Pa·s or less at 25t. [6] The modified resin composition of any one of the above (1) to [5] wherein the epoxy equivalent of the epoxy resin (1) is not less than 3 Åg / eq. [7] The modified resin composition according to any one of (1) to [6] wherein the epoxy resin (A) is a polyfunctional epoxy resin composed of a glycidyl etherate of a polyphenol compound. . [8] The modified resin composition according to any one of [1] to [7] wherein the epoxy resin (A) is a bisphenol A type epoxy resin. The above-mentioned composition of the alkoxydecane compound represented by the following general formula (3) is a coldness of 0.01 or more. 1.4 or less: ❹ Mixed index { (; 5n2) / (cold n〇 + ^ nl)} (3) (In the formula (3), the stone η2 represents the alkoxy sinter compound represented by the general formula (1) The content (m〇i%) of the alkoxy sinter compound of η=2, and 10,000 nO represents the content of the oxydecane compound of n=〇 in the alkoxydecane compound represented by the general formula (1) (mol%) 'βηΐ represents the content (mol%) of the alkoxy group compound of η=1 in the alkoxydecane compound represented by the general formula (1), and the above values satisfy the following formula: 〇$ U々n0 ) / (々n0+ /3nl+ ygn2)}g〇. 1). [10] The modified resin composition according to any one of the above [1] to [9], wherein: 321346 10 201004993, the epoxy resin (a) represented by the following general formula (4) and the aforementioned alkoxylate The mixing index y of the compound of the compound is 〇. 02 to 15 : mixing index 7 = ( 7 * a) / ( T s) (4) (in this 'formula (4) ' ra table epoxy resin (a) The mass (g), *Ts represents the mass (g) of the alkoxydecane compound having n = 〇 to 2 in the alkoxy oxime compound represented by the general formula (1). [11] A method for producing a modified resin composition, which comprises at least (B) & (C) represented by the following general formula (1) in the presence of an epoxy resin (A) A method for producing a modified resin composition according to any one of the above [1] to [1], wherein the method comprises the following steps (a) and (b): a) Step: in the presence of the epoxy resin (A), at least the alkoxydecane compound of the formula (B) and (C) represented by the formula (1) is subjected to a reflux step without dehydration. J £ (hydrolysis) to produce an intermediate step; 0 (b) step: the step of dehydration condensation reaction of the intermediate produced in step (a); (R)) n-Si - (〇R2Vn (1) (wherein η represents an integer of 3 or more and 整数 or more; and R1 each independently represents a hydrogen atom, at least one or more organic groups selected from the group consisting of 3) to c): a) An aliphatic hydrocarbon unit composed of one or more kinds of structures of a chain-like, branched, or cyclically formed structure which is unsubstituted or substituted, and contains a carbon number of 4 or more and 24 or less And oxygen atom 321346 11 201004993 The number is an organic group of a cyclic ether group composed of 1 or more and 5 or less; b) having a structure group selected from a chain, a branch, and a ring selected from unsubstituted or substituted An aliphatic hydrocarbon unit composed of one or more kinds of structures, and a monovalent aliphatic organic group having a carbon number of 1 or more and 24 or less and an oxygen atom number of 0 or more and 5 or less; c) an unsubstituted or substituted aromatic group a hydrocarbon unit and, if necessary, a fatty steroid hydrocarbon unit composed of one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, or cyclic structures, and having a carbon number of 6 or more and 24 or less and a monovalent aromatic organic group having an oxygen atom number of 0 or more and 5 or less; on the other hand, R2 each independently represents a hydrogen atom, and one or more organic groups selected from the group consisting of d) : d) an aliphatic hydrocarbon unit having one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, or cyclic groups, and having a carbon number of 1 or more and 8 or less a monovalent organic group), q (B) n = 1 or 2 and having at least one cyclic ether group as at least R1 An alkoxydecane compound; (C) at least one alkoxydecane compound having at least one aromatic organic group as R1; and the alkane represented by the following general formula (2); The mixing index α of the oxydecane compound is 0.001 or more and 19 or less: the mixing index a = ( ac) / ( ab) (2) (here, in the formula (2), ab represents the above component (B) The content (mol%), ac represents the content (mol%) of the above component (C). 12 321346 201004993 [12] A method for producing a modified resin composition, which comprises at least (B) and (C) represented by the following general formula (1) in the presence of an epoxy resin (A) The method for producing the modified resin composition according to any one of the above [1] to [10], wherein the method comprises the following steps (c) and (d): Step: a step of producing an intermediate by at least alkoxydecane compound of (B) and (C) represented by the general formula (1) by co-hydrolysis without a reflux step with dehydration; β (d) Step: in the intermediate produced by the step (c), the epoxy resin (A) is allowed to coexist, and the step of dehydration condensation reaction is carried out; (R')n-Si-(0R2)4-n (1) ( Here, η represents an integer of 0 or more and 3 or less; and R1 each independently represents a hydrogen atom, at least one or more organic groups selected from the group consisting of a) to c): a) having a selected from An aliphatic hydrocarbon unit composed of one or more kinds of structures of a chain group, a branched form, or a ring-shaped φ group which are not substituted or substituted, and contains a carbon number of 4 or more and 24 And an organic group of a cyclic ether group having an oxygen atom number of 1 or more and 5 or less; b) having a structure group selected from a chain, a branch, and a ring selected from unsubstituted or substituted An aliphatic hydrocarbon unit having a structure of at least one of the above, and a monovalent aliphatic organic group having a carbon number of 1 or more and 24 or less and an oxygen atom number of 0 or more and 5 or less; c) an unsubstituted or substituted aromatic hydrocarbon unit And, if necessary, a fat-free hydrocarbon monoterpene composed of one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, and ring 13 321 346 201004993, and carbon number The valence-free aromatic organic group of 6 or more and 24 or less and the number of oxygen atoms is 〇 or more and 5 or less. In addition, R 2 each independently represents a chlorine atom, and one or more organic groups selected from the group consisting of d) Base: d) an aliphatic hydrocarbon unit 7G having one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, or cyclic groups, and having a carbon number of 1 or more and 8 The following valence organic group), (B) n=l or 2 and at least one cyclic ether group as at least R1 An alkoxydecane compound; (C) at least one alkoxydecane compound having n = 1 or 2 and having at least one aromatic organic group; and the alkane represented by the following general formula (2) The mixing index α of the oxydecane compound is 0. 〇〇1 or more and 19 or less: the mixing index a = ( ac) / ( ab) (2) _ (in the 'formula (2)' ab represents the aforementioned (B) The content of the component (mol%), ac represents the content of the above component (C) (m〇i%)). [13] The method for producing a modified resin composition according to the above [11] or [12], wherein the mixing index yS of the alkoxydecane compound represented by the following general formula (3) is from 0.01 to 1.4, a mixing index β={(;3η2)/(βη0+ySnl)} (3) (In the formula (3), 泠n2 represents an alkoxy group of n=2 in the compound of the compound of the formula (1). The content of the decyl group compound (m〇i%), β nO represents the content (mol%) of the 14 321 346 201004993 oxy-shi Shi Yuan compound of n=0 in the alkoxy oxime compound represented by the general formula (1), / 3nl represents the content (mol%) of the oxyl dreaming compound of n=1 in the non-sintered calcined compound of the general formula (i), and the lines satisfy the following formula: OS {(3n0)/ (/5n0 + y5nl+ ySn2)}$〇. 1). [14] The method for producing a modified resin composition according to any one of the above [1] to [13], wherein the epoxy resin (A) represented by the following general formula (4) and the alkoxylate described above The mixing index τ of the alkane compound is 〇. 〇2 to 15 : mixing index 7 = ( ra) / ( 7 s) (4) (In the formula (4), γ a represents the mass of the epoxy resin (A) (g), rs represents the mass (g) of the alkoxylated compound of n=〇 to 2 in the alkoxydecane compound represented by the general formula (丨). [15] The method of the modified resin composition according to any one of the above [π] to [14] wherein the temperature in the reflux step without dehydration is from 50 to 100 t. [16] = the above-mentioned method of the composition of the modified composition of the above-mentioned [(1) to the towel, wherein the condensation ratio of the intermediate obtained by co-hydrolysis without a reflux step with dehydration is 78% or more . [17] The method for producing a modified resin composition according to any one of the above [U] to (10), wherein in the co-hydrolysis, a sintering oxide (aIk〇Xide)-based organotin is used as a catalyst. . (10): a lipid composition obtained by modifying the resin composition of the above (1): a compound: oxetane (.) compound (9). Planting: ί, a composition, which is formed in the modified tree wax of the above [1], and is formed by adding a human phosphor (8). 321346 15 201004993 [20] A conductive resin composition obtained by adding a conductive metal powder (F) to the above-mentioned [n modified resin composition]. [21] An insulating resin composition obtained by adding an insulating powder (G) to the modified resin composition of the above [丨]. [22] A resin composition obtained by adding an epoxy resin (A,) to the modified resin composition of the above [丨]. [23] A curable resin composition obtained by adding a curing agent (H) to the resin composition according to any one of the above [A], [18], or [19]. [24] A curable resin composition obtained by adding a curing accelerator (I) to the resin composition of the above [23]. [25] A photosensitive resin composition obtained by adding a photo-acid generator to a resin composition according to any one of the above [丨], [18], or [19] (J) ). [26] A light-emitting component obtained by using the resin composition of the above [24] or [25]. 27 [27] An optical lens obtained by using the resin compositions of the above [24] and [25]. [28] A light-storing material obtained by using the resin composition of the above [24] or [25]. [29] A semiconductor device comprising the light-emitting component of the above [26] and/or the optical lens of the above [27]. [30] A curable resin composition obtained by adding the curing accelerator (I) to the resin composition according to any one of the above [2] to [22]. [31] A photosensitive resin composition obtained by adding a photoacid generator (j) to a resin composition according to any one of the above [2〇] to [22], which is a compound of 16321346 201004993. [32] A coating composition comprising the resin composition according to any one of the above [24], [25], [30], or [31]. A coating film obtained by using the coating agent of the above [32]. (Effect of the Invention) According to the present invention, it is possible to provide a modified tree having excellent storage stability, which can form a cured product having excellent light resistance and thermal shock resistance (thermal crack resistance). * [Embodiment] The following describes the mode for carrying out the invention (hereinafter, referred to as ",,,,,,,,,,,"). The present invention is not limited to the form shown below. Only the modified resin composition in the shape of the sorrow is a modified resin composition obtained by reacting an epoxy group (A) and an alkoxy oxime compound represented by the following formula (1), vR )n — Si — (OR )4-n

Q (wherein 'n represents an integer of 0 or more and 3 or less; and 'R each independently represents a hydrogen atom, and at least one organic group selected from the group consisting of a) to c): a) = a group of hydrocarbons consisting of a structure selected from the group consisting of unsubstituted or substituted chains, branches, and rings, and having two or more structures, and having 3 carbon atoms of 4 or more and 24 or less The number of atoms and the organic group of the cyclic ether group constituted by the above; (1) or more and 5) b) having one or more structures selected from the group consisting of unsubstituted or substituted chain-like or branch-inhibiting structures Aliphatic furnace-like composition 17 321346 201004993 201004993 The aliphatic group having a carbon number of 1 or more and 24 or less and having an oxygen atom number of 0 or more; c) having an unsubstituted or substituted (IV) unit has a The structure of one or more types of chains or groups of groups that are substituted or substituted, the number of straight breaks is 6 or more and 24 or less, and the number of gas atoms is an aromatic organic group; In the aspect, R2 is independently derived from + _, 乂 也 also represents a hydrogen atom, and is selected from the following d) The group: d) has a monovalent organic group consisting of a structure selected from the group consisting of unsubstituted or substituted chain, branched, or cyclically branched structure groups, and having a carbon number of 1 or more and 8 or less) , wherein the anterior oxyphyllin (8) n = 1:2 and has at least one cyclic, dialkoxy decane compound; and one ❹ (C) n = 1 or 2 and at least one type of oxygen burning (four) Burning compound; $々 organic group as R at least the following general formula (2) indicates the arrow index Xie. 19 mixed Weiwei Wei compound mixed mixing index a = (ac) / (α μ ) (2) ( In the formula (2), ' _ab indicates the content of the above-mentioned component (B) in the addition of (B) (In〇^(1), which is not in the oxy-stone compound, and the above-mentioned two-zero in the alkoxy compound And aC is not in the general formula (1) and 'the content of the component in the modified resin composition (m〇1%)); the amount of residual alkoxy group of T is 5% or less. 321346 18 201004993 is used in this embodiment The epoxy resin (A) is not particularly limited, and examples thereof include an alicyclic epoxy resin, an aliphatic epoxy resin, and glycidol from a polyphenol compound. A polyfunctional epoxy resin composed of an ether compound, a polyfunctional epoxy resin belonging to a glycidyl ether compound of a novolac resin, a nuclear hydride of an aromatic epoxy resin, a heterocyclic epoxy resin, or a glycidyl group An ester epoxy resin, a glycidyl amine epoxy resin, an epoxy resin obtained by glycidylating a halogenated phenol, etc., and these epoxy resins may be used singly or in combination. (tricyclodecene oxide) The alicyclic epoxy resin which can be used in the present embodiment is not particularly limited as long as it is an epoxy resin having an alicyclic epoxy group. For example, it has a cyclohexene oxidation. (cycl〇hexene〇xide)*, three-cyclopentene oxide II? Pentene oxide based epoxy resin. Specific examples of the alicyclic epoxy t-ester As the monofunctional alicyclic epoxy compound, epoxy hexahydrodicarboxylic acid dioctyl ester and epoxy hexamethylene phthalate-2-ethylhexanoic acid may be mentioned. . β •^j~ τ*·, ifia . As a 2-functional alicyclic epoxy compound,

Monoterpene epoxide, lanthanum fluorenyl hydrazide, ethyl bis (3,4 epoxide ring such as: 4-vinyl epoxy cyclohexane 3, oxygen. (3, ring J Ester, ethyl alcohol II (3, 19 201004993 hexane carboxylate), 1,2, 8, 9-diepoxylimene (1,2, 8, 9-diepoxylimonene), etc. as a multifunctional alicyclic epoxy The compound may, for example, be a 1,2-epoxy-4-(2-cyclohexene)cyclohexene adduct of 2,2-bis(hydroxymethyl)-1-butanol. In addition, as a commercial product of the polyfunctional alicyclic type oxy-compound, eP0LEAD GT401, EHPE 3150 (made by DaiCel Chemical Industry Co., Ltd.), etc. are shown. example.

201004993

The aliphatic epoxy resin which can be used in the present embodiment is not particularly limited, and specific examples thereof include 1,4-butanediol, 1,6-hexanediol, polyethylene glycol, and poly A glycidyl ether of a polyhydric alcohol such as propylene glycol, pentaerythritol or xylylene glycol derivative. The following is a representative example of an aliphatic epoxy resin. 21 321346 201004993

The polyfunctional epoxy resin composed of a polyglycidyl ether compound of a compound which can be used in the present embodiment is not particularly limited, and specific examples thereof include: double age A, double expectant F, double test S , 4, 4'-linked (4, 4'-biphenol), tetramethyl bis-A, dimethyl bisphenol A, tetradecyl bisphenol F, dimethyl bisphenol F, tetramethyl bisphenol S, dimethyl bisphenol S, tetra ◎ methyl 4-, 4'-biphenol, dimercapto-4, 4'-biphenol ((^11^7, 4'-biphenylphenol), 1-(4-Phenylphenyl)-2-[4-(1,1-bis-(4-pyridylphenyl)ethyl)phenyl]propane, 2, 2'-methylene-bis- (4-methyl-6-tert-butylphenol), 4,4'-butylene-bis(3-mercapto-6-tert-butylphenol), trisylphenylpyrene, isophthalic acid Resorcinol, hydrogen brewing, 2,6-di(t-butyl) hydrogen brewing, arsenic (?71'〇8811〇1), phenols with diisopropylene backbone, 1,1- a polyfunctional epoxy resin having a phenolic phenolic compound such as bis(4-hydroxyphenyl)anthracene or a phenolic phenolic polybutadiene compound, such as a glycidyl group-compound. Representative examples of the backbone of the phenolic glycidyl ether compounds of multifunctional epoxy resins.] 346 201 004 993 22 32

When a polyfunctional cyclic oxime resin which is a glycidyl ether compound of a polyphenol compound is used, the repeating unit (n in the chemical formula of the above representative example) is not particularly limited, and the range of 0 or more and less than 50 is good. When the repeating unit is 50 or more, the fluidity is lowered, and there is a problem in practical use. From the viewpoint of improving the reactivity with the alkoxylated compound, from the viewpoint of improving the fluidity of the obtained modified resin composition, the range of the repeating unit is 0.001 or more and 10 or less. Preferably, it is preferably in the range of 1 or more and 2 or less.多 The polyfunctional epoxy resin which is a glycidyl ether compound of a phenol resin is not particularly limited, and examples thereof include phenol, cresol, ethyl phenol, butyl phenol, and octyl phenol. a phenolic resin containing various phenols such as bisphenol A, bisphenol F, bisphenol S, and naphthol as raw materials; a phenol novolac resin containing xylylene backbone, and a backbone containing dicyclopentadiene A variety of phenolic-based conversion resins such as resin, a biphenyl-containing age-old resin, and a phenolic phenolic resin such as a sacral phenolic resin are used. The following is a representative example of a polyfunctional cycloolefin resin which is a glycidyl group of an acid anhydride. 321346 23 201004993 PS PS 涔 CH-0 CH-0 CH-€ 0Λ 0Λ 0Λ

The nuclear hydride of the aromatic epoxy resin which can be used in the present embodiment is not particularly limited, and examples thereof include a hydrazine compound (biguanide A, bisphenol F, bisphenol S, 4, 4'-linked). Glycidyl etherate of phenol, etc.; various phenols (phenols, phenols, ethyl phenols, butyl phenols, octyl phenols, bisphenol A, bisphenol F, bisphenol S, naphthols) a nuclear hydride of an aromatic ring; or a nuclear hydride of a glycidyl etherate of a phenol resin. The heterocyclic epoxy resin is not particularly limited, and examples thereof include a heterocyclic epoxy resin having a hetero ring such as an isocyanuric ring or a hydantoin ring. The glycidyl ester-based epoxy resin is not particularly limited, and examples of the compound Q include a hexahydrophthalic acid diglycidyl group, a tetrahydro arsenic acid diglycidyl ester, and the like. Epoxy resin, etc. The glycidylamine-based epoxy resin is not particularly limited, and examples thereof include aniline, indoleamine, p-phenylenediamine, m-phenylenediamine, diaminodiphenylmethane derivative, and diaminol group. An epoxy resin obtained by glycidylating an amine such as a benzene derivative. The epoxy resin obtained by glycidylation of a halogenation is not particularly limited, and examples thereof include brominated double age A, desertification double test F, brominated bisphenol S, and brominated phenol novolac. Bromophenol phenolic phenol, gasified bisphenol S, gas 24 321346 201004993 The phenolic phenols such as bisphenol A are glycidyl etherified and epoxy eucalyptus. In the above, the cured product obtained by curing the modified resin composition in the form of the present silver is easily obtained, and has excellent transparency, heat resistance, heat discoloration resistance, light resistance, and It is preferable to use a polyfunctional epoxy tree raft composed of an alicyclic epoxy resin, an aliphatic epoxy resin, or a polyglycidyl ether compound of a polyphenol compound in the tendency of the thermal cycle. An alicyclic epoxy resin, a polyfunctional epoxy resin composed of a glycidol® ether compound of a polyphenol compound, preferably a polyfunctional epoxy resin composed of a polyglycidyl ether compound: More preferably, the double age A type epoxy resin is particularly good. The adhesiveness of the epoxy resin (A) used in the present embodiment is limited to 25 t: but the compatibility with the alkoxylate compound is improved in order to ensure the fluidity of the liquid. Therefore, it is preferable to use a liquid below the surface s, preferably 5 kPa or less, preferably better than $ Q, and preferably 100 Pa·s or less. Regarding the epoxy resin (A) of the epoxy resin (A) used in the present embodiment, and the 'restriction of the special J', the viewpoint of the qualitative property of the modified resin composition of the present embodiment is It is preferable to increase the cleavage property of the cured product obtained by curing the modified resin composition in the form of 1 〇〇g/eq or more, preferably 7 〇〇g//eq or less. It is preferable that the range of 5 〇〇g/eq or less is (10) or more, and it is more preferably in the range of seq. q or more and g/eq or less. The alkoxy-based compound which can be used in the embodiment refers to an anthracene compound having 25 321 346 201004993 1 to 4 alkoxy groups, which is expressed by the following general formula (1). (R!)n - Si - (OR )4-n (1) (wherein η represents an integer of 0 or more and 3 or less; further, R1 independently represents a hydrogen atom, and is selected from the following a) ^ c) At least one or more organic groups in a group: a) an aliphatic hydrocarbon having one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, and cyclic groups The grass element, 箕 contains an organic group having a ring-shaped engraving group composed of a carbon number of 4 or more and 24 or less and an oxygen atom number of i or more and 5 to the underarm; b) having a chain selected from unsubstituted or substituted, An aliphatic tobacco unit composed of one or more types of structures in a branched or cyclic structure; and a monovalent aliphatic organic group having a carbon number of 1 or more and 24 or less and an oxygen atom number of 5 or more and 5 or less; c) having an unsubstituted or substituted aromatic hydrocarbon unit, and having one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, and cyclic groups, if necessary The aliphatic hydrocarbon unit having a carbon number of 6 or more and 24 or less and an oxygen atomic number of 5 or less and a valence aromatic organic group, and R2 is independently The site represents a hydrogen atom and one or more organic groups selected from the group consisting of: d) having one of a chain group selected from the group consisting of unsubstituted or substituted chain, branched, and soiled The aliphatic hydrocarbon unit having the above structure is a monovalent organic group having a carbon number of 1 or more and 8 or less. The cyclic ether group in the present embodiment will be described. The base of the capital is 321346 26 201004993 The cyclic bond group is an organic base that has the carbon atom of the tobacco-like smoke replaced by an oxygen atom. It has 3 to 6 members. The cyclic bond group of the ring structure, wherein 'the ring-shaped secret of the 3-membered ring or the 4-membered ring with large ring strain energy and high reactivity is better', especially the ring-shaped test base of the 3-membered ring is better. In the present embodiment, f is a hydrogen atom, and at least one organic group selected from the group consisting of a) to c) below: a) having an organic group selected from the group consisting of a) An aliphatic hydrocarbon unit composed of an unsubstituted or substituted chain, branched or cyclic group of H 1 or more structures, and having a carbon number of 4 or more and 24 or less and an oxygen atom number of i or more An organic group having a cyclic acid group consisting of ruthenium; b) an aliphatic hydrocarbon having one or more structures selected from the group consisting of unsubstituted or substituted touch, material, and cyclic a unit, and a monovalent aliphatic organic group having a carbon number of 1 or more and 24 or less and an oxygen atom number of 5 or less, c) having no substitution or being An aromatic hydrocarbon unit, and if necessary, an aliphatic smoke unit composed of one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, and cyclic structures And an i-valent aromatic organic group having a carbon number of 6 or more and 24 or less and an oxygen atom number of 5 or more and 5 or less. The above a) has a chain, a branch, or a ring selected from the group consisting of unsubstituted or substituted. For example, the organic base having a cyclic ether group composed of a carbon number of 4 or more and 24 or less and an oxygen atom number of 2 or more and the following may be contained in the structure of one or more types of the structural group. List: 泠~ shrinking water 27 321346 201004993 Oxy-ethyloxyethyl (r-cilycidoxyethyl), r, glycidyloxypropyl, 7-glycidyloxybutyl, etc. Glycidyloxyalkyl group bonded by glyceryl group; glycidyl group, stone-(3,4-epoxycyclohexyl)ethyl, τ-(3,4-epoxycyclohexyl)propyl, stone- (3,4-epoxycycloheptyl)ethyl, s-(3,4-epoxycyclohexyl)propyl, s-(3,4-epoxycyclohexyl)butyl, - (3, 4-epoxycyclohexyl)pentyl group or the like having an oxirane group substituted with a cycloalkyl group having 5 to 8 carbon atoms, etc. The above b) has a selected from An aliphatic hydrocarbon unit composed of one or more types of structures of a chain, a branched, or a cyclic group which are unsubstituted or substituted, and having a carbon number of 1 or more and 24 or less and an oxygen atom number of 0 or more and 5 or less The monovalent aliphatic organic group may, for example, be (b-fluorene)methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutylene tert-butyl, second butyl, n-pentyl Base, isopentyl, neopentyl, n-hexyl n-heptyl, octyl, decyl, decyl, undecyl, dodecane, Q, dodecacarb, tetradecyl burn, a fifteen-carbon alkyl group, a hexadecanocarbon, a hexadecyl group, an octadecyl group, or the like, which is composed of an aliphatic hydrocarbon, a bond (b-2) cyclopentyl group, a methylcyclopentyl group, a cyclohexyl group, An organic group consisting of a hydrocarbon containing a cyclic unit such as a methylcyclohexyl group; a fluorenyl group (b-3) a methoxyethyl group, an ethoxyethyl group, a propoxyethyl group , propyl, ethoxypropyl, propoxypropyl An organic bond containing an ether bond (b-4), an ethylene group, an allyl group, an isoprofen (isopr〇penyi), a butenyl group, an isobutenyl group, a pentenyl group, a hexene group; An unsubstituted or substituted aromatic quinone, and having a structure of more than one selected from the group consisting of unsubstituted or substituted chain-like, branched-shaped 'rings, as required by 321346 28 201004993 Examples of the aromatic hydrocarbon group having a fatty dihydrocarbon unit & = and having a carbon number of 6 or more and 24 or less and an oxygen atom number of 5 or more and 5 or less may be exemplified by a phenyl group, a f-group, and a dimethyl group. Benzyl, α-methylstyryl, 3-mercaptostyryl, 4-fluorenyl-alkenyl, alkoxy (tetra) compound may also be a mixture of the above a) to C) organic species . ^2, as long as it is within the above range of the number of carbon atoms and the number of oxygen atoms, organic: oxygen: monoterpene unit, methoxy unit, fluorenyl unit, carboxy unit, ?; oxy oxime, fluorine or chlorine The halogen atom or the ester bond, the atom other than the oxygen atom or the nitrogen of the (tetra), the sulfur or the like, the organic I is the upper 34 MG), one or a mixture of the two components is present. The hardened resin of the modified resin of the present embodiment is hardened to have a light-resistance, or the ampule of the hydroxy group is rn. ... the total number of moles of Wang Sl, which contains the element, the m-unit of the bauxite, the unit of the subtraction, and the unit of the alkenyl group, in addition to the oxygen, the two atoms, or the vinegar bond, further combined with the base (4) The organic atom of a hetero atom such as a nitrogen, a dish or a sulfur is preferably the following, and the second is preferable. In the case of a 1% compound, the modified resin composition of the present embodiment is used to make it far away. Is it safe and reproducible? 29 32]346 201004993 Relative to the total number of moles of all Si units, tendency (b-4) vinyl, propyl, isopropyl, butadiene The total number of moles of the group, the isobutyl group, the pentyl group, and the monovalent aliphatic group is less than 1% by mole. The following is preferred, and 1% or less is more preferable, and it is preferably not contained at all. 5% 5% In order to improve the heat-resistant discoloration property of the modified resin composition of the present embodiment, the organic group R1 of the general formula (1)选自 selected from the above a) '丨 丨 Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο Ο , τ, hydroglyceryloxybutyl, etc., glycidyloxyalkyl group, glycidyl group, 3-(3,4-epoxycyclohexyl), which is bonded by an oxyglycidyl group at a carbon number. Ethyl, Bu (3 epoxycyclohexyl) propyl, bis-(3,4-epoxycycloheptyl)ethyl, ^(3,4-epoxycyclohexyl)propyl epoxycyclohexyl) An organic group in which a group of ketones, Κ3 4-epoxycyclohexyl)pentyl group and W) and 2) have a carbon number of i or more and 8 or less and an oxygen atom number is a group, and a phenyl group or a phenyl group It is more preferred to be selected from the group; to be an oxygenated silk water having a carbon number of 4 or less selected from the group consisting of d-glycidyloxyethyl, Iglycidyloxypropyl, r, hydroglyceryl butyl, and the like. The glyceryl group is combined with a red glycidyloxyalkyl group, a glycidyl group, a fluorene-(3,4-epoxycyclohexyl)ethyl group, and a dip) and a 2) carbon number of 1 or more and 3 or less and oxygen. It is particularly preferable that the number of atoms is an organic group of the group of sputum and the group selected from the group of phenyl groups. Next, the description of R2 in the present embodiment will be described. R2 of the present embodiment independently represents a gas atom, d Having a choice from no substitution Or one or more structures in which a group of bonds, a sub-technical structure, or a ring-formed structure are substituted. 30 321346 201004993 A monovalent organic group having an aliphatic hydrocarbon unit and having a carbon number of 1 or more and 8 or less, the d The monovalent organic group may be exemplified by: mercapto, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, tert-butyl, t-butyl, n-pentyl, isopentyl, new Amyl, n-hexyl, n-heptyl, octyl, decyl, decyl, undecyl, dodecyl, thirteen carbon, tetradecyl, fifteen carbon, ten a chain-like organic group composed of an aliphatic hydrocarbon such as a hexacarbyl group, a heptacarbonaceous group, an octadecyl group and a octadecyl group; a cyclopentyl group, a fluorenylcyclopentyl group, a cyclohexyl group, a fluorenylcyclohexyl group, and a borneol An organic group composed of a hydrocarbon having a cyclic unit or the like. The alkoxydecane compound may be a mixture of two or more kinds of the above-mentioned d) organic groups. Further, one type or two or more types of organic groups may be present in combination. Among these organic groups, a thiol group, an ethyl group, a n-propyl group or an isopropyl group is preferred because of the tendency to increase the reactivity of the alkoxylate compound, and a methyl group or an ethyl group is more preferable. In the present embodiment, in the alkoxydecane compound, the alkoxydecane compound represented by the above formula (1) contains at least: (B) n = 1 or 2 and at least one cyclic ether group. At least one alkoxydecane compound of R1 and at least one alkoxydecane compound of (C) n=l or 2 and at least one aromatic organic group as R]. When at least one alkoxydecane compound having at least one cyclic ether group and having at least one cyclic ether group as R1 is contained, the cured product obtained by curing the modified resin composition of the present embodiment is cured. Cracking and adhesion are not sufficient. On the other hand, in the case of at least one alkoxydecane compound which does not contain (C) n = 1 or 2 and at least one aromatic organic group as R], the modified resin composition is phase-separated, and is obtained. To the genus 31 321346 201004993 resistance to thermal shock resistance and adhesion. Specific examples of the component (B) used in the present embodiment include 3-glycidyloxypropyl (methyl) dimethyloxycarbazide and 3-glycidyloxypropyl (fluorenyl). Diethoxy zeshi, 3-glycidyloxypropyl (methyl) dibutoxy decane, 2-(3,4-epoxycyclohexyl)ethyl(methyl)dimethoxy decane , 2-(3,4-epoxycyclohexyl)ethyl(phenyl)diethoxydecane, 2,3-epoxypropyl(indenyl)didecyloxydecane, 2,3-epoxypropane (phenyl) dimethoxy decane, 3-glycidyloxypropyl trimethoxy decane, 3-glycidoxy propyl triethoxy decane, 3-glycidyloxypropyl Tributoxy sulphate, 2-(3,4-epoxycyclohexyl)ethyltrimethoxy oxetane, 2-(3,4-epoxycyclohexyl)ethyltriethoxy decane, 2,3-epoxypropyltrimethoxycrushed, 2,3-epoxypropyltriethoxy, etc. These may be used alone or in combination of two or more. Specific examples of the component (C) used in the present embodiment include dimethoxyindenyl decane, diethoxynonylphenyl decane, phenyltriethoxy decane, and trioxane. Alkyl [3-(phenylamino)propyl]decane, dimethoxy diphenyl monoxide, diphenyldiethoxy calcination, phenyl tridecyloxy chopping, and the like. These may be used alone or in combination of two or more. Further, in the modified resin composition of the present embodiment, in addition to the components (A) to (C), the following may be used as the other component: the above formula (1) indicates the number of R1. n = 0, specifically, an alkoxylate compound obtained by combining four (0R2). Examples of such an alkoxy calcined compound include tetramethoxy cerium, tetraethoxy cerium, tetrapropoxy decane and the like. These may be used alone or in combination of two or more. 321346 201004993 Here, the mixing index α used in the present embodiment will be described. In the (8) general formula (1), η = 1 or 2 and at least one cyclic ether group is used as at least j alkoxydecane compounds of r1 in the general formula (1). And (c) in the general formula (1), η = ι or 2 and at least one aromatic organic group as a mixture ratio of at least one of the ruthenium species of the ruthenium compound "(4) is a formula (2) calculation &; mixed indicator a ° (2)

The mixing index a=(ac)/(ab) (in the 'Formula (2)' ab represents the content of the component (8) in the oxylate smoldering represented by the general formula (1) (m〇W ' ac represents the general formula (1) In the present embodiment, in order to ensure the fluidity and storage stability of the modified resin composition, the above-mentioned mixing index "must be Q. (four) or more, and the other In order to ensure the fluidity of the modified resin composition or the crack resistance of the cured product, the mixing index a must be in the range of 19 or less. The above = 〇 · 2 or more and 5 or less is better than G 3 or more and 2 or less. ^: The shape of the modified tree is a product, and the composition is burned in the composition; / the material oxygen exceeds _, and the composition is hardened, and the crack resistance or adhesion of the heat cycle is not good. The amount of residual methoxy group in the tree is preferably u _ lower, and 卩u is preferably 0.5% or less lower than 曰 '', and is preferably not contained at all. Further, the quantitative value of the amount of residual activating oxygen, It can be calculated by using the calculation, 2 - 4 Mo Yi Xu as the internal standard material surface measurement and listed as the internal of 321346 33 201004993 The area ratio of the quasi-wave peak to the peak derived from the residual alkoxy group is obtained. Specifically, it can be obtained by the method and the analytical method described below. <H-NMR measurement> (1) 10 mg of the resin composition and 20 mg of an internal standard material (1,1,2,2-tetrabromoethane; Tokyo Chemical Industry Co., Ltd.) were uniformly mixed with the hydrogenated chloroform 970rag as a solution for H-NMR measurement. ^ (2) The solution of the above (1) was measured for H-NMR spectrum under the following conditions: Apparatus: "α-400 type" manufactured by Sakamoto Electronics Co., Ltd. Nuclear species: Η Cumulative number: 200 times &lt; analysis of measurement results &gt; (3 The area value of the peak derived from the residual alkoxy group in the H-NMR spectrum was calculated. (4) The area ❹ of the peak derived from the internal standard substance in the H-NMR spectrum was calculated. (5) The above (3), ( 4) The obtained area values are substituted into the following formula, and the obtained result is defined as the amount of residual alkoxy groups (°/.). The amount of residual alkoxy groups (%) = (area value derived from the wave of residual alkoxy groups) / (area value derived from the peak of the internal standard substance) χ100 The modified resin composition of the present embodiment is at 25 ° C The degree is not particularly limited. However, in order to ensure the fluidity of the liquid, it is preferable to improve the handling property, and the mixing with the additive to be added as needed is easy, so that it is 1, OOOPa· Preferably, the liquid below s is preferably 34 321 346, 2010 04 993, 500 Pa.s or less, preferably more preferably below the valvular as, and preferably s or less. The epoxy equivalent of the modified resin composition of the present embodiment. (10)) The blending is particularly limited, but from the viewpoint of improving the storage stability of the modified resin composition, it is preferred to select a functional group having a ring enthalpy equivalent of 1 〇〇 g/eq or more. From the viewpoint of the cured product obtained from the resin composition, the epoxy equivalent is selected to be 7 〇〇g/eq or less (0 is preferred, and the range is at 1 〇〇g). The range of /eq or more and 500 g/eq or less is more preferably in the range of 3 〇〇g/eq or less. Next, the mixing index used in the present embodiment will be described; In the alkoxydecane compound used in the present embodiment, "n=2 alkoxylate compound", "n=l alkoxylate compound" and "n=〇 alkoxydecane compound" The mixing ratio is defined as the mixing index calculated according to the following formula (3). ❹ Mixed index y5={(y5n2 WnO+ySnl)} (3) (In the formula (3), cold n2 represents an alkoxy decane of η=2 in the alkoxydecane compound represented by the general formula (1). The content (mol%) of the compound, /3 η Ο represents the content (mol%) of the alkoxydecane compound of η = 0 in the alkoxydecane compound represented by the formula (1), and ySnl represents the general formula (1) The content (mol%) of the alkoxydecane compound in the alkoxydecane compound, and these are values satisfying 0${(stone 11〇)/(stone 11〇+cold 111+/5112)}$0.1) . In the present embodiment, in order to improve the fluidity of the modified resin composition and to improve the handleability, the above-mentioned mixing index 0 is at 35 321 346 201004993 on the other hand, and in order to improve the hardening.至以下的以下以下。 0. The following is preferably in the range of 0.03 or more. The range is better. Next, the mixing index r used in the present embodiment will be described. The mixing ratio of the epoxy resin (A) used in the present embodiment and the alkoxylated compound of "n = 0 to 2" in the alkoxy calcining compound is defined as the following formula (4) Calculate the mixed indicator r. ® Mixing index 7 = ( 7 a) / ( 7 s) (4) (In the formula (4), ra represents the mass (g) of the epoxy resin (A), and rs represents the general formula (1) The mass (g) of the oxy-cobalt compound of n = 0 to 2 in the alkoxylate. In the present embodiment, the crack resistance in the thermal cycle of the cured product obtained by curing the modified resin composition tends to be improved, and the mixing index 7 is 0.2 or more. On the other hand, in order to make the hardened modified resin The light resistance of the cured product of the composition tends to be improved, and the mixing index r is preferably in the range of 15 or less, preferably in the range of 0.04 or more and 7 or less, and more preferably in the range of 0.08 or more and 5 or less. . In the modified resin composition of the present embodiment, the storage stability of the modified resin composition, that is, the condensation ratio of the alkoxydecane compound from the viewpoint of suppressing the viscosity of the resin during storage and improving the handleability Preferably, it is 80% or more, more preferably 82% or more, more preferably 85% or more, and more preferably 88% or more. Further, the condensation ratio of the alkoxydecane compound of the present embodiment is 36.321346 201004993. The molar number (U) of ((10)2) contained in the alkoxycalcinous compound represented by the general formula (1) The molar number (v) of the (OR2) group in the polyoxonium component present in the modified resin composition is expressed by the following formula (5): the condensation ratio of the alkoxydecane compound (%Μ(υ-ν)/υ]χΐ00 (5) Next, an example of a specific production method of the modified resin composition of the present embodiment will be described. The modified resin composition of the embodiment of the present invention can be used in the ring. In the presence of the oxygen resin (A), a mixed index of at least the alkoxydecane compound represented by the following formula (1) (β) and (C) and represented by the following formula (2) is烷. 001 or more and 19 or less alkoxydecane compounds are produced by the following method of [Production Method 1] or [Production Method 2]. (ROn-^Si - (〇R2)4-n (1) (in Here, n represents an integer of 0 or more and 3 or less, and each independently represents a hydrogen atom and at least one organic group selected from the group consisting of a) to C) below: a) The selected from a substituted or unsubstituted linear, branched, cyclic formed by

An aliphatic group unit composed of one or more types of structural groups, B '^ contains an organic group having a cyclic ether group composed of a carbon number of 4 or more and 24 or less and an oxygen atom number of 1 or more and / or less; b) An aliphatic hydrocarbon unit having one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, cyclic, or structural groups, wherein the number of j is 1 or more and 24 or less and the number of oxygen atoms is 〇 Above 5 or less 9 i-valent aliphatic organic group; 321346 37 201004993 with a carbonaceous price C) having an unsubstituted or substituted aromatic hydrocarbon unit 'and optionally having a bond or branch selected from unsubstituted or substituted An aliphatic hydrocarbon unit composed of one or more kinds of structures of a shape, a ring shape, or a group of groups; an aromatic organic group having a ruthenium number of 6 or more and 24 or less and an oxygen atom number of 5 or more; on the other hand, R2 Each of the organic groups independently selected from the group consisting of a hydrogen atom and a group selected from the group consisting of: 〇d) having one selected from the group consisting of unsubstituted or substituted chain, branched, and cyclic structures The aliphatic hydrocarbon unit constituted by the above structure has an f number of 1 or more and 8 or less. An organic group), and bis (B) n = l or 2 and having at least one ether group, a cyclic group as Rl burning matter to burn Sleeper compound. (C) at least one alkoxydecane compound having n=l or 2 and having at least one aromatic organic group as R1; 夕 匕 指标 α α = ( α c) / ( α b) ... (2 ❹ (In the formula (2), ' ab indicates the content of the component (8) (rib 1%), and "c indicates the content of the component (c) (m 〇 1%)). [Production method 1] contains The following two steps are: (a) step and (b) step of the method for producing the modified resin composition. (a) Step. In the presence of the epoxy resin (1), at least the general formula (1) is not included (B) And the alkoxydecane compound of (c), the step of producing an intermediate by co-hydrolysis without a reflux step with dehydration. (b) Step 'Step 38 of the dehydration condensation reaction of the intermediate produced in the step (a) 321346 201004993 [Manufacturing Method 2] The method for producing a modified resin composition comprising the following two steps: (c) step and (d) step: (c) Step: at least containing the above-described formula (1) (B) and (C) an alkoxydecane compound, a step of producing an intermediate by cohydrolysis without a reflux step of dehydration. (d) Step: In (c) In the intermediate produced by the step, the epoxy resin (A) is allowed to coexist and the step of dehydration condensation reaction is carried out. Here, the "step of producing an intermediate by co-hydrolysis with a reflux step without dehydration" and "Step of performing dehydration condensation reaction". The "step of producing an intermediate by co-hydrolysis without a reflux step with dehydration" means water or a solvent to be blended for co-hydrolysis, and water derived from a burnt-oxygen-casting compound produced in the reaction or The solvent is subjected to a reaction step while flowing back to the reaction solution. The reaction pattern is not particularly limited, and it can be carried out by one or a combination of two or more kinds of anti-Q styles such as a batch type, a semi-batch type, or a continuous type. Specific examples thereof include a method in which a cooling tube is attached to the upper portion of the reaction vessel, and the generated water or solvent is refluxed while being reacted, or a reaction is carried out while stirring and/or circulating the reaction solution in a closed vessel. On the other hand, the "step of performing the dehydration condensation reaction" refers to a step of subjecting the added water or solvent and the water or solvent produced in the above-mentioned "reflow step without dehydration" to a condensation reaction while removing. For example, it can be carried out by using one or a combination of two or more of the following devices: a rotary evaporator, a vertical stirring tank equipped with a distillation tube, a surface renewal type stirring tank, 39 321346 201004993 thin film evaporation apparatus, surface renewal A biaxial kneader, a biaxial transverse agitator, a wetted wall reactor, a free-falling type porous plate type reactor, a reactor in which a volatile component is distilled off while the compound is dropped along the support, and the like. The modified resin composition of the present embodiment can be produced by any of the above methods [manufacturing method U and [manufacturing method 2]. In the case of producing the modified resin composition of the present embodiment, the reaction method of the alkoxylate compound is not particularly limited, and the reaction may be carried out in the initial stage of total conversion, or may be added to the reaction system one by one or continuously for reaction. In addition, in any of [Production Method 1] and [Manufacturing Method 2], the epoxy resin (A) may be added all at once or separately. Further, in the case of [Production Method 1], the steps (a) and (b) may be continuously carried out, or the reaction mixture obtained in the step (a) may be separated or recovered, and then the step (b) may be carried out. On the other hand, in the case of [manufacturing method 2], the steps (c) and (d) may be continuously carried out, and the reaction mixture obtained in the step (c) may be recovered, and then the step (d) may be carried out. Therefore, the epoxy resin (A) and the alkoxydecane compound used in [Production Method 1] and [Production Method 2] are the same as those of the above-exemplified epoxy resin (A) and alkoxydecane compound. Substance. Further, in [Production Method 1] and [Production Method 2], the suitable range of the mixing index α to 7 for the alkoxy sulphur-burning compound is the same as the above. In the [Production Method 1] or the [Production Method 2] of the present embodiment, when the step of producing an intermediate by co-hydrolysis without a reflux step with dehydration is completed, the condensation ratio of the intermediate is 78% or more. More than 80% is better than 321346 40 201004993, more preferably m or more. When the condensation ratio of the t intermediate is less than 78%, even after the subsequent dehydration condensation step, many (10) groups derived from polyoxo are left in the resin composition to be produced, and the residual GH group may be in storage. Condensation significantly reduces the amount of the fat composition, which tends to deteriorate the preservation stability. Further, in the present embodiment, the condensation ratio in the middle of the step of producing the intermediate by co-hydrolysis is the number of moles of the (10) 2) group contained in the oxycyl compound of the formula (1). (R), the number (8) of the base of the (IV) oxygen component (10)) present in the modified resin composition is expressed by the molar fraction shown by the following formula (6): Condensation rate of the alkoxy compound (%M) (R_S)/R] (6) In the method for producing a modified resin composition of the embodiment, the storage stability of the resin composition is changed, that is, from the viewpoint of suppressing the viscosity of the resin during storage and improving the handleability. In addition, the condensation ratio of the alkoxy compound is preferably 継 or more, preferably m or more, more preferably (4) or more, and particularly preferably 88% or more. Further, the alkoxylated compound of the present embodiment The condensation rate is based on the number of moles (8) of (10) 2) contained in the compound (10) 2) of the general formula (1), so that the presence of the modified ship is two (〇m) The number of ears (8) is expressed by the oxygen concentration of μ mol of the following formula (5): Condensation rate of the calcined carbaryl compound (5) This embodiment In the method for producing a modified resin composition, the residual amount of the hospitalic oxygen in the obtained modified resin composition is set to 5%, and the amount of oxygen in the residual resin is more than 5%. 321346 41 201004993 In the thermal cycle of the cured product, the crack resistance or adhesion is insufficient. The amount of residual alkoxy groups in the obtained modified resin composition is preferably 3% or less, and is preferably 1% or less. Preferably, it is more preferably 〇 (10) or less. It is particularly preferred to be completely non-contained. In the step (a) or (c) of the present embodiment, in order to hydrolyze the alkoxydecane compound, the reaction system is The water is added to the water. The addition of water is mainly for the hydrolysis of the alkoxydecane compound. The time of adding the water is not particularly limited, as long as it is added until the step of producing the intermediate until cohydrolysis is completed. Alternatively, a method of adding all at once in the initial stage of the reaction, a method of sequentially adding in the reaction, or a method of continuously adding in the reaction may be used, and it is preferred to use a method of fully adding at the initial stage of the reaction. Here, the description The amount of added water. The ratio of the amount of added water (molar number) to the amount of (OR2) in the above general formula (1) (molar number) is defined as a mixed index ε represented by the following formula (7) Mixed index ε = ( ε w) / ( ε s) (7) 0 (In this equation (7), 'ew represents the amount of water added (m〇i number), on the other hand, £ s The amount of (0R2) in the general formula (1) (mol number). The mixing index ε of the present embodiment is preferably in the range of 〇. 1 or more and 5 or less, and preferably in the range of 0.2 or more and 3 or less. The range below q 3 is more than 1 5 j; the range below is better. When the mixing index ε is less than 〇·!, the two-reaction reaction may not be performed, and when it exceeds 5, the storage stability of the modified resin composition may be lowered. The above step (a) or (c) may be carried out without a solvent or may be carried out in a solvent. When a solvent is used, a known solvent can be used as long as it is an organic solvent which can dissolve the epoxy resin and the 321346 42 201004993 alkoxy Wei compound and is inactive. The solvent of hydrazine may, for example, be dimethyl ether, diethyl ether, diisopropyl ether, 1,4-dioxane, 1,3-di-alkane, tetrahydrofuran, ethylene glycol dimethyl ether or ethylene glycol diol. μ, propane m propanediol single? An ether such as fine acetic acid vinegar or benzene f ether is a solvent such as mf-ethyl ketone or methyl isobutyl hydrazine; a linalic hydrocarbon such as calcined, cyclohexyl, gypsum, morphological, or isoxin; ; toluene, o-xylene, m-xylene, p-xylene, ethylbenzene = Fangxiangzhi Zhao solvent; ethyl acetate, butyl acetate and other ester solvents; methanol ethanol, butanol, isopropanol, positive Butanol, butyl cellosolve (ring) = 〇solve), butyl carbene (10), solvent. These solvents may use a mixture of 1 = more than one type. Among them, the epoxy group oxime in the inhibition reaction, the ketoxime solvent, the aliphatic hydrocarbon solvent, and the nicotine solvent are preferred, and the solvent containing 5% by mass of the solubilizing agent is preferably selected from the group consisting of U-diazepam, tetrazole, ethylene glycol dimethyl hydrazine, (iv) at least one or a mixture of two or more of the group ''·· better' W 1,4-H ton is county : Regarding the amount of addition of the solvent 'In the step (4), the co-hydrolysis is carried out in the course of the flow, and at the end of the (4) (4), the product is the product (10) and the material (10) is homozygous (4): square: at the step (C) In the step of producing the intermediate by the reflow step without dehydration: the total mass of the step of producing the intermediate is preferably 10 times the amount of oxygen added to the hydrazine. Since it can be added according to the solvent 321346 43 201004993 Since the molecular weight of the modified resin composition of the present embodiment is controlled in an amount, the amount of the solvent to be added is in the above range, and a resin composition having an appropriate amount of the appropriate amount to obtain an appropriate viscosity is obtained. Or the reaction temperature in step (c) is usually above 20 (TC below the range of TC). When it is not reached (the water sometimes solidifies, on the other hand, it exceeds 20 (the resin composition may be colored when TC is used. From the viewpoint of improving the reaction rate and suppressing the resin such as the riding of the oxygen group), The anti- ❹ temperature is 20. (: The range of 15 generations or less is better, and the range of 12 generations or less above the ankle boots is preferable, and the range below 1 〇 is better. The reaction temperature is within the above range. The reaction time may not be changed. The reaction time of the step (a) or (c) is not particularly limited, but the reaction rate of (10) 2) in the above general formula (1) is improved while suppressing the modification of the resin. In the case of α〇. H, the time above and not up to i 〇〇 hours is preferred, and the range of 1 hour or more and less than 8 hours is preferably 3 hours, and the range is less than 60 hours. More preferably, the range of 5 hours or more and less than 5 hours is particularly preferred. On the other hand, the reaction temperature of the step (b) or the step (d) is usually in the range of 〇C or more and 20 〇t or less. When the 〇〇c is not reached, the reaction speed will decrease by 1 and the time will become longer. The composition may be colored. From the viewpoint of improving the reaction rate and suppressing the modification of the resin such as ring opening of the epoxy group, the reaction temperature is 2 〇 t or more and 15 (the range under rCw is preferably 40 C or more and 120 C). The following range is preferable, and it is more preferably in the range of 5 ° C or more and 100 C or less. The reaction temperature is only 321346 44 201004993 in the above range, and it is not necessary to be constant, and may be changed in the initial stage of the reaction or during the reaction. b) The reaction time of the step or the (d) step is not particularly limited, but from the viewpoint of increasing the reaction rate and suppressing the modification of the resin, it is preferably in the range of 0.1 hour or more and less than 100 hours. The range of 0.5 hours or more and less than 80 hours is preferable, and the range of 1 hour or more and less than 50 hours is more preferable, and the range of 3 hours or more and less than 50 hours is particularly preferable. The modified resin composition of the present embodiment can be produced in an inert gas such as nitrogen, helium, neon, argon, helium, neon, carbon dioxide or a lower saturated hydrocarbon or air. Among these gases, from the viewpoint of suppressing the modification of the resin, an inert gas such as nitrogen, helium, neon, argon, helium, neon, carbon dioxide or lower saturated hydrocarbon is preferred, and nitrogen, helium, Helium, argon, helium, neon, and carbon dioxide are preferred, and nitrogen and helium are preferred, and nitrogen is preferred. The steps (a) to (d) of producing the modified resin composition of the present embodiment can be carried out under the above-described gas atmosphere, under the above-mentioned gas flow, under reduced pressure, by Q press, or in a combination thereof. Further, the pressure does not have to be constant, and may vary during the course of the reaction. Wherein, the step (a) or the step (c) is industrially easy because one of the water or the solvent blended for the co-hydrolysis and the water or solvent derived from the alkoxylated compound produced in the reaction must be industrially It is preferred to carry out the reaction while flowing back to the reaction solution, so that it is preferably carried out under the atmospheric pressure of the gas and/or under pressure. On the other hand, in the steps (b) and (d), the water or solvent added in the step (a) or (c) and the water produced in the above-mentioned "steps without dehydration 45 321346 201004993" or The solvent-surface removal-surface is subjected to a condensation reaction, so that it is preferably carried out under a flow of an inert fluorine gas and/or under reduced pressure. In the present embodiment, the "co-water scale" of the above (Α) epoxy (tetra) sulphur-oxygen compound may be carried out by adding a condensation condensation. Ο ❹ The hydrolysis-condensation catalyst is not particularly limited as long as it is a conventionally known hydrolysis-promoting reaction, and examples thereof include: metal (manufactured by Na, traitor, face, recorded, town, pin, recorded, zinc, ' Chin, aunt, 锗, tin, wrong, 锑, Shi Shen, ornaments, rotten, recorded, fierce, material), organic metals (bell, sodium, bell, tear, recorded, (four), 钡, town, zinc, titanium, Ming, recorded, tin, wrong, recorded, arsenic, antimony, boron, recorded, fierce, New Zealand, organic oxides, organic acid salts, organic compounds, burned oxides, etc.), inorganic tests (hydrogenated town, Oxide, hydrogen hydroxide, barium hydroxide, hydroxide steel, potassium hydroxide, hydroxide chain, barium oxide, sodium carbonate, potassium carbonate, sodium hydrogencarbonate, potassium hydrogencarbonate, etc.), organic test (ammonia hydrogen) Oxidized tetramethyl group, etc.). Among the above organometallics, organic tin is also preferred. The organotin refers to a combination of at least one organic group in the tin atom, and examples of the structure include monoorganotin, diorganotin, triorganotin, tetraorganotin and the like. The organotin may, for example, be tin tetrachloride, tri-butylated monobutyltin, monobutyltin oxide, monooctyltin trichloride, tetra-n-octyltin, tetra-n-butyltin dibutyltin oxide, dibutyltin diacetate or dioctanoic acid. Dibutyltin, dibuty tin diVersatate, dibutyltin dilaurate, dibutyltin oxylaurate, dibutyltin stearate, dibutyltin dioleate, dibutyltin·decyl ethyl reactant, a compound of dibutyltin salt and bismuth salt, a compound of dioctyltin salt and oxalate, bis(ethyl acetate) dibutyltin, bis(ethyl apple 321346 201004993 acid) dibutyltin, bis(butyl phthalate) Dibutyltin, bis(2-ethylhexylmalic acid) dibutyltin, bis(benzylmalic acid)dibutyltin, bis(stearyl malate)dibutyltin, bis(oleyl malate)dibutyltin,malic acid II Butyltin, dibutyltin bis(0-phenylphenoxide), bis(2-ethylhexylhydrothioacetate) dibutyltin, bis(2-ethylhexylhydrothiopropionic acid) dibutyltin, bis(isoindole Base-3-hydrogen Thiofanoic acid) dibutyltin, bis(isooctylthiothioacetate) dibutyltin, bis(3-hydrothiopropionic acid) dibutyltin, dioctyltin oxide, dioctyltin dilaurate, diacetic acid Dioctyltin, dioctyl® tin dioctoate® tin, di(dodecyl)hydrogenthiodioctyltin, dioctyltin wilsonate, dioctyltin distearate, bis(ethyl Malic acid) dioctyltin, bis(octylmalate)dioctyltin, dioctyltin malate, bis(isooctylthiocarbamic acid) dioctyltin, bis(2-ethylhexylhydrogen) Thioacetic acid) dioctyltin, dibutyltin dioxime oxide, dibutyltin diethoxylate, dibutyltin dibutoxide, dioctyltin dioxime oxide, dioctyltin diethoxylate, dioctyltin Dibutyl oxide, tin octoate, tin stearate, and the like. φ Further, among the above organometallics, an alkali organometallic which exhibits a basicity when the ligand is free is suitable. By using the organic metal as the hydrolysis condensation catalyst, the storage stability of the modified resin composition of the present embodiment tends to be improved. Further, since the organic phase of the organic metal is used, the condensation reaction tends to be rapid, so that it is very useful when a resin composition having an intermediate condensation ratio of 78% or more is obtained. Among the alkali organometallics, alkali organotin is also preferred, and an alkoxide-based organometallic is particularly preferred. Examples of the calcined oxide organotin include dibutyltin dimethoxide, dibutyltin diethoxylate, dibutyltin dibutoxide 47 321346 201004993, dioctyltin dioxime oxide, dioctyltin diethoxylate. , dioctyltin dibutyl oxide, and the like. On the other hand, when an acid-based organic metal which exhibits acidity when the ligand is free is used as a hydrolysis condensation catalyst, the hydrolysis reaction proceeds rapidly, but the condensation reaction tends to be difficult to proceed, which is not preferable in practical use. These hydrolysis-condensation catalysts may be used singly or in combination of two or more. For example, an organic acid tin may be used in combination with an alkali organotin to react an organic acid salt such as tin, or may be treated with an inorganic base. In this case, the inorganic base, ® is preferably a hydroxide of a polyvalent cation such as barium magnesium oxide, calcium hydroxide, barium hydroxide or barium hydroxide. The amount of the hydrolysis-condensation catalyst to be added is not particularly limited, and a suitable addition amount is obtained by the following mixing index (5) as a ratio of (0R2) in the above formula (1). It is represented by the following formula (8): a mixed index (5 = (6e) / ((5s) ... (8) ^ (here, in the formula (8), (5 e represents the addition amount of the hydrolysis condensation catalyst (mol number) (5s represents the amount (mol number) of (OR2) in the above formula (1)). The mixing index 5 is preferably in the range of 0.0005 or more and 5 or less, and more preferably in the range of 0.001 or more and 1 or less. The range of 005 or more and 0.5 or less is better. According to the composition of the modified resin composition, when the mixing index 5 is less than 0.0005, the promoting effect of hydrolysis condensation may be difficult to obtain, and when it exceeds 5, it may sometimes be promoted. The ring opening of the cyclic ether group may cause deterioration of the preservation stability. 48 321346 201004993 The modified resin composition of the present embodiment has good storage stability and good transparency, and t heat. a modified resin composition of a cured product having a thermal discoloration property, a light resistance property, and a crack resistance during thermal cycling, Since the cured product is formed by heat or energy rays, it can be suitably used as a raw material resin composition such as a light-emitting element sealing material, an optical lens, a photosensitive resin, a fluorescent resin, a conductive resin, or an insulating resin. In the modified resin composition of the present embodiment, oxetane (D), phosphor (E), conductive metal powder (F), ® insulating powder (G), or the like may be blended. Epoxy resin (A'), hardener (Η), hardening accelerator (I), photoacid generator (J), cationic polymerization catalyst, modifier, vinyl ether compound, epoxy An organic resin other than the resin (Α'), and a dreaming coupling agent. A resin composition obtained by adding an oxetane compound (D) to the modified resin composition of the present embodiment. The alkane compound (D) is not particularly limited as long as it is an oxetane ring-containing compound, and is, for example, 3-ethyl-3-hydroxyindenyloxybutane or 3-ethyl-3. -(2-ethylhexyloxymethyl)oxetane, bis(3-ethyl-3-oxetanyl)ether, 3-B -3-(phenoxymethyl)oxetane, 3-ethyl-3-(2,3-epoxypropoxydecyl)oxetane, etc. by blending the oxalate The cyclobutane compound tends to have a higher polymerization rate, and the viscosity of the composition tends to decrease. Representative examples of the oxetane compound are shown below. 49 321346 201004993

The blending amount of the above oxetane compound is not particularly limited. The blending ratio of the resin composition: oxetane compound = 20: 80 to 95: 5 (total 100) is preferably carried out, preferably 40: 60 to 80: 20. When the blending ratio of the resin composition is less than 20, the hardening reaction may not proceed normally, and when it exceeds 95, the adhesion of the cured product may be deteriorated. In order to improve the compatibility of the resin composition with the oxetane compound, for example, an oxetane compound having an aromatic ring is usually used as a resin composition using an epoxy resin having a bisphenol backbone as a raw material. Combine and so on and select the appropriate combination. A fluorescent resin composition obtained by adding a phosphor (E) to the modified resin composition of the present embodiment will be described. In the present embodiment, the phosphor (E) is a substance that emits fluorescence. In short, as long as it absorbs energy such as electron beams, X-rays, ultraviolet rays, and electric fields, the absorbed energy is more efficiently used as visible light. Injection (luminescence) 50 321346 201004993 Yes, there is no special limitation, and it can be used in inorganic or organic systems: 'In the case of bismuth, an inorganic phosphor that exhibits excellent luminescence is usually used. The size of the inorganic phosphor which can be used in the present embodiment is limited, and a powder having a particle diameter of from 1 to several tens is usually used. Further, in order to express the performance of the inorganic phosphor, a compound called an activator (light-emitting center) is introduced into the compound A called a parent, and the user is usually "parent A: activator β". Said. In particular, when the fluorescent resin composition is used as a sealing material for an LED, it is preferable to use a phosphoric acid (YAG: Ce phosphor) which is an inert gas for the reason described later. When it is used as a light-storing material, it is preferable to use a light-emitting body, and these may be used alone or in combination of two or more. Regarding the blending amount of the phosphor, in terms of mass ratio, it is preferably a resin composition: phosphor = 30: 70 to 95: 5 'more preferably 5 〇: 5 〇 to 8 〇: 2 〇 (合什100). When the amount of the phosphor is more than that of the resin composition: phosphor: ❹70, the fluidity of the fluorescent resin composition is deteriorated. When the amount is less than 95:5, the function of the phosphor is insufficient. The situation. The precursor A and the activator β are not particularly limited. For example, the precursor a may be, for example, an oxide phosphor or a nitride glaze. Further, the activator β may be a rare earth element such as Eu (Eu) or cerium (Ce). As the above-mentioned oxide phosphor, for example, the parent a is strontium aluminate (YdhO 2: hereinafter referred to as YAG) and the activator B is 钸 ((: 〇 「 "yag:

Ce phosphor." When this is irradiated with blue light (near 46 〇 nm), yellow light is effectively caused. This fluorescent system can change the structure of the mother A by replacing a part of 321346 51 201004993 of γ of "YsAh〇i2" with another Gd or Tb or the like, or by replacing a part of A1 with Ga or the like. It is very useful to move to the long wavelength side or the short wavelength side. In short, the "YAG: Ce phosphor" is a structure in which the parent A is YAG, or a part of Y is replaced by another Gd or Tb, or a part of the yt is replaced by Ga or the like, and the structure of the parent A is changed. The activator B is not particularly limited as long as it is a phosphor of Ce. Specific examples thereof include ❺ "Y3Al5〇12: Ce3+" or "(γ3, Gdu)Al5〇12: Ce3+". In the case of the oxide phosphor, it is known that the parent A is Sr'Ba 2Si〇4 and the eu (eu) is introduced as the activator B ((Sr,Ba)2 S1O4 ·· Eu phosphor." This material can adjust the luminescent color to green to discolor by changing the composition ratio of Sr to this. As the above-described nitride phosphor, for example, the following examples are given. Sialon phosphor · · maternal A is a crystal formed by solid-solving metal ions such as Ca and aluminum and oxygen in α-type tantalum nitride crystal, and ❹ "[Mp(Sl,AI)12(〇, Here, N represents a metal ion, and p represents a solid solution amount. Specifically, "Cap (Si, A1)" (〇, N) i6: £ or the like can be cited. Cold-Sialon phosphor: The matrix A is represented by a composition of "SihAl^Nh" in which solid aluminum and oxygen are formed in a stone-type tantalum nitride crystal. Here, 9 indicates a solid-flux amount. Specific examples thereof include "Sh-qAlAN8-q: Eu" and the like.

CaAlSiN3 phosphor: The matrix A is a nitride crystal obtained by reacting calcium nitride, aluminum nitride and tantalum nitride at a high temperature of 1800 C, and specific examples thereof include "CaAlSiNs: Eu". 321346 52 201004993 Specific examples of the inorganic illuminant include, for example, "_.AS crystal: w, Yam: EU", "cauQ1 Eu〇, Ga3〇7j.rBaY〇. 9Sm, lGa3〇7j, rCa(Y〇5Eu〇s)^ (7)”, “Y3〇3:Eu, m:Eu”“(4): Eu”, “35MgG.〇5Mg F2Ge〇2: Mn4+”, “( Y · Cd) B〇2 : Euj, etc. Those with blue luminescent color can be cited as: "(Ba, Ca, MgMp〇4) 3

Cl. Eu", "(Ba,Mg)2Al 16〇27: Eu2+", "Ba3MgSi2〇8: Eu", "BaMg2 〇Ο 八116〇," (Yi, heart (ie 4) 2: Such as 2+", "(义加^ci2 nB2〇3.Eu", "Sru)(P〇4)6ci2:Eu2+","(Sr,Ba Ca;)5(p〇4)3 Cl . Eu2" , "Sr2P2〇7: Eu", "Sr5(P〇4)3 C1 : Eu", "(Sr,Ba,Ca)3 (P〇〇6C1 .Eu", "Sr〇·p2〇5 · B2〇" 5: Eu", "(BaCa)5(p〇4)3C1 : ^'"SrLausTmowGa^'rznS : Ag", "GaW〇4", "Y2Si〇6: Ce=, "ZnS. Ag, Ga, Cl "Ca2B4〇cl: rib 2+", "BaMgAl4〇3: EU", "(M1,Eu)1°(P〇4)6Ch (Ml is selected from the group consisting of Mg, Ca, Sr, and Ba) At least one element in the group), etc.. Those having a green luminescent color include "ML: Ce3+ (YAG)", "Y2Si〇5 W, plus +", "(4) side, 2SrCh: Eu", "BaMg2Ah6〇27. Eu2+ 'Mn2+", "grab. 4: Mn", "Ζη2"〇4: Mn",

LaP〇4 : Tb", "srAi2〇4 : E "SrLa. 2Tbfl 8Ga3〇

CaY°. 9Pr〇lGa307”, “ZnGd〇·8Ho.·2Ga3〇7”, “SrLa.·6 Tb〇. 4 A13 Kenting, Z “nS. Cu' A1”, “(Zn, Cd)S: Cu, A1", "ZnS: Cu, Au, A1", "ZmS i 〇4: Μη", "2ns i 〇4: Mn", "ZnS: Ag, Cu", "(Zn · Cd) s : CU "ZnS. Cu", "Gd〇S: Tb", "LaOS: Tb", "YSi〇4: Ce • Tb", "ZnGe〇4. fc", "GeMgA1〇: Tb", "SrGaS: Rib 2+", 53 321346 201004993 "ZnS: Cu · C〇", "MgO · nM) 3: Ge, Tb", "LaOBr: Tb, I'm", "La2〇2S: Tb", etc. Further, "γν〇4: Dy" having a white-based luminescent color or "CaLu〇.5Dy〇.5Ga3〇7" having a luminescent color of a κ color system may be mentioned. Specific examples of the organic fluorescent material include, for example, 1,4-bis(2-methyl strepinyl)benzene (Bis_MSB) and trans-4,4'-diphenyl having a blue-based luminescent color. Styrene (1)1^) and other stilbene (51:11|^) coloring 0, 7-hydroxy-4-methylcoumarin (coumarin 4) and other coumarin pigments . have! For the color system to the green color, the commercial products can be listed as follows:

Brilliant sulfoflavine FF, Basicyellow HG, Sinloihi

Color FZ-5005 (manufactured by SINLOIHI Co., Ltd.). For those who have a yellow to red fluorescent color, commercially available products can be listed as follows:

Eosine, Rhodamine 6G, Rhodamine B, etc. When a general phosphor is blocked by light or an electron beam as an excitation source, the luminescence is immediately attenuated and destroyed. However, as far as the exception is concerned, there is a phosphor which exhibits residual light for several seconds to several tens of hours after blocking the excitation source, and this is called a light-storing phosphor. As long as the property is displayed, the type is not particularly limited. Specifically, for example, "CaS:

Eu, Tid", CaS · Bi", "CaAI2O4 : Eu, Nd", "CaSrS : Bi, "Sr2MgSi2 (h : Eu, Dy", "SnA1 win: Eu, Dy", "SrAh〇:: Eu, Dy" "Sr A1 must be: Eu", "ZnS: Cu", r ZnS : Cu, c〇", "Y2〇2S: EU, Mg, Ti", "CaS:Eu, Tffi", etc. "SnMgShO?: Eu, Dy", "Sr4All4〇25: Eu, Dy", "SrAh〇4:

Eu, Dy" and "SrA 12〇4 : Eu" are preferred. 321346 54 201004993 The method for producing the fluorescent resin composition of the present embodiment is not particularly limited, and examples thereof include a mixing device in which a modified resin composition and a phosphor are simultaneously or separately heated as needed. A method of stirring, mixing, dispersing, or a method of defoaming under reduced pressure after the above method. Further, a curing agent, a curing accelerator, a polymerization initiator, an additive, and the like which will be described later may be appropriately added in any of the above steps. The above-described mixing device is not particularly limited, and examples thereof include a kneader, a 3 ® roller mill, a ball mill, a planetary mixer, a line mixer, and a homogenizer. ), uniform dispersion machine, etc. A conductive resin composition obtained by adding a conductive metal powder (F) to the modified resin composition of the present embodiment will be described. The conductive metal powder (F) which can be used in the present embodiment is not particularly limited as long as it is a metal powder containing silver, and may be not only silver powder but also metal powder in which silver is adhered or coated on the surface. The metal powder referred to herein may be a metal element such as aluminum, bismuth, boron, carbon, magnesium, nickel, copper, graphite, gold or palladium, or a metal oxide or metal nitride powder thereof. Among the above, aluminum, nickel, gold, and palladium are preferred from the viewpoint of conductivity. Specific examples of the metal oxide and the metal nitride include oxidized magnesium, magnesium carbide, aluminum nitride, boron nitride, tantalum nitride, molten cerium oxide, crystalline cerium oxide, magnesium citrate, and aluminum. An oxide of a composite metal with ruthenium, an oxide of a composite metal of 1 Lu and iron, and the like. The V-free metal powder may also be a polyethylenimine 55 321346 201004993 (polyethylenimine), a polyvinylpyrrolidone, a polyacrylic acid, a mercaptomethylcellulose, a polyvinyl alcohol, and a polyethylene A surface coating of a polymer such as a copolymer of an amine moiety and a polyethylene oxide moiety. By coating with such a polymer, the dispersibility of the resin composition tends to be improved. Since silver is an element having a low volume resistivity, and the conductivity of the metal powder is more dependent on the surface state or the like depending on the support as the core, the entire particles of the conductive metal powder can be used even if it is not silver. A metal powder that adheres or coats silver on its surface. The shape of the silver powder is not particularly limited, and examples thereof include a scaly shape, a spherical shape, and a tree shape. The scaly silver powder-based silver powder has many joints and is excellent in electrical conductivity, and when it is made into a conductive resin composition from the orientation thereof, it exhibits excellent workability because it exhibits thixotropy. On the contrary, when used in a precision material, the electrical joint failure due to its alignment property may cause a problem. Further, the size thereof is not particularly limited, and the average particle diameter obtained by the laser diffraction type particle size distribution measuring apparatus is preferably 50 / / m or less, and preferably 1 to 20 / / m. When the average particle diameter is used for a precision electronic component or the like, it is preferable because the possibility of causing electrical bonding failure is lowered. Since the spherical silver powder has almost no alignment, it is less likely to cause problems in electrical bonding. However, since the particles are in point contact with each other, the conductivity tends to be deteriorated. Further, the size thereof is not particularly limited, and the average particle diameter is preferably 20 // m or less, preferably 5 / i m or less. When the average particle size exceeds 20 // m, the conductivity of 56 321346 201004993 tends to be low. In addition, when it is used together with the scaly silver powder for the purpose of burying the gap and achieving conductivity, it is preferable to select 5# m or less. The dendritic silver powder has a large specific surface area and excellent electrical conductivity, but its quality is unstable due to its specific shape. The size thereof is not particularly limited to 3 〇; m or less is preferable, and preferably 5 A 111 or less. It is preferred that the average particle diameter is formed so that the treatment tends to be excellent. This embodiment is based on the purpose or use, and in view of its nature, it is preferable to use silver powder of different shapes. Further, the conductive metal powder is suitably blended in an amount of 60 to 85% by mass, preferably 7 to 80% by mass, based on the resin composition. When the blending amount is 60% by mass or more, the conductivity is preferably changed, and when it is 85 mass% or less, the bleed phenomenon tends to be prevented. An insulating resin composition obtained by adding an insulating powder (G) to the modified resin composition of the present embodiment will be described. Specific examples of the insulating powder (G) which can be used in the present embodiment include non-oxide ceramic powders such as carbon, boron carbide, boron nitride, aluminum nitride, and titanium nitride; wrinkles, towns, and Mings , oxides of oxides such as titanium; oxidized dreams, nitrogen

η 'factory ~ material, Wo; rubber), iron fluoride (registered trademark) and other tree month / month luxury powder. These can be used alone to make soda glass, boron bismuth, and shixi rubber (silicon 321346 57 201004993 • 'This is used in combination. In the above, from the point of view of easy accessibility and insulation Oxide oxide, nitrite, molten gas, fossilized cerium oxide, and other cerium-containing fillers are preferred. The insulating powder may also be a smelting compound, or a polyethyleneimine or polyethylene. Surface coating, such as fine base material, polyacrylic acid, slow-base thiol cellulose, polyethylidene alcohol, and a copolymer having a polyethyleneimine moiety and a polyethylene oxide moiety. When the polymer is coated with the polymer, the dispersibility of the resin composition is preferably improved. The appropriate blending amount of the insulating powder bundle is preferably 5 to 50% by mass based on the resin composition. When the amount of the blending is 5% by mass or more, the insulating property is preferably changed, and if it is 5% by mass or less, the semiconductor device is improved by the stress relieving effect. The tendency of reliability In the modified resin composition of the form, the epoxy resin (A) contained in the modified resin composition of the present embodiment may be further contained in the epoxy resin (A'). An organic resin other than the epoxy resin (A) is blended, for example, an organic resin such as a polyoxyxylene resin, an acrylic resin, a urea resin, or a quinone imide resin. In the modified resin composition of the present embodiment, it may be added. The curing agent (H) and/or the curing accelerator (I) are used to form a curable resin composition. The curing agent is not particularly limited as long as it is used to cure the resin composition. An acid anhydride compound, an amine compound, a guanamine compound, a phenol compound, etc., in particular, an acid anhydride such as an aromatic acid anhydride or a cyclic aliphatic 321346 58 201004993 aliphatic acid anhydride or an aliphatic acid anhydride is preferred, and a carboxylic acid anhydride is preferred. Further, the acid anhydride-based compound may contain an alicyclic acid anhydride, and the carboxylic acid anhydride may preferably be an alicyclic carboxylic acid anhydride. These cured products may be used singly or in combination of two or more. Specific examples of the curing agent may be used. For example: phthalic anhydride, succinic anhydride, trimellitic anhydride, pyromellitic anhydride, maleic anhydride, tetrahydrophthalic anhydride, mercapto tetrahydro acid anhydride, Methyl Nadic ® anhydride, six Hydroquinone anhydride, methyl hexahydrofuric acid needle, norbornene-2, 3-dicarboxylic anhydride, mercapto norbornane-2, 3-dicarboxylic anhydride, diaminodiphenylcarbamate, diethylene Amine, triethylenetetramine, diaminodiphenyl, isodardiamine, dicyandiamide 'tetraethylenepentamine, dimethylbenzylamine, ketimine compound, Polyamide resin synthesized from 2nd linolenic acid and ethylenediamine, bisphenols, phenols (phenol, alkyl substituted phenol, naphthol, alkyl substituted naphthol) Polycondensate of dihydroxy-Q benzene, dihydroxynaphthalene, etc. with various aldehydes, polymer of phenols and various diene compounds, polycondensation of a mixture of di- and methyl groups, or dimethoxymethyl a condensate of a phenyl group with a naphthol or a phenol, a bisphenol and a modified substance thereof, a hydrazine, a trifluorochemical shed-amine complex, and a guanidine derivative. Wait. Specific examples of the alicyclic carboxylic anhydride include 1,2,3,6-tetrahydrophthalic anhydride, 3,4,5,6-tetrahydrophthalic anhydride, hexahydrophthalic anhydride, and "4-mercapto-6". Hydrophthalic anhydride/hexahydrophthalic anhydride=70/30”, 4-mercaptohexahydrophthalic anhydride, “mercaptobicyclo[2.2.1]heptane-2,3-dicarboxylic anhydride/bicyclo[2. 2 . 1] heptane-2, 3-two 59 321346 201004993 carboxylic anhydride" and the like. In the curing agent (H), since the light resistance of the cured product obtained by curing the modified resin composition of the present embodiment tends to be improved, the alicyclic acid anhydride has two or more molecules in one molecule. Preferably, the functional group of the acid anhydride is a polyoxyl oxide as a substituent, and methyl hexahydrophthalic anhydride, hexahydrophthalic anhydride, norbornane-2, 3-dicarboxylic anhydride, decyl norbornane-2, 3- Dicarboxylic anhydride is more preferred. These hardeners may be used alone or in combination of two or more. The amount of the hardener (Η) added can be obtained as a mixing index with respect to the ratio of the cyclic ether group contained in the epoxy resin and the alkoxy siloxane compound. The mixed index is expressed by the following formula (9): Mixed index Γ = (Γ〇 / (Γ1〇...(9) (in the formula (9), (f represents the addition amount of the hardener (H) (mol) (k) the amount of the cyclic ether group contained in the epoxy resin and the alkoxy siloxane compound (mol number). The mixing index is preferably in the range of 〇. 1 or more and 1.5 or less. The range of 0. 2 or more and 1.3 or less is preferable, and the range of 0.3 or more and 1.3 or less is more preferable. When the mixing index f is less than 0.1, the hardening speed is lowered, and more than 1 5, the moisture resistance of the cured product is deteriorated. The hardening accelerator (I) is a curing catalyst used for the purpose of promoting the curing reaction. As the curing accelerator (I), the tertiary amine and The salt is preferred. Specific examples of the hardening accelerator include the following: a 3-amine, a benzyldimethylamine, a 2,4,6-tris(dimethylaminomethyl)phenol, and a cyclohexyl group. Mercaptoamine, triethanolamine, etc.; imidazoles: 2-methylimidazole, 2-n-heptyl imidazole, 2-n-undecyl halide 60 321346 201004993 imidazole, 2-phenylimidazole, 2-phenyl-4- Methylimidazole _2_methylimidazole, 1-pyr-2-pyridyl imidazole, L2-dimethylimidazole, 2-methyl-1-methyl-t-sodium (2-cyanoethyl)-2-methyl, m Saliva, Bu (2j-ethyl)-2-n-undecyl imidazole, i - cyanoethyl) - phenyl imidazole, (2-cyanoethyl)-2-ethyl _4- Mercaptoimidazole, 2-phenyl-4-yl-indenyl-5-ylmethylimidazole, 2-phenyl-4,5-bis(hydroxymethyl)imidazole, anthraquinone-ethyl)-2-phenyl -4, 5-bis[(2,-cyanoethoxy)indolyl]imidazole, partial bismuth dicarboxylic acid (2-cyanoethyl)-2-n-decene-carbon silk frozen salt, partial benzene 1-(2-cyanoethyl)-2-phenylimidazolium succinate, trimellitic acid (2-cyanoethyl)-2-ethyl-4-indolyl imidazolium salt, 2 deducted 2 [2,-methyl-saltylethyl triterpenoid, 2 s-diamine _6: (2, n-undecylalkyl imidazolyl) ethyl-s-triazine, 2,4_ Diaminoethyl_4, monomethylimidazolyl-(],) ethyl-S-trimorphine, 2-methylimidazolium iso-cyanate adduct, 2-phenylimidazole Polycyanate adducts, etc.; organophosphorus compounds: diphenylphosphine, triphenylphosphine, phosphorous acid ❹ esters; 4 grade phosphcmium salts: gasified benzyl triphenyl scales, tetra-n-butyl bromide scales, methyl triphenyl scales, ethyl triphenyl scales, bromine N-butyl diphenyl scale, tetraphenyl bromide 'Iodide ethyl triphenyl scales, acetamethylene diphenyl scales, hydrazine, hydrazine _ diethyl dithiophosphate tetra-n-butyl scales (tetra-n-butyl phosphonium 0,0-diethyl ph〇Sph〇r〇dithi〇nate), tetra-n-butyl benzyl triazole, tetra-n-butyl tetrafluoroborate, tetraphenyl-tetra-butyl Base scale, four # base butterfly acid tetraphenyl scales. 321346 61 201004993 Diazabicycloolefins: 1,8-diazabicyclo[5.4.0]undecene-7 (l'8-Diazabicyclo[5.4. 0]undec-7-ene) and its organic acids蹿, etc.; existing metal compounds: zinc octoate, tin octoate, acetonitrile, aluminum, mis-injection, etc.; θ ° 4 grade ammonium salts: tetraethylammonium bromide, tetra-n-butylammonium bromide, etc.;

Metal halide: boron compound such as boron trifluoride or triphenyl borate; zinc oxide, stannic chloride, and the like. The amount of the hardening accelerator (1) to be added can be determined from the following mixing index of the ratio of the mass to the mass of the above epoxy resin. The mixed index 77 is expressed by the following formula (1〇): Lower mixed index e=Ug)/(??k) .··〇〇)

V (here, /(10), Μ represents the mass of the hardening promotion mm) (4), k represents the mass (g) of the epoxy resin and the alkoxy siloxane compound. And /: combination index: It is better to use a range of ,.01 or more and 5 or less, and a range of 1 or more and 1 or less. When it is less than 0. (U, there is a case where the hardening does not proceed well, and more than 5 犄 'the cured product is colored. Illustratively, the photoacid generator (J) is added to the modified resin composition of the present embodiment. A photosensitive resin composition which can be used in the form of a photoacid generator (1) which can be used as long as it emits acid by irradiation with light, and which does not contain special mosquitoes, in the pot, (4) salt is preferable. Specifically, it can be transferred to: Qianjing salt, (4), and salt-dissolving (SUH〇niumsalt), etc., which are aromatic 321346 62 201004993 diazonium, aromatic hydrazine, and aromatic

SbiV, [BL]' (herein, an anion moiety is βίν, Ρΐν, 隹, X, X is a phenyl group substituted with at least two or more fluorine groups), and the like Tungsten salt. The acid generator is as follows. Not 〇

Here, R, R' and R' ' represent an arbitrary substituent.

321346 63 201004993 More specific examples can be exemplified by: an aryldiazonium salt of boron tetrafluoride, a diaryl salt of hexafluoride, a diarylsulfonium salt of a fluorinated scale, and a ruthenium hexafluoride. Triaryl sulfonium salt, diaryl sulfonium salt of ruthenium hexafluoride, tris-methylphenyl sulfonium salt of arsenic hexafluoride, tris--4-decyl sulfhydryl salt, antimony tetrachloride Pentafluorophenyl)boronic acid triarylsulfonium salt, ruthenium (pentafluorophenyl)borate diaryl lock salt, ethylene-branched I-block salt and o-nitrobenzyl-stone-bake base mixture, phenyl sulfide 0 More than π fixed salt 'six gasified propylene dilute-iron complex and so on. Commercially available products include: CD-1012 (manufactured by SARTOMER Co., Ltd.), PCI-019, PCI-021C (Japan Chemicals® Co., Ltd.), OPTMER SP-150, and OPTMER SP-170 (made by ADEKA Co., Ltd.) ), UV1-6990, UVI-6974 (manufactured by The Dow Chemical Company), CPI-100P, CPI-100A, CPI-100L (manufactured by San-apro Co., Ltd.), TEPBI-S (Japan Catalyst) (Rhodorsi 1 2074 (manufactured by Rhodia Co., Ltd.), etc., may be used alone or in combination of two or more. In the above-mentioned "from the viewpoint of the coloring of the cured product, the cerium salt and the cerium salt are preferred, and when the curing property is considered, the cerium salt is particularly preferable. 〇 In addition, in the above-mentioned photosensitive resin composition, an ethylene group compound compound can be pushed in accordance with the demand. The % compound may, for example, be a vinyl-free compound having no trans group. Specific examples thereof include ethylene glycol divinyl sulfonate, butanediol divinyl ether, cyclohexane dimethanol divinyl ether, cyclohexanediol monoethyl amide, and trimethyl methacrylate triethylene Base, pentaerythritol tetraethyl ether, glycerol trivinyl ether, triethylene glycol divinyl ether, diethylene glycol divinyl ether, and the like. Further, the modified resin composition of the present embodiment may be blended with a conventional cationic polymerization catalyst. Cationic polymerization catalyst series which can be used 64 321346 201004993 For example: Lewis acid catalyst represented by BF3 amine complex, PFs, BFs, AsFs, SbFs, etc.; bismuth or quaternary ammonium salt, strontium salt , benzyl ammonium salt, benzyl group than occluded salt, benzyl salt, hydrazine hydrate (hydrazinium salt), tareate ester, sulfonate, amidoxime represented by thermosetting cationic polymerization catalyst An ultraviolet curable cationic polymerization catalyst typified by diaryl sulfonium hexafluorophosphate or bis(dodecylphenyl)phosphonium hexafluoroantimonate. Among the above, it is preferred to use a thermosetting cationic polymerization catalyst ® because a transparent cured product having a high glass transition temperature and excellent solder heat resistance or adhesion is desired. For example, commercially available products of the thermosetting cationic polymerization catalyst include SI-100L of a phosphonium salt-based cationic polymerization catalyst, SI-60LC or higher, manufactured by Sanshin Chemical Industry Co., Ltd., and CP-66 and CP-77C or higher. , Asahi Chemical Industrial Co., Ltd., etc. The modified resin composition obtained in the present embodiment may contain a modifier as needed from the viewpoint of imparting flexibility to the cured product and improving peeling adhesion. The modifier to be used may be a polyol having two or more Q hydroxyl groups in one molecule, for example, ethylene glycol, diethylene glycol, triethylene glycol, polyethylene glycol, and 1,2-propanediol. , 1,3-propanediol, dipropylene glycol, tripropylene glycol, polypropylene glycol, 1,2-butanediol, 1,4-butanediol, neopentyl glycol, glycerol, pentaerythritol, trihydroxydecyl propane, 1 An aliphatic polyhydric alcohol such as 2,4-butanetriol or a polycarbonate diol or a polyoxyl group having a sterol group at the end is preferred. These modifiers may be used singly or in combination of two or more. In the modified resin composition of the present embodiment, various decane coupling agents can be used for the purpose of improving physical properties such as adhesion. At this time, the residual alkoxy group in the composition of the modified resin 65 321346 201004993 must be 5% or less. When the residual alkoxy group exceeds 5 ° / 〇, the hardened material obtained by hardening the composition becomes insufficient in the thermal cracking property or the adhesion. Examples of the decane coupling agent suitable for the modified resin composition of the present embodiment include 3-glycidyloxypropyltrimethoxy decane and 3-glycidyloxypropyltriethoxy zebra. 3-glycidyloxypropyl decyl decyloxydecane, 3-glycidyloxypropyl decyl diethoxy decane, 3-glycidyloxypropyl decyl decyloxy decane , 3-glycidyl® oleyloxypropyl decyl ethoxy decane, 2-(3,4-epoxycyclohexyl)ethyltrimethoxydecane, 2-(3,4-epoxycyclohexyl Ethyl triethoxy oxime, 3-aminopropyltrimethoxy sulfonate, 3-aminopropyl triethoxy chopping, 3-aminopropylmethyldiethoxy sinter , 3-aminopropyldidecylethoxy ketone, N-(2-aminoethyl)amino fluorenyl ruthenyloxy, N-(2-aminoethyl) (3_ Aminopropyl)trimethoxy-burning, N-(2-aminoethyl)(3-aminopropyl)triethoxymethane, N-(2-aminoethyl)(3-amine Propyl 曱 曱 ❹ 曱 曱 曱 、, N-[Ν'-(2-aminoethyl)(2-aminoethyl)](3-aminopropyl) Trioxane, calcination, 2-(2-aminoethyl)thioethyltriethoxymethane, 2-(2-aminoethyl)thioethylmethyldiethoxylate, 3 -(N-phenylamino)propyltrimethoxy oxime, 3-(N-cyclohexylamino)propyltrimethoxy decane, (N-phenylaminoindenyl)trimethoxy decane (N-Phenylaminoindenyl) fluorenyldimethoxymethane, (N-cyclohexylaminomethyl)triethoxymethane, (N-cyclohexylaminomethyl)methyl Ethoxy decane, piperylene decyl tridecyloxy decane, piperylene methyl triethoxy decane, 3-piperidinyl propyl tridecyl oxyalkylate, 3-pyridyl propyl fluorenyl Dimethoxyl-crushed, 3_glypropylpropyl 66 321346 201004993 triethoxydecane, thiomethylmethyltrimethoxy decane, thiosulfanyltriethoxy decane, thiol thiol Dimethoxy decane, thiophanylmethyl diethoxy decane, 3-hydrothiopropyltrimethoxy decane, 3-hydrothiopropyltriethoxy pulverization, 3-hydrogen Thiopropyl decyl dimethoxy acid, 3-azathiopropyl decyl diethoxy pulverization, 3 _ trimethoxy chopping base Propyl succinic anhydride, 3-(triethoxydecyl)propyl succinic anhydride, tetramethoxy decane, tetraethoxy decane, decyl tridecyl decane, decyl triethoxy decane, ethyl Trimethoxy decane, ethyl triethoxy decane, propyl tri methoxy decane, propyl triethoxy decane, vinyl trimethoxy decane, ethyl bake triethoxy dream Cyclohexyltrimethoxymethane, cyclohexyltriethoxydecane, cyclopentyltrimethoxyoxydecane, cyclopentyltriethoxydecane, phenyltrimethoxydecane, phenyltriethoxydecane, two Methyldiazepine calcination, dimercaptodiethoxy pulverization, mercaptoethylene dimethoxy pulverization, mercaptovinyldiethoxy decane, nonylphenyl dimethoxy decane , nonylphenyldiethoxydecane, methylcyclohexyldimethoxysilane, methylcyclohexyldiethoxydecane,nonylcyclopentyldimethoxyoxydecane,nonylcyclopentyl Ethoxy decane, 3-methacryloxypropyl decyl decyloxydecane, 3-mercapto propylene methoxy propyl trimethoxy decane, 3-mercapto propylene decyloxy Propylmercaptodiethoxydecane, 3-mercaptopropenyloxypropyltriethoxylate, etc. A partial condensate of such a sulphur coupling agent can also be used. Further, in the modified resin composition of the present embodiment, an inorganic filler, a coloring agent, a leveling agent, and a lubricant other than the above may be appropriately added in accordance with the purpose of not impairing the function of the resin composition. , surfactants, antioxidants, light stabilizers, etc. In addition, it can be blended with other plasticizers, flame retardants, and anti-static agents commonly used as 67 321346 201004993 resin additives.

Impact-resistant enhancer, foaming agent, antibacterial, anti-I w, Qin agent, conductive filler, anti-fogging agent, cross-linking agent, etc. In the case of inorganic filling materials, for example, it can be listed as a problem. _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ Sirning (irnned Silica), colloidal silica dioxide (cow· talc, clay, magnesium hydroxide, crushed acid, sage ca), sedimentary dioxide), carbon cutting, nitrogen cutting, nitriding shed, Calcium carbonate, magnesium carbonate, barium sulfate, calcium sulfate 'mica oxide, magnesium oxide, zirconium oxide, aluminum hydroxide, f 酉 aluminum, lithium aluminum niobate, zirconium silicate, barium titanate, glass fiber, carbon fiber, two Molybdenum sulfide and the like. In particular, cerium oxide, calcium carbonate, aluminum oxide, aluminum hydroxide, calcium citrate or the like is preferred. Further, when considering the physical properties of the cured product, it is preferred to use a gasified hydrazine. These inorganic fillers may be used singly or in combination of two or more. The coloring agent is not particularly limited as long as it is used for the purpose of coloring, and examples thereof include phthalocyanine, azo 'disazo, quinacridone, and brewing. &gt;, scallions _ (Flavanthrone), $^i^(perinone), 茈, dioxazine, condensed azo, azomethine are various organic pigments; titanium oxide, lead sulfate, Inorganic pigments such as steam, zinc yellow, chrome vermilion, red iron oxide (Bengala), zizi, prussian blue, ultramarine blue, carbon black, chrome green 'chromium oxide, cobalt green, etc. These colorants may be used singly or in combination of two or more. The coating agent is not particularly limited, and examples thereof include oligopolymers having a molecular weight of 4000 to 12,000 composed of acrylates such as ethyl acrylate, 68 321 346 201004993 butyl acrylate, and 2-ethylhexyl acrylate; epoxidation; Soy fatty acid, epoxidized rosin alcohol, hydrogenated castor oil, titanium coupling agent, and the like. These coating agents may be used singly or in combination of two or more. The lubricant is not particularly limited, and examples thereof include hydrocarbon-based lubricants such as solid paraffin, microcrystalline wax, and polyethylene wax; and advanced lauric acid, myristic acid, palmitic acid, stearic acid, arachidic acid, and behenic acid. Fatty acid-based lubricants; stearylamine, palm amide, ceramide, sulfhydryl bis-lipidamine, ethyl bis-lipidamine, and other fatty acid amide-based lubricants; hardened castor oil, hard Higher fatty acid ester-based lubricants such as butyl acrylate, ethylene glycol monostearate, pentaerythritol (mono, di-, tri- or tetra) stearate; cetyl alcohol, stearyl alcohol, Alcohol-based lubricants such as polyethylene glycol and polyglycerin; lauric acid, myristic acid, palmitic acid, stearic acid, arachidic acid, behenic acid, ricinoleic acid (1^(:丨11〇1€丨0 3 (: 丨 (1), ring-burning acid, etc., metal soaps of metal salts such as catching, tin, lock, zinc, and wrong; carnauba 0 wax, candeli 1 la wax ), natural waxes such as bee stings, lignite sputum, etc. These lubricants may be used singly or in combination of two or more. It is an amphiphilic substance having a hydrophilic group having no affinity for a solvent and an affinity group (usually water-based) having affinity for a solvent. The type of the surfactant is not particularly limited, for example, The surfactant may be used alone or in combination of two or more. The antioxidant is not particularly limited, and examples thereof include triphenyl phosphate. 69 321346 201004993 Phosphate phenyl isophthalic acid has oxidizing agents such as organic thiopurines such as dipropionate, several hydrazines, phenolic antioxidants such as stearyl-3,3'-sulfur, 2, 6" - The tert-butyl-p-cresol light stabilizer is not particularly benzophenone-based or salicylic acid-salt, and may be exemplified by stupid and tri-salt, second-order ultraviolet absorber, and feline.酉 系 、 、 ' ' ' ' ' ' 本 本 本 本 本 本 本 本 本 本 系 系 系 系 系 系 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改 改(8), phosphor hardener (U) and hardening s edge material (6), &amp; oxygen tree wax (Α' A hardening method for hardening by a cation palm/(1) or a photoacid generator (7), a further epoxy resin catalyst, a modifier, a vinyl ether compound, a hydrazine, a coupling agent, and the like The method of ^/ produces a cured product, wherein the hardening method of the light is cured by the hardening of the epoxy resin, or the generally used one. The 16 V is added as an example of the method suitable for the embodiment or hard: Agents, etc.: different, :::: temperature 2 due to the epoxy resin used

..., particularly limited, but usually in the range of 20 to 20 (TC I. Line or Jia 1 light, UV low pressure mercury lamp, medium pressure water source, for example: / κ silver lamp, surface pressure mercury lamp, super High-pressure mercury lamp, m-extinguishing lamp, metal halide lamp, camplight lamp, crane lamp, Yiyi every shot, false laser, 氦氖 laser, 氪 ion laser, various semiconductor laser, YAG laser, quasi Molecular laser (Excimeriaser), light-emitting diode 321346 70 201004993 official, CRT light source, plasma light source and other light sources. In addition to the reaction can be carried out in the air, but also in the case of nitrogen, helium, argon The reformed resin composition of the present embodiment is, for example, a) the modified resin composition of the present embodiment, and b) the addition of oxygen to the modified resin composition of the present embodiment. a resin composition obtained by cyclizing the compound (D), c) a camphor resin composition obtained by adding a human phosphor (E) to the modified resin composition of the present embodiment, or the above ahc a resin composition obtained by adding a hardener (8) to the middle • It is excellent in adhesion to components or difficult materials (cury material), does not cause cracking, and has excellent brightness for a long period of time. It is excellent for light-emitting element sealing materials; A material for a curable resin composition which is excellent in dimensional stability and is used for producing an optical lens having light resistance. Moreover, the curable resin composition obtained by further adding the curing accelerator (I) to the resin composition obtained by adding the curing agent (η) to the above a) to c), or in the above a) 〇 to c) A photosensitive resin composition obtained by adding a photo-acid generator may be used as the above-mentioned light-emitting element sealing material, or a curable resin composition for producing an optical lens, or a photosensitive resin composition. By using a curable resin composition containing the modified resin composition of the present embodiment, the light-emitting element is sealed, whereby a light-emitting component such as a light-emitting diode can be manufactured. Further, the light-emitting diode and/or the optical lens described above, for example, can be suitably used as a light source such as a liquid crystal display device, a backlight, an illumination, various sensors, a printer, a copy machine, or the like. Sources, signal lights, display lights, display devices, light sources for planar illuminators, 321346 71 201004993 Display semiconductor devices such as ceremonies, decorations, and various lamps. The light-emitting wavelength of the light-emitting element sealed by the sealing material for a light-emitting element which is composed of a curable resin composition having a modified resin composition of the present embodiment is from infrared to red, green to blue, and purple. It is possible to use a wide range of ultraviolet light, and it is possible to use light having a wavelength of from 250 coffee to 55 Å which is deteriorated in light resistance of the conventional sealing material. Therefore, a white light-emitting diode having a long life, high energy efficiency, and high color reproducibility can be obtained. Here, the emission wavelength refers to the wavelength of the main emission peak. Specific examples of the light-emitting element to be used include a light-emitting element formed by laminating a semiconductor material on a substrate. At this time, the semiconductor material can be enumerated as follows:

GaAs, GaP, GaAlAs, GaAsP, AlGalnP, GaN, InN, A1N,

InGaAIN, SiC, etc. Examples of the substrate include sapphire, spinel, SiC, Si, ZnO, and GaN single crystal. A buffer layer may also be formed between the substrate and the semiconductor material as necessary. Examples of such a buffer layer include GaN, A1N, and the like. The method of laminating the semiconductor material on the substrate is not particularly limited, and for example, a MOCVD method, an HDVPE method, a liquid phase growth method, or the like can be used. The structure of the light-emitting element may, for example, be a homojunction having a MIS junction, a PN junction, a PIN junction, a heterojunction, or a double heterostructure. It can also be made into a single or multiple multi-quantum well structure. By using a light-emitting element sealing material comprising a curable resin composition containing the modified resin composition of the present embodiment, the light-emitting element is sealed to produce a light-emitting diode. The seal at this time can seal the light-emitting element only with the light-emitting element sealing material, but it can also be combined with other sealing materials. 72 321346 201004993 = When using other 9 sealing materials, it is used to seal the sealing material. After the completion and sealing, the modified resin grade obtained by the second light-emitting element 4 (4) which is densely sealed with another sealing material is used, and the material is sealed around the material. For other sealing materials, for example, a light-emitting element 葙X can be obtained by using a % resin, a polyoxynium p-imide resin, a surface p (tetra) b sand, a urea resin, or a modified resin composition of the sealing embodiment. The method of sealing the first 7L member may be, for example, a mold frame in which a light-emitting element sealing material is preliminarily injected, and a surface in which the light-emitting element + - ' is fixed after the ten-dip is fixed is applied to the mold into which the light-emitting element has been inserted. A light-emitting element sealing material is injected into the frame, and a method of refining or the like is performed. In this case, the method of injecting the light-emitting element sealing material may be, for example, injection molding from a dispenser, transfer molding (transfer molding), injection molding, or the like. Further, other sealing methods include a method in which a light-emitting element sealing material is dropped onto a light-emitting element, and is applied by stencil printing, screen printing, or a barrier mask to be hardened; In a cup or the like of a light-emitting element, a method of injecting a light-emitting element sealing material by a dispenser or the like and hardening it. The curable resin composition containing the modified resin composition of the present embodiment can also be used as a passivation film which is used as a die bonding material or a die bonding material or a light emitting device in which a light emitting device is fixed to a lead terminal or a package. Package substrate ° The shape of the sealing portion may be, for example, a cannonball type lens shape, a plate shape, a thin film shape, a film shape, or the like. The light-emitting diode ’ obtained by using the modified resin composition of the present embodiment can be improved in performance according to a conventional method. The method for improving the performance includes, for example, a method of providing a light reflecting layer or a light collecting layer on the back surface of the light emitting element, a method of forming a complementary coloring portion on the bottom portion, and providing light having a shorter wavelength than the main light emitting peak on the light emitting element. a layer method, a method of molding a hard material after sealing a light-emitting element, a method of inserting a hair-emitting diode into a through-hole, and fixing the light-emitting element by flip chip A method of connecting to a lead member or the like and connecting the lead member or the like and extracting light from the substrate direction. The light-emitting diodes obtained by using the modified resin composition of the present embodiment include, for example, backlights, illuminations, light sources for various types of liquid crystal displays, sensors, printers, copying machines, and the like. Light-emitting parts such as a light source, an L-shaped lamp, a display lamp, a display device, a light source of a planar illuminator, a display, a decoration, and various lights. On the other hand, a curable resin composition obtained by adding a curing agent (^) to a fluorescent resin composition obtained by adding a polishing agent (E) to the modified resin composition of the present embodiment In the photosensitive resin composition in which the photoacid generator (J) is added to the modified material of the present embodiment, the photosensitive resin composition is cured, whereby a light-storing material having excellent luminosity can be produced. Repeat, start /,, explain the light storage material. In general, a light-storing material is excited by light stimuli such as too poor light, a whole center &amp; , a lamp, and an 'outside line, and the energy is converted and released with ί |τ~[ yjj, β is released to stop the above. After the excitation caused by the number of spurs, the material is still slowly lighted for a long time. 321346 74 201004993 The use of the light-storing material using the modified resin composition of the present embodiment is not particularly limited, and examples thereof include display at nighttime and power failure, disaster prevention and safety signs, clocks, wallpapers, and electric switches. Kanban, clothing, shoes, bicycles, reflectors such as locomotives, adhesive tapes, fishing hooks, buoys and other fishing gear, sports equipment, accessories, access toys, toys, etc. Further, for example, d) a conductive resin composition obtained by adding a conductive metal powder (F) to the modified resin composition of the present embodiment is excellent in fluidity, conductivity, and adhesion, and suppresses voids. In the present embodiment, the insulating resin composition in which the insulating powder (G) is added to the modified resin composition of the present embodiment is used as the raw material of the conductive resin composition. An insulating resin composition obtained by adding an epoxy resin (A,) and an insulating powder (G) to the morphologically modified resin composition, or a curing agent (Η) added to the above d) to f) The resin composition is used as a raw material of an insulating resin composition which is excellent in insulating properties and adhesion and which has curability in suppressing occurrence of voids. Further, in the resin composition obtained by adding the curing agent (11) to the above-mentioned d) to f), a curing resin composition obtained by further adding a curing accelerator (I) or d) to f described above is added. The photosensitive resin composition obtained by adding the photoacid generator (J) may be used as a curable conductive resin composition or a curable insulating resin composition. The use of the conductive resin composition using the modified resin composition of the present invention is not particularly limited, and examples thereof include formation of a semiconductor element and a peripheral member, formation of a conductor wiring, and surface assembly. Replace welding; obstruction, quartz crystal vibrator (qUartz crystai unit) '乂父Μ益, switch machine Yisi injection type and circuit unit, various parts of the seal 321346 75 201004993 installed IC LED + conductor, generator, Rotating machine coils such as motors, coil impregnation, printer wiring boards, transparent substrates instead of glass, medium-sized sub-categories, wire_, connectors, terminals, and other electronic components 'and their use in the class Agent or grain bonding agent; conductive coating material, electrode, printed circuit, conductive resin, etc. 绝缘 An insulating resin made of a modified resin composition of the present invention is used, and the use of the product is not limited. For example, the mounting of a semiconductor wafer (semiconductor chip) in a semiconductor device (m_p enables a semiconductor wafer (IC, LSI, etc.) to be bonded to a ceramic box, a lead frame: a seesaw, etc.) Granule cement, adhesive, etc. Further, it can be applied to semi-crying body seals, intermediaries (interpQser) or printed circuit boards, display T, solar cells, generators, motor substrates, automotive substrates, etc. Use of a highly exothermic insulating material. 0. For example, a) a modified resin composition of the present embodiment, b) a human oxygen heterocyclic T-burning compound (D) is added to the resin composition of the present invention, and c) a fluorescent resin composition obtained by repeating the precursor (E) in the modified resin composition of the present embodiment, and hardening obtained by adding the curing agent _) and the curing accelerator (1). Or in the above a) to c), further adding a photoacid generator 2: a monthly conductivity, for example, 'd) a conductive metal powder (F) of the modified dendrimer in the present embodiment An insulating resin composition obtained by adding an insulating powder G:) to the composition of the present modified form resin, and f) an epoxy resin on and an insulating powder (6) are added to the composition of the present embodiment. Two = 321346 76 201004993 Resin composition, adding hardener (Η) and hard in the d) to Ο The curable resin composition obtained by the chemical accelerator (I) or the photosensitive resin composition obtained by further adding the photoacid generator (J) to the above d) to f) is less susceptible to oxygen The coating agent can be suitably used as the coating agent. The coating agent in the present embodiment is not particularly limited as long as it is a coating material that forms a coating film on the surface of the material, and the main purpose of use is as follows. It is also possible to use a pigment bite pigment or the like as a coating material or an ink in the above-mentioned coating agent as necessary. (1) Protection of coating or substrate, imparting long-lasting and beautiful appearance (protecting and shielding ultraviolet rays) , Infrared, Oxidation, Corrosion, Damage, Dust, Contamination, Temperature, Humidity, etc.) (2) Coating or imparting luster to the substrate (3) Coating or water-repellent processing on the substrate (4) Anti-skid processing of the floor etc.

Insulation (5) Sealing of electronic parts It is generally considered that although the polymerization of the epoxy compound starts quickly, the subsequent aggregation = is not fast. However, the inventors have unexpectedly discovered that by blending an oxygen-heterocyclic filament in a resin composition having a % oxygen group, that is, a photosensitive tree having excellent photocurability and adhesion is used. By selecting an oxetane compound, the viscosity of the resin composition can be lowered. In the photosensitive resin group of the embodiment of the present invention, the readiness of the material in the photosensitive resin group is 4', and the liquidity is 4', preferably 0.05 or more, 50Pa, and 321346 77, the range of 201004993 S or less. Preferably, it is a range of 0.2 or more and 30 Pa·s or less. When the viscosity of the photosensitive resin composition exceeds the circle Pa.s, the fluidity may be impaired, and there may be cases where it is not applicable. The coating agent of the present embodiment is applied by a conventional method, and secondly, a coating film can be formed by curing. At this time, the coating method includes brush coating, roll coating, blow coating, bar coater, intimate coater, burn coating, dip coating, electrodeposition coating, and electrostatic coating. Printing technology such as packaging, powder coating, evaporation, electroplating, inkjet, f-printing, rotary printing, gravure printing, screen printing, etc. On the other hand, the method of forming a coating film is by force. The method of hardening, or the method of hardening by irradiation of light, is applicable. The use of the coating agent and the coating film of the present embodiment is not particularly limited. For example, it can be used as a coating agent (coating, resin, plastic, metal, steel & car, building wood, fiber, etc.) ), coating or subsequent printing of optical discs (DVD, CD, Blu-ray disc, etc.), ink (inkjet printing, gravure printing, flexographic printing, photoresist for printed wiring boards, ϋν printing applications, etc.), printing plate material 〇 ( Photovoltaic (resistance for semiconductors, resist for printed wiring boards, resist for photo processing, etc.), printed wiring boards, ICs, LSIs, etc., ps, photosensitive resin relief, screen printing materials, etc.) Patterning of various electronic components, shirt color filter forming materials for liquid crystal or PDP displays, sealing materials for liquid crystal or organic EL, semiconductors and LED peripheral materials (sealing materials, lens materials, base materials, and die bonding materials) , wafer coating materials, laminates, optical fibers, optical waveguides, filters, adhesives for electronic parts, coating materials, sealing materials, insulating materials, photoresists, encap materials, / Huofu materials ( Potting material), Light transmission through the layer 78 321346 201004993 or interlayer insulation layer, printed wiring board, laminated board, light guide plate, anti-reflection film, etc., coatings (anti-corrosion coating, maintenance, ship coating, etched lining, automotive, electric Primer for products, beverages, beer cans, exterior coating, air-dried coating, general anti-corrosion coating, maintenance coating, woodworking products, automotive plating primer, other industrial electroplating coatings, beverages Coat Coating on the inner surface of beer cans, Coil Coating, drums · Wood coatings on the inner surface of tanks, acid-proof coatings, wire ename 1 , insulating enamel coatings, automotive bottoms Paint, various metal products, beauty and anti-corrosion coating, pipeline interior and exterior coating, electrical parts insulation coating, etc.), composite materials (chemical industry Wei pipelines; tanks, aircraft materials, automotive materials, Various sporting goods, carbon fiber composites, aramid fiber composites·#), civil construction materials (flooring, paving, film, non-slip and thin layer paving, concrete joints • heightening Engineering, anchor Fill in the following, concrete joints, ceramic tile, concrete structure crack repair, base / 3⁄4 slurry coating, water tank or sewer facilities, anti-surname, waterproof coating, sump storage type Materials, anti-rice coating of iron structures, clay coating on the outer wall of buildings, etc.), adhesives (metal, glass, ceramics, cement concrete, wood, plastic equivalents or adhesives of different materials, automotive, iron). Road vehicles, adhesives for assembly such as airplanes, adhesives for prefabricated composite panels, etc.: one-liquid type, two-liquid type, sheet type), aircraft, automobile, plastic forming tools (pressure mold, drawing die) (removing (j die), resin molds such as molds, vacuum forming, blow molding molds, master models, casting patterns, build-up tools, various inspection tools, etc.) , modifiers and stabilizers (resin processing of fibers, 79 321346 201004993 stabilizer for polyvinyl chloride, additives for synthetic rubber, etc.). It is useful for the use of a coating agent, a coating material, an adhesive, and a photo-forming resin. In the example of the embodiment, the embodiment of the present embodiment will be specifically described, and the state is not to exceed the gist of the present invention, that is, the following example 1 S 26 and the comparative example! The evaluation of the physical properties to 9 is carried out. ο &lt;Epoxy equivalent (WPE)&gt;, measured according to "JISK 7236: 2GG1 (Method for calculating epoxy of epoxy resin wax)". Field &lt;Viscosity&gt; The measurement was carried out under the following conditions. Rotary E-shaped viscometer · · Dongji Industry Co., Ltd., "n_22 type converter: 3 ° x R14 (other rotators can be selected if necessary) Measuring temperature: 25 ° C ° ❹ Sample size: 〇. 4 ml <calculation of the target index &> The mixing index α is calculated by the following general formula (2). Mixed index a=((2c)/((2b) (2) Here, Q :b: (8) In the general formula (1), n = 1 or 2 and at least one of the cyclic two soils as the alkoxydecane compound of the R group, m 〇 1% of the family ac: («, in the general formula (1), n=l or 2 and at least having a kind of aromaticity, and the machine base is m〇1% of the alkoxy compound of R. 321346 80 201004993 &lt;calculation of mixing index &&gt; The mixing index β is the following general formula (3) Calculation. Mixed index/5={(βη2)/(point n0+/Snl)} (3) Here, cold n2: In the general formula (1), the mol of the alkoxydecane compound of n=2 % cold nO : In the general formula (1), n = mol% of the alkoxy decane compound of hydrazine cold nl: in the general formula (1), η = ι alkoxy decane compound m 〇 l0 / 0 , but satisfy OS Κ/3η〇)/(βη〇+ y3nl+ y5n2)}S0. 1 〇<mixing index r Calculation &gt; The mixing index T is calculated by the following general formula (4): Mixed index 7 = (7 a) / (rs) (4) Here, 7 a : quality of epoxy resin (g), rs: - In the general formula (1), the mass (g) of the alkoxydecane compound of n: =0 to 2. ❹ <Calculation of the mixing index 5> The mixing index Θ is calculated by the following general formula (5). =Ue)/((5s) (5) Here, de: the amount of addition of the hydrolysis condensation catalyst (number of moles), : the amount of (0R2) in the general formula (1) (number of moles). Calculation of £&gt; The storage index ε is calculated by the following general formula (6). Mixed index e=(ew)//Us) (6) 81 321346 201004993 Here, ε w : water addition amount (mo 1 number) , es: The amount of (OR2) in the general formula (1) (number of moles). &lt;Calculation of the mixed index f&gt; The mixed index Γ is calculated by the following general formula (Ό. Mixed index Γ = (ΓΟ/ (Γ1〇(7) Here,

Tf : the amount of the hardener added (mol number), rk: the amount (mol number) of the cyclic ether group contained in the epoxy resin and the alkoxydecane compound. &lt;Calculation of Mixed Indicators 7?&gt; Mixed Indicators? ? It is calculated by the following general formula (8). Mixed indicators? ? =( 7? g)/( ?? k)xl00 (8) Here, C g : the mass of the hardening accelerator (g), ?? k : the mass of the epoxy resin and the alkoxy chopping compound (g) . &lt;Preservation stability of the stability index 保存, and storage stability of the resin composition &gt; The storage stability in the resin composition is evaluated by the storage stability index 0 shown by the following general formula (9). Preservation stability index 0 = (preservation viscosity) / (starting viscosity) (9) The container of the resin composition immediately after manufacture is sealed, and the temperature is adjusted at 25 ° C for 2 hours, and then measured at 25 ° The viscosity in C is taken as the "starting viscosity". 82 321346 201004993 Further, the container of the resin composition was sealed and stored in a 25 ° (: incubator for 2 weeks. After storage, the viscosity at 25 ° C was measured, and this was taken as "preservation viscosity". When the resin composition has fluidity (viscosity is 1 〇〇〇pa·s or less) and the storage stability index 0 is 4 or less, it is judged to have storage stability. <H-NMR measurement of the intermediate> Condensation of the intermediate The rate is determined by H-NMR measurement of the sample solution (intermediate) taken after the completion of the refluxing step, and is obtained by the following procedure. 6 (1) In the sample bottle, the 3 〇nig reflux step is completed. After the sample solution was added to the gas-form-d (manufactured by Wako Pure Chemical Industries, Ltd.), it was adjusted to ig. (2) The solution of the above (1) was transferred to an NMR tube having a diameter of 5 mm Φ, as follows. Conditions, measurement of H-NMR. Fourier transform nuclear magnetic resonance apparatus: "α-400 type" manufactured by Nippon Denshi Co., Ltd. Nuclear species: Η 〇 Cumulative number: 200 times <Residual oxyl group in modified resin composition Calculation of amount: H-NMR measurement &gt; H-NMR measurement is performed by the following steps (1) In the sample bottle, weigh 1 mg of the modified resin composition and 2 〇mg of the internal standard substance (1,1,2,2-tetrabromoethane; Tokyo Chemical Industry Co., Ltd.), and add the gas. Imitation-d (manufactured by Wako Pure Chemical Industries, Ltd.) 970 mg was dissolved and prepared. (2) The solution of the above (1) was transferred to an NMR tube having a diameter of 5 mm Φ, and H-NMR was measured under the following conditions. Conversion nuclear magnetic resonance apparatus: "321346 83 201004993 400 type" manufactured by Sakamoto Electronics Co., Ltd. Nuclear species: 累积 Cumulative number: 200 times From the above measurement results, the amount of residual alkoxy groups (%) is calculated according to the following procedure. (3) The H-NMR chart calculates the area value of the peak derived from the residual alkoxy group. (4) Calculates the area value of the peak derived from the internal standard substance from the H-NMR chart. (5) Read the above (3) and 4), the area value is substituted into the following formula to calculate the amount of residual alkoxy group (%). The amount of residual alkoxy group (%) = (area value derived from the peak of the residual alkoxy group) / (from the internal standard) The area value of the peak of the substance) x 100 Here, the area value of the peak derived from the residual alkoxy group is calculated by the following method. When the peak of the residual alkoxy group is a single peak &gt; ◎ The area of the portion surrounded by the baseline and the peak is regarded as the area value derived from the peak of the residual alkoxy group. The peak derived from the residual alkoxy group may be present in plural. In this case, the area value of the peak derived from the residual alkoxy group in the present embodiment is the sum of the areas of the plurality of bees derived from the residual alkoxy group. &lt;When the peak derived from the residual alkoxy group is a complex peak&gt; starts from a point where the slope between the peak derived from the residual alkoxy group and the peak derived from the residual alkoxy group is 0 The area of the peak derived from the residual alkane 84 321346 201004993 is derived from the area of the peak surrounded by the peak of the residual (tetra)oxy group from the peak of the wiring and the residual alkoxy group. The product value is taken as the source, and the peak of the residual oxy group is the wave bee... (4) When there is no point with a slope of G between the peak of the private base and the main generation of w = Waves: Not considered a wave bee, the wave bee is all regarded as a source bee. Further, when the peak derived from the residual oxy group is the wave of the oxy group and the peak derived from the residual alkoxy group is derived from the residual main component, there is no slope between the 主 and _ = The crest is the peak. The peak of Α is not regarded as &lt;Light resistance test of hardened material&gt; The light resistance of the cured product was evaluated by the following method. (1) The cured product prepared by the method described later was hardened to prepare a cured product having a thickness of 20 mm x 10 mm x 3 mm. clothes

(2) The cured product was covered with a black mask of 25 mm x 15 min x thickness 1.2 ram having a diameter of 5. 5 mni as a sample for light resistance test. (3) The preparation device is configured to illuminate the UV light from the UV irradiation device ("50〇1:(:1^^5?7-25〇1)8") manufactured by Ushi0 Electric Co., Ltd.) via an optical fiber. The above sample in an incubator at a constant temperature of 50 °C. (4) The above sample was placed in an incubator at 50 ° C in a state where the black mask was placed on the top. (5) UV light of 2 W/cm2 was irradiated for 96 hours from the upper portion of the cover of the 321346 85 201004993 by irradiating the UV light to a hole having a diameter of 5. 5 mm. (6) The spectroscopic color meter ("SD5000" manufactured by Sakamoto Electric Co., Ltd.), which has been modified into a diameter of 10 mm, was used to measure the sample irradiated with UV. (7) Yellowness (Π) is based on “ASTM D1925-70U988: Test Method for Yellowness Index of Plastics”. When this YI is 13 or less, it is judged that it has light resistance. &lt;Cold and thermal shock test of hardened material&gt; 评估 The thermal shock resistance of the cured product was evaluated by the following method. (1) A substrate and a germanium wafer as shown below are prepared. (1-1) Substrate, manufactured by Solvay Advanced Polymers Co., Ltd., "AMODEL A-4122NL WH 905" (a hole having a diameter of 1 〇mmx and a depth of 1. 2 mm in the center of a flat plate of 15 mm x 15 mm x 2 mm) (1-2) Each of the wafer cassettes (2) is prepared by injecting a solution for a cured product prepared by a method described later into the substrate, and one wafer is placed therein, and the cured person is used as a sample for a thermal shock test. (3) The above-mentioned sample women's clothing is used in a thermal shock device ("Espec", "TSE-11-A"), at "(_4〇. (: to 120 °C) / cycle: exposure time 14 In the minute, the temperature rise and fall time is 1 minute, the heat cycle is performed. (4) The sample is taken out after 50 cycles of heat, and the permeate ("MICRO-CHECK" manufactured by K0HZAI Co., Ltd.) is used. Spray, view 321346 86 201004993 Check for abnormalities (peeling or cracking) and record the number. (5) After the above (4) confirmed that there is no abnormality, the sample is placed again in the device, and after 50 cycles of thermal cycling, After doing the same operation and evaluating, secondly, perform 100 thermal cycles and evaluate them in the same way. Repeat these operations and evaluate them. (6) When two of the 10 samples are seen as abnormal, the evaluation is interrupted. The number of times of thermal shock resistance = (the number of thermal cycles interrupted) - (50 times) was obtained. When the number of thermal shock resistances was 50 or more, it was judged to have the resistance to hot and cold impact, as determined below. The above is less than 100 times: 〇 100 times or more: ◎ About Examples 1 to 26 and Comparative Examples 1 to 9 The raw materials used are indicated in the following (1) to (9). (1) Epoxy resin (1-1) Epoxy resin A1: Poly(bisphenol A-2-hydroxypropyl ether) (hereinafter, Q It is called Bis-Al epoxy resin.) • Trade name: manufactured by Asahi Kasei Epoxy Co., Ltd., “AER2600” In addition, the epoxy equivalent (WPE) and viscosity measured by the above method are as follows. • Epoxy equivalent (WPE) ) : 187g /eq • Viscosity (25°C) : 14. 3 Pa · s (1-2) Epoxy Resin A2 : Poly(bisphenol A-2-hydroxypropyl ether) (hereinafter referred to as Bis-A2 Epoxy) Resin) • Product name: Asahi Kasei Epoxy Co., Ltd., "AER2500" 87 321346 201004993 In addition, the epoxy equivalent (WPE) and viscosity measured by the above method are as follows. • Epoxy equivalent (WPE): l86g/ Eq • Viscosity (25 C ) : 1 〇. 2 Pa · s (1-3) Epoxy Resin A3 : Poly(bisphenol A-2-hydroxypropyl ether) (hereinafter referred to as Bis-A3 Epoxy Resin) • Goods Name: Asahi Kasei Epoxy Co., Ltd., r AER6〇71" ❹ And the epoxy equivalent (WPE) measured by the above method is as follows. However, the epoxy resin A3 is solid at 25 ° C, so it cannot be Determination of viscosity • Epoxy equivalent (WPE): 470g/eq (1 -4) Epoxy resin B: 3,4-epoxycyclohexyl-fluorenyl-3',4'-epoxycyclohexyl carboxylate (hereinafter referred to as Epoxy resin) • Trade name: manufactured by Daicel Chemical Industry Co., Ltd., “ceii〇xide 2021P” The epoxy equivalent (wpE) and viscosity measured by the above method are as follows. • Epoxy content (WPE): 131 g/eq • Viscosity (25t): 227 mPa · s (2) Calcined base-based calcined compound (2~1) alkoxylated compound H:3-glycidyloxy Propyltrimethoxy decane (hereinafter referred to as GPTMS) • Trade name: Shin-Etsu Chemical Co., Ltd., "KBM_4〇3" (2~2) alkoxydecane compound 丨: phenyl tridecyloxy矽 ( 以下 以下 ( 88 88 88 88 88 It is called DMDMS) • Product name: Shin-Etsu Chemical Co., Ltd., "KBM-22" (2-4) Alkoxydecane compound K: Tetraethoxydecane (hereinafter referred to as TEOS) • Trade name: Shin-Etsu Chemical Industry Co., Ltd., "KBE-04" (2-5) alkoxydecane compound L: 2-(3,4-epoxycyclohexyl)ethyltrimethoxy decane (hereinafter referred to as ECETMS) • Product name: Shin-Etsu Chemical Co., Ltd., "KBM-303" (3) decane partial condensate (3-1) tetramethoxy decane partial condensate (alias: polyoxy methoxy oxane) (hereinafter referred to as P-MS) • Trade name: Fusang Chemical Industry Co., Ltd., “Methyl decanoate 51” (3-2) Mercapto trioxy decane partial condensate (alias: poly(methyl trimethyl) Oxydecane) (hereinafter referred to as P-MTMS) • Trade name: manufactured by Tama Chemical Industry Co., Ltd., "MTMS-A" (4) Solvent (4-1) Tetrahydrofuran: manufactured by Wako Pure Chemical Industries Co., Ltd. Contains no stabilizer (hereinafter referred to as THF) (4-2) Ethanol: Wako Pure Chemical Industries Co., Ltd. (hereinafter referred to as EtOH) (4-3) Isopropanol: Wako Pure Chemical Industries Co., Ltd. (below) Abbreviation i-PrOH) 89 321346 201004993 (5) Hydrolysis condensation catalyst (5-1) Dibutyltin dilaurate: Wako Pure Chemical Industries Co., Ltd. (hereinafter referred to as DBTDL) (5-2) Dibutyltin diacetate: Tokyo Chemical Industry Co., Ltd. (hereinafter referred to as DBTDA) (5-3) Dioctyltin diacetate: manufactured by Yudong Chemical Co., Ltd., "Neostann U-820" (hereinafter referred to as D0TDA) (6) Hardener : "4-Mercaptohexahydrophthalic anhydride / hexahydrophthalic anhydride = 70/30"

® • Trade name: New Japan Physical and Chemical Co., Ltd., “RIKACID MH-700Gj (7) Hardening accelerator: Amine hardener • Trade name: “U-CAT 18X” by San-apro Co., Ltd. ( 8) Polyxylene resin: "SCR-1012CA liquid and liquid B" manufactured by Shin-Etsu Chemical Co., Ltd. (9) Inorganic filling material: colloidal cerium oxide Q • Trade name: Nissan Chemical Industry Co., Ltd. System, "nonanol dioxide sol" (Si〇2: 30%, particle diameter: 10 to 20 nm) (10) Internal reference material 1,1,2, 2-tetrabromoethane: manufactured by Tokyo Chemical Industry Co., Ltd. [ Example 1] The resin composition was produced and evaluated by the following procedure. (1) Preparation: The circulating constant temperature water tank was set to 5 ° C to return to the cooling pipe. Further, an 80 ° C oil bath was placed on a magnetic stirrer. 90 321346 201004993 (2) According to the composition ratio of Table 1 'Bis ai oxy-resin, alkoxy decane compound and THF are added to the flask which has been thrown in % of the collection under the environment of 25t, and after mixing and stirring, further added Water and water two: Catalyst, mixed and given. , (3) Next, install a cooling tube in the flask, and quickly immerse it in 8 (Γ(:, &, by, and start stirring) while refluxing for 7 hours (reflow step cold (4) after the reaction is completed, Cool to 25 ° C ' and then remove from the flask to cool it. After the end of the reflux step, 'take the sample solution (intermediate). ® (5) After the end of the reflux step, determine the sample solution (intermediate). (OR2) of formula (1) is hydrolyzed to (OH) (R^n-Si-COR2)^ (1) (6) The solution after the reflux step is finished using 'evaporator at 4〇〇pa, 50 ° After the distillation was carried out for 1 hour, the mixture was further subjected to dehydration condensation reaction (dehydration condensation step) at 8 (rc) for 5 hours. (7) After completion of the reaction, the mixture was cooled to 25 ° C to obtain a resin composition. When the H-NMR of the resin composition of the tree was measured and calculated together with the internal standard substance, the amount of residual alkoxy group was 0% by weight 5%. (8) The mixing index α 1 to e 1 of the resin composition is shown in the table. (3) Further, the epoxy equivalent (WPE), the initial viscosity, and the resin composition obtained in the above (6) are measured by the above method. Further, the storage stability index 61 1 ' was obtained and expressed in Table 3. The epoxy equivalent (WPE) = 230 g / eq' of the resin composition of the above Example 1 showed an appropriate value. And 'starting viscosity=32. 7 Pa· s &lt; 1000 Pa · s 'and, preservation viscosity = 46. 4 Pa · s &lt; 1000 Pa · s, both are 91 321346 201004993 liquid with fluidity. The storage stability index 0 1 = l 42 s 4 was determined, and it was judged that the resin composition having the stability was stored. Next, the cured resin was stored and evaluated by the following procedure using the resin composition stored at 25 ° C for 2 weeks. (10) The resin composition, the curing agent, and the hardening accelerator are mixed and mixed according to the composition ratio of Table 2 in an environment of 25 C, and degassed under vacuum to obtain a solution for the cured product. 〇〇 1) Thickness 3 The 3D shape of the 矽 rubber 挟 is made between two stainless steel sheets coated with a release agent. (12) For the molding jig and one of the above substrates for the thermal shock test, the above-mentioned A solution for the hardened material, and one piece of the dream wafer was placed in each of the substrates. (13) The above-mentioned molding jig and the substrate for thermal shock test were placed in an oven, and hardened at 1 hour and further at 150 ° C for 1 hour to produce a cured product. After the internal temperature of the oven has dropped to 3 〇t or less, the cured product is taken out, and the sample for light resistance test and the sample for thermal shock test are prepared according to the above method. (15) Light resistance is measured by the above method using the above sample. The results of the test and the thermal shock test are shown in Table 3. The indicator of the light resistance of the cured product is YI = 1 (US13, which is judged to have light resistance. Furthermore, the number of tests for cold and hot shock is sub-^{{) times, and it is judged that there is resistance to cold and heat. From the above results, it is known. In the embodiment i, the composition of the tree has a fluidity, and the stagnation of the sputum is a sputum. The cured product of the resin composition has light resistance and 92 201004993 resistance to cold and thermal shock, so it is judged to be qualified. [Example 2] A product and a cured product were obtained in the same manner as in Example 1. The resin group α? δ ρ 9 „ will be produced with the manufacturer 2'. The result of the method is estimated, the mixture is captured to £2, and the stability formula is used to confirm the intermediate (10) in the above formula (1). Water 2 Table 3... The amount of the base of the resin composition and the internal standard substance is 0% S5%. 残留ίβ residual Shen Gongyi

"Table 3" shows that the epoxy equivalent of the composition of the composition ^ 231g / eq ' is not appropriate. Also, the starting point = ιι 1000Pa.s^XM^#i^ = 17. 〇Pa.s&lt;i〇〇〇paes^ are all liquids with fluidity. Further, the storage stability index ^ = 1 4 ' was determined to have a resin composition for preservation stability. Further, the index of the light resistance test of the cured product ΥΙ = 8. 3^13, and it was judged to be rich in light. Further, the number of thermal shock tests was 5 〇〇 or more and 5 〇 times, and it was judged that there was resistance to thermal shock. From the above results, it is understood that the resin composition of the second embodiment has fluidity and storage stability, and that the cured product of the resin composition has light resistance and thermal shock resistance. [Example 3] A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables 1 and 2. The results of evaluation in the same manner as in Example 1, the mixed indexes α3 to ε3, and the storage stability index Θ3 are shown in Table 3. Further, it was confirmed that (0R2) in the above formula (1) of the intermediate was hydrolyzed to (〇Η). 321346 93 201004993 The residual graft oxygen content calculated from the resin composition and internal reference materials is 0%$5%. Epoxy equivalent of the resin composition of Example 3 as shown in Table 3 (WPE^

253g/eq ' shows the appropriate value. Also, the initial viscosity = 27. · S ς, rain lOOOPa · s, and 'save viscosity = 39. 6Pa · s &lt; 100 〇 Pa ι 4-5 ^ are liquids with fluidity. Further, the stability index Θ 4 was stored, and it was judged that there was a resin composition for preserving stability. At the same time, the indicator of the light resistance test of the cured product ΥΙ=9.2$13 ’ ® is light-resistant. Further, the number of thermal shock tests was 500 or more and 50 +, and it was judged that there was resistance to thermal shock. From the above results, the resin composition of Example 3 has "IL" and storage stability, and the cured product of the resin composition has light resistance and thermal shock resistance. [Example 4] In the same manner as in Example 1, according to Tables 1 and 2, a wax composition and a cured product were produced. The results of the evaluation in the same manner as in Example ι, the mixed indexes "4 to ε4, and the security qualitative index Θ 4 are shown in Table 3. Further, it was confirmed that (OR2) in the above formula (1) of the intermediate was hydrolyzed to (0H). The amount of residual alkoxy groups calculated from the resin composition and the internal standard material was 0% S5%. As shown in Table 3, the epoxy equivalent of the resin composition of Example 4 (liver £) - 208 g/eq, Suitable for the value. Also, the initial viscosity = pa · s &lt; lOOOPa · s, and the preservation viscosity = 16·7Pa · s &lt; i〇〇〇pa · s, both are liquid liquids. Further, the storage stability index Θ 4 = i 43 321346 94 201004993 $4' is determined to have a resin composition for preserving stability. Further, the indicator of the light resistance test of the cured product was γι = 8. 7 $13, and it was judged to have light resistance. Further, the number of thermal shock tests was 45 〇 25 times, and it was judged to have thermal shock resistance. From the above results, it is understood that the resin composition of the fourth embodiment has fluidity and storage stability, and the cured product of the resin composition has light resistance and thermal shock resistance. [Example 5] 树脂 In the same manner as in Example 1, a resin composition and a cured product were produced in accordance with Tables 1 and 2. The results of evaluation in the same manner as in Example 1, and the mixing indexes α 5 to ε 5 and the storage stability index 0 5 are shown in Table 3. Further, it was confirmed that (〇R2) in the above formula (1) of the intermediate was hydrolyzed to (10)). The amount of residual alkoxy groups calculated from the resin composition and the internal standard material is. As shown in Table 3, the epoxy equivalent (wpE) of the resin composition = 245 〇 g / eq, which showed a suitable value. Further, the initial viscosity = 13.2 Pa.s &lt; 1000 Pa·s, and the storage viscosity = 18.7 Pa·s &lt; round pa·s, both of which are fluid liquids. Further, the stability index 05 = 1.42 $4 was stored, and it was judged that the resin composition having the stability was stored. Further, the indicator 50.0 of the light resistance test of the cured product was judged to have light resistance. Moreover, the number of thermal shock tests was 25 ^^5 〇 times, and it was judged that there was a cold and thermal shock. From the above results, the resin composition of Example 5 has fluidity and storage stability, and the cured product of the resin composition has (4) optical properties and resistance to thermal shock resistance of 321346 95 201004993. [Example 6] A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables 1 and 2'. The results of the evaluation in the same manner as in Example 1, the mixing indexes α 6 to £ 6, and the storage stability index Θ 6 are shown in Table 3. Further, (〇r2) in the above formula (1) which confirms the intermediate is hydrolyzed to (0Η). The amount of residual alkoxy group calculated from the resin composition and the internal standard material was 0% by weight. 〇 As shown in Table 3, the epoxy resin equivalent (WPE) of the resin composition of Example 6 was 221 g/eci, which showed an appropriate value. Further, the initial viscosity = 18.2 Pa · s &lt; lOOOPa · s, and the preservation viscosity = 26. 6 Pa · s &lt; 1000 Pa · s, both are liquid liquids. Further, the storage stability index Θ6=1.46$4 was determined, and it was judged that there was a resin composition for preserving stability. Further, the indicator of the light resistance test of the cured product ΥΙ = 8. Κ 13, and it was judged to have light resistance. Furthermore, the number of thermal shock tests was 350 times ^ 50 times. Q was judged to have thermal shock resistance. From the above results, it is understood that the resin composition of the sixth embodiment has fluidity and storage stability. Further, since the cured product of the resin composition has light resistance and thermal shock resistance, it is judged to be satisfactory. [Example 7] A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables 1 and 2'. The results of evaluation in the same manner as in Example 1, the mixed indexes α 7 to ε 7 , and the storage stability index Θ 7 are shown in Table 3. Further, it is confirmed that (〇R2) in the above formula (1) is hydrolyzed to (0Η). 96 321346 201004993 The amount of residual alkoxy groups calculated from the resin composition and internal reference materials is 0%$5%. As shown in Table 3, the epoxy equivalent (WPE) of the resin composition of Example 7 was 217 g/eq, which showed an appropriate value. Further, the initial viscosity = 10.3 Pa · s &lt; lOOOPa · s, and the preservation viscosity = 14. 5 Pa · s &lt; lOOOPa · s, both of which are fluid liquids. Further, the storage stability index 0 7 = 1.41 S 4 was determined, and it was judged that there was a resin composition for preserving stability. Further, the indicator of the light resistance test of the cured product was YI=8. 3^13, and it was judged that the light resistance was light. Further, the number of thermal shock tests was 450 times and 450 times, and it was judged that there was resistance to thermal shock. From the above results, the resin composition of Example 7 has fluidity and storage stability, and the cured product of the resin composition has light resistance and thermal shock resistance. [Example 8] In the same manner as in Example 1, according to Tables 1 and 2, a resin composition Q material and a cured product were produced. The results of evaluation in the same manner as in Example 1, the mixed indexes α8 to e8, and the storage stability index Θ8 are shown in Table 3. Further, it was confirmed that (OR2) in the above formula (1) of the intermediate was hydrolyzed to (0Η). The amount of residual alkoxy groups calculated from the resin composition and the internal standard material is. As shown in Table 3, the epoxy resin equivalent (WPE) of the resin composition of Example 8 was 213 g/eq, which showed an appropriate value. Also, the initial viscosity = 10. 6 Pa · s &lt; lOOOPa · s, and the preservation viscosity = 15. 3 Pa · s &lt; lOOOPa · s, both are liquid liquids. Further, the storage stability index 0 8 = 1.45 S 4, 97 321346 201004993 It was judged that there was a resin composition for preserving stability. Further, the indicator YI of the light resistance test of the cured product was 7.6, and it was judged to have light resistance. Further, the number of thermal shock tests was 150 times 2 50 times, which was judged to be resistant to thermal shock. From the above results, it can be seen that the resin composition of the eighth embodiment has fluidity and storage stability, and that the cured product of the resin composition is rich in light and thermal shock resistance. 9] A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables 1 and 2'. The results of evaluation in the same manner as in Example 1, the mixed indexes α9 to ε9, and the storage stability index Θ9 are shown in Table 3. Further, it was confirmed that (〇R2) in the above formula (1) of the intermediate was hydrolyzed to (ΟΗ). The amount of residual alkoxy groups calculated from the resin composition and the internal standard material is. As shown in Table 3, the epoxy resin equivalent (WPE) ❹ = 235 g/eq of the resin composition of Example 9 showed an appropriate value. Further, the initial viscosity = 27.8 Pa · s &lt; lOOOPa · s ' and the storage viscosity = 28.6 Pa · s &lt; lOOOPa · s ' Both are fluid liquids. Further, the storage stability index 0 9=1. 03$4 was determined as a resin composition having a storage stability. Further, the indicator YI = 8 · 0S13 ' of the light resistance test of the cured product was judged to have light resistance. Further, the number of thermal shock tests was 350 times ^ 50 times, and it was judged to have thermal shock resistance. From the above results, it is understood that the resin composition of the ninth embodiment has fluidity and storage stability, and that the cured product of the resin composition has light resistance and thermal shock resistance. [Example 10] A tree wax composition and a cured product were produced in the same manner as in Example 1 according to Tables 1 and 2. The results of evaluation in the same manner as in Example 1, the mixed indexes α10 to ε 10, and the storage stability index Θ10 are shown in Table 3. Further, it was confirmed that (0R2) in the above formula (1) of the intermediate was hydrolyzed to (〇Η). The residual alkoxy group calculated from the resin composition and the internal standard material was 〇% S5%. As shown in Table 3, the epoxy equivalent (??) of the resin composition of Example 10 = 214 g/eq, which showed an appropriate value. Also, the initial viscosity = 13. 2 Pa · s &lt; lOOOPa · s, and the storage viscosity = 13. 7 Pa · s &lt; lOOOPa · s, both are liquid liquids. Further, the storage stability index Θ l〇=i. 04$4 was judged to have a resin composition for preserving stability. Further, the indicator of the light resistance test of the cured product ΥΙ = 7. 8^13, and it was judged to have light resistance. In addition, the number of thermal shock tests was 45 ^ ^ 5 〇 times, and the ❹ was determined to have thermal shock resistance. From the above results, the resin composition of Example 10 has fluidity and preserves virginity, and the cured product of the resin composition has light resistance and thermal shock resistance. [Example 11] A resin composition and a cured product were produced in accordance with Tables 1 and 2 in the same manner as in Example 1. Will be with the real side]! (5) The result of the sample Fangnu Nu, the mixed indicator heart to ^, and the preservation of the W index W shirt. Further, it is confirmed that (4) of the 4th type (1) towel is hydrolyzed to (4). 99 321346 201004993 The amount of residual alkoxy group calculated from the resin composition and the internal standard substance is 0% by weight 5%. As shown in Table 3, the epoxy equivalent (WPE) of the resin composition of Example _ is 228g/eq. Show the appropriate value. Further, the initial viscosity = 41. IPa · s &lt; 1000 Pa · s ' and the preservation viscosity = 65 · 8 Pa · s &lt; lOOOPa · s, both of which are fluid liquids. Further, the stability index 0 11 = 1. 60S4 was stored, and it was judged that there was a resin composition for preserving stability. Further, the index of the light resistance test of the cured product was YI = 7. 5S 13, and it was judged to have light resistance. Further, the number of thermal shock tests was 450 times 2 50 times, and it was judged to have thermal shock resistance. From the above results, it is understood that the resin composition of the eleventh embodiment has fluidity and storage stability. Further, the cured product of the resin composition is rich in light and thermal shock resistance. [Example 12] A resin composition of a sputum and a cured product was produced in the same manner as in Example 1 in accordance with Table 2 and Table 2. The results of evaluation in the same manner as in Example 1, the mixed indexes α12 to ε12, and the storage stability index 012 are shown in Table 3. Further, it was confirmed that (0R2) in the above formula (1) of the intermediate was hydrolyzed to (〇{1). The amount of residual alkoxy group calculated from the resin composition and the internal standard material was 0% by weight. As shown in Table 3, the epoxy equivalent (wpf:) = 23 〇 g / eq' of the resin composition of Example 12 showed an appropriate value. Further, the initial viscosity = 33 7pa.s < circle ? &amp;.3, and the 'preservation viscosity = 48 genus. 3 &lt; 1 () qing ^, both are fluid liquids. Further, the preservation stability (four) standard Chuan = 1 * (6), 321346 100 201004993 was determined to have a resin composition for preservation stability. Further, the index of the light resistance test of the cured product was YI = 9. 8S 13, and it was judged to have light resistance. Further, the number of thermal shock tests was 45 times and 50 times, and it was judged that there was resistance to thermal shock. From the above results, it is understood that the resin composition of Example 12 has fluidity and storage stability, and further, the cured product of the resin composition has calendering properties and thermal shock resistance. [Example 13] A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables 1 and 2. The results of evaluation in the same manner as in Example 1, the mixed indexes α 13 to ε 13 , and the storage stability index Θ 13 are shown in Table 3. Further, it was confirmed that (0R 2) in the above formula (1) of the intermediate was hydrolyzed to (〇Η). The amount of residual alkoxy groups calculated from the resin composition and the internal standard material is 〇%$5%. As shown in Table 3, the epoxy resin equivalent (WPE) ❹ = 253 g/eq of the resin composition of Example 13 showed an appropriate value. And 'starting viscosity=27. 5Pa· s&lt; 1〇00

Pa · s, and the storage viscosity = 40. 8Pa · s &lt; lOOOPa · s, both are liquid liquids. Further, the storage stability index θ 13 = 1.4854 was determined, and it was judged that there was a resin composition for preserving stability. Further, the indicator YI of the light resistance test of the cured product was 9.9S13, and it was judged to have light resistance. Further, the number of thermal shock tests was 450 times ^ 50 times', and it was judged that there was resistance to thermal shock. From the above results, the resin composition of Example 13 has fluidity and storage stability, and further, the cured product of the resin composition has light resistance and J01 321346 201004993 resistance to thermal shock resistance. [Example 14] The same procedure as in Example 1 was carried out except that the curing temperature of (12) of Example 1 was changed to 110 ° C for 4 hours, and further 150 ° C for 1 hour. And 2, making a resin composition and a cured product. The results of evaluation in the same manner as in Example 1, the mixing index α 14 to ε 14 , and the storage stability index Θ 14 are shown in Table 3. Further, it was confirmed that (0R2) in the above formula (1) of the intermediate was hydrolyzed to (0Η). The amount of residual alkoxy groups calculated from the resin composition and the internal standard material is. As shown in Table 3, the epoxy resin equivalent (WPE) of the resin composition of Example 14 was 192 g/eq, which showed an appropriate value. Further, the initial viscosity = 1.77 Pa · s &lt; lOOOPa · s, and the storage viscosity = 3. 08 Pa · s &lt; 1000 Pa · s, both are fluid liquids. Further, the stability index θ 14=1. 74 S4 was stored, and it was judged that the resin composition having the stability was stored. In addition, the indicator of the fiscal property test of the cured product ΥΙ = 5. 2S 13, and it is judged to be rich in luminosity. Further, the number of thermal shock tests was 150 times and 150 times, and it was judged that there was resistance to thermal shock. From the above results, the resin composition of Example 14 has fluidity and storage stability. Further, since the cured product of the resin composition is rich in light and thermal shock resistance, it is judged to be qualified. [Example 15] A resin composition was produced in the same manner as in Example 1 except that the curing temperature of (13) of Example 1 was changed to 110 ° C for 4 hours, in accordance with Table 1 and 2, 102 321 346 201004993. With hardened matter. The results of the evaluation of the same method as in Example 1, the mixing index α 15 to ε 15 , and the storage stability index Θ 15 are shown in Table 3. Further, it was confirmed that (〇R2) in the above formula (1) of the intermediate was hydrolyzed to (邡). The amount of residual alkoxy groups calculated from the resin composition and internal standard materials was 〇%$5%. The epoxy equivalent (WPE) of the resin composition of Example 15 as shown in Table 3.

= 2i4g / e (l' shows the appropriate value. Again, the initial viscosity = 4. 80Pa · s &lt; 1 〇〇〇 Pa · s, and the preservation viscosity = 9. 23Pa. s &lt; 1000Pa. s, both It is a liquid with fluidity. In addition, the storage stability index is 0 15=1· 92^4, and it is judged that there is a resin composition for preserving stability. Further, the indicator of the light resistance test of the cured product ΥΙ=8 8^13 Further, it was judged that there was a pair of optical properties. Further, the number of thermal shock tests was 25 times and 25 times, and it was judged to have thermal shock resistance. From the above results, the resin composition of Example 15 was fluid and preserved. Further, the cured product of the resin composition has light resistance and thermal shock resistance, and is generally judged to be qualified. [Example 16] In the same manner as in Example 1, the resin composition was produced according to Tables 1 and 2. ^ The results of the evaluation in the same manner as in Example 1, the mixing index α ε 16, and the storage enthalpy index (4) are shown in Table 3. Further, a () is hydrolyzed to _. From the tree 曰, and the composition and the interior The standard substance is measured by 0% S5%. The residual alkanoyl group 321346 103 201004993 As shown in Table 3, the tree of Example 16 The epoxy equivalent (WPE) of the composition = 214 g/eq, showing an appropriate value. Further, the initial viscosity = 12. 7 Pa.s &lt; 1000 Pa · s, and the storage viscosity = 15. 4 Pa · s &lt; 1000 Pa · s, both are liquids with fluidity. Moreover, the storage stability index 0 16=1. 21 S4, which is judged to have a resin composition for preserving stability. Further, the indicator of the light resistance test of the cured product YI = 12.4S13, it is judged that it has light resistance. Further, the number of thermal shock tests is 450 times 2 50 times, and it is judged that it has thermal shock resistance. From the above results, the resin composition of Example 16 has fluidity and preservation stability. Further, in the case where the cured product of the resin composition has light resistance and thermal shock resistance, it was judged to be qualified. [Example 17] In the same manner as in Example 1, the resin composition was prepared according to Tables 1 and 2. The product and the cured product. The results of the evaluation in the same manner as in Example 1, the mixing index α Π to ε17, and the storage stability index 0 22 are shown in Table 3. Further, ® is the intermediate formula (1) of the intermediate (OR2) is hydrolyzed to (OH). Resin composition and internal standards The amount of residual alkoxy group calculated from the substance was 〇%$5%. As shown in Table 3, the epoxy equivalent (fpE) of 238 g/eq' of the resin composition of Example I showed an appropriate value. Initial viscosity = 18. 9Pa.s &lt; 1000 Pa · s, and 'save viscosity = 28 9 pa · s &lt; 1 〇〇〇 pa · s, both liquids with fluidity. In addition, the storage stability index Θι7=153$4 is judged as a resin composition having preservation stability. Further, the index of the light resistance test of the cured product was γ Ι = 7. 2^13, and it was judged that 104 321346 201004993 was light resistant. Further, the number of thermal shock tests was 15 times and 25 times, and it was judged that there was resistance to thermal shock. From the above results, it is understood that the resin composition of Example 17 has fluidity and storage stability, and further, the cured product of the resin composition has light resistance and thermal shock resistance. [Example 18] A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables 2 and 2. The results of evaluation in the same manner as in Example 1, the mixed indexes α 18 to ε 18 , and the storage stability index 0 18 are shown in Table 3. Further, it was confirmed that (0R2) in the above formula (1) of the intermediate was hydrolyzed to (〇Η). The amount of residual alkoxy groups calculated from the resin composition and internal standard materials is 0% by weight. The epoxy equivalent (wpE) of the resin composition of Example 18 as shown in Table 3 was 245 g/eq, and an appropriate value was shown. Also, the initial viscosity = 18 2pa.s &lt; 1 〇〇〇 Pa · s, and the 'preservation viscosity = 3 〇. 5pa · s &lt; 1 〇〇〇 pa · s, both © liquid with liquidity. Further, the storage stability index 623^.68^4 was determined, and it was judged that there was a resin composition for preserving stability. Further, the indicator YI of the cured product was judged to have a light resistance of $step, and the number of thermal shock tests was 150 times of 250 times, which was judged to have thermal shock resistance. From the above, it can be seen that the resin composition of Example 18 has fluidity, two preservations of Andu, and the cured product of the dragon composition (IV) and the thermal shock resistance, so it is judged to be qualified. [Example 19] 105 321346 201004993 A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables i and 2. The results of the evaluation in the same manner as in Example 、, the mixed indexes α 19 to ε 19 , and the storage stability index 0 19 are shown in Table 3. Further, it was confirmed that (〇R2) in the above formula (1) of the intermediate was hydrolyzed to (〇Η). The amount of residual alkoxy groups calculated from the resin composition and the internal standard material was a value which was not suitable as the epoxy equivalent (wpE) = 235 g/eq' of the resin composition of Example 19 as shown in Table 3. Further, the initial viscosity = 16. 2 Pa.s &lt; 1000 Pa · s, and the storage viscosity = 24. 3 Pa · s &lt; 1 〇〇〇 Pa · s, both of which are fluid liquids. Further, the stability index 024 = 15 〇 g4 was stored, and it was judged that there was a resin composition for preserving stability. Further, the index γ Ι = 7·3^13 of the light resistance test of the cured product was judged to have light resistance. Further, the number of thermal shock tests was 5 times, and it was judged that there was resistance to thermal shock. As a result of the above, the resin composition of Example 19 has fluidity and storage stability, and further, the cured product of the resin composition has light resistance and thermal shock resistance. [Example 20] A resin composition and a cured product were produced in the same manner as in Example i according to Tables i and 2. The results of evaluation in the same manner as in Example 1, the mixing indexes α 20 to e 20 , and the storage stability index θ 20 are shown in Table 3. Further, it was confirmed that (OR2) in the above formula (1) of the intermediate was hydrolyzed to (〇H). The amount of residual alkoxy groups calculated from the resin composition and internal standard materials is 〇%$5%. ^ 321346 106 201004993 As shown in Table 3, the epoxy equivalent (WPE) of the resin composition of Example 20 = 296 g/eq ' showed an appropriate value. Further, the initial viscosity = 25.2 Pa · s &lt; 1000 Pa · s, and the preservation viscosity = l 〇〇 8 Pa · s &lt; lOOOPa · s, both are liquid liquids. In addition, the stability index Θ 20=4$ 4 was stored, and it was judged that there was a tree and fat composition for preserving stability. Further, the index of the light resistance test of the cured product was YI = 7. 8S 13, and it was judged to have light resistance. Further, the number of thermal shock tests was 50 times 2 50 times, and it was judged that there was resistance to thermal shock. From the above results, the resin composition of Example 20 has fluidity and storage stability. Further, the cured product of the resin composition has light resistance and thermal shock resistance. [Example 21] A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables i and 2. The results of evaluation in the same manner as in Example 1, the mixing indexes α21 to ε21, and the storage stability index 021 are shown in Table 3. Further, (OR2) in the above formula (1) which is an intermediate is hydrolyzed to (0). The amount of residual alkoxy groups calculated from the resin composition and internal standard materials was 〇%$5%. As shown in Table 3, the epoxy equivalent (WpE) of the resin composition of Example 21 was 270, which showed an appropriate value. Further, the initial viscosity = 2 〇. 3 pa · s dOOOPa· s' and the storage viscosity = 75 ipa· s &lt; 1 〇〇〇 pa. s, the rain is a fluid liquid. Further, the stability index 021 = 3 7 $4 was stored, and it was judged that there was a resin composition for preserving stability. Further, the indicator of the light resistance test of the cured product was γι=8·4$ΐ3, and it was judged that 321346 107 201004993 was polarized. Further, the number of thermal shock tests was 5 50 times 2 50 times, and it was judged that there was resistance to thermal shock. From the above results, the resin composition of Example 21 has fluidity and storage stability. Further, the cured product of the resin composition has light resistance and thermal shock resistance. [Example 22] A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables 1 and 2. The results of evaluation in the same manner as in Example 1, the mixed index α 22 to ε 22, and the storage stability index 0 22 are shown in Table 3. Further, it was confirmed that (〇R2) in the above formula (丨) of the intermediate was hydrolyzed to (〇Η). The amount of residual alkoxy groups calculated from the resin composition and the internal standard material was as shown in Table 3. The epoxy equivalent (WPE) of the resin composition of Example 22 was -208 g/eq, which showed an appropriate value. Further, the initial viscosity = 21. 9 pa · s &lt; 1000 Pa · s ' and the storage viscosity = 87. 6 Pa · s &lt; 1000 Pa · s, both are liquids having fluidity. Further, the storage stability index 0 22 = 4$ 4 ' was determined to have a resin composition for preserving stability. Further, the indicator of the optical property test of the cured product was YI = 8. 2$ a, and it was judged to have light resistance. Further, the number of thermal shock tests was 5 ^ 5 times, and it was judged to have thermal shock resistance. As a result, it was found that the resin composition of Example 22 has fluidity and storage stability, and further, the cured product of the resin composition has light resistance and thermal shock resistance. [Example 23] 321346 108 201004993 A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables 1 and 2. The results of evaluation in the same manner as in Example 1, the mixed indexes α 23 to ε 23 , and the storage stability index 023 are shown in Table 3. Further, it was confirmed that (〇R2) in the above formula () of the intermediate was hydrolyzed to (0Η). The amount of residual condensate &gt; oxy group calculated from the resin composition and the internal standard material is as shown in Table 3. The epoxy equivalent (ψρΕ) = 190 g/eq ' of the resin composition of Example 23 shows an appropriate value. The initial viscosity = 14.4 Pa · s &lt; © lOOOPa·s, and the 'preservation viscosity = l〇〇. 8Pa· s &lt; 1 〇〇〇pa · s, both of which are fluid liquids. Further, the storage stability index &lt;9 23 = i. 2$ 4 was judged to have a resin composition for preserving stability. Further, the index of the light resistance test of the cured product ΥΙ = 13·〇13 was judged to have light resistance. Furthermore, the number of thermal shock tests was 5 times or more and 50 times, and it was judged that there was resistance to thermal shock. From the above results, the resin composition of Example 23 has fluidity and storage stability, and the cured product of the resin composition has light resistance and thermal shock resistance. [Example 24] The resin composition was produced in the following procedure and evaluated. (1) Preparation: Set the circulating constant temperature water tank to 5 Torr to return it to the cooling pipe. Further, an oil bath of 80 Å was placed on a magnetic stirrer. (2) According to the composition ratio of Table 1, under the environment of 25 ,, (4) oxycaya compound and THF are added to the flask which has been fed with the stir-mixer and mixed (4), then the step-by-step addition of water and hydrolysis condensation catalyst , mixing. 321346 109 201004993 (3) Next, install a cooling tube in the flask 'quickly immersed in 8 (TC oil bath and start stirring, and react for 7 hours while refluxing (reflow step). (4) After the reaction is finished, cool down to At 25 ° C, the cooling tube was removed from the flask, and the sample solution (intermediate) was taken after the completion of the reflux step. (5) After the reflux step, the H-NMR of the sample solution (intermediate) was measured. It was confirmed that (0R2) of the following formula (1) was hydrolyzed to (〇H). (6) The Bis-A epoxy resin of Table 1 was added to the intermediate and stirred until homogeneous, and then placed in an evaporator. ' After distilling at 400 Pa at 50 ° C for 1 hour, it was further carried out at 80. (: Distillation was carried out for 5 hours, and dehydration condensation reaction was carried out (dehydration condensation step). (7) After the reaction was finished, 'cooling to The resin composition was obtained at 25 ° C. The amount of residual alkoxy groups calculated by the resin composition and the internal standard material was (8) The mixing index of the resin composition 〇: 24 to £24 indicates Table 3. (9) Further, according to the above method, the resin obtained in the above (6) was measured. The epoxy equivalent (WPE) of the composition, the initial viscosity, and the storage viscosity. Further, the preservation of the virginity index Θ 24 ' is shown in Table 3. The epoxy equivalent of the resin composition of the above only Example 24 ( wpE)=233g/call, showing the appropriate value. Also 'start sticky ms&lt;i_pa· preservation viscosity=16.8 Pa · s&lt;_ Pa · s, both are liquids. Also, save the stability index to 4=1 (4) The resin composition having the stability of preservation was judged. The same procedure as in the hardening example 1 was carried out to prepare a resin composition and a cured product according to Table 2. The results of the evaluation in the same manner as in Example 1 are shown in Table 3. 32]346 110 201004993 The index of the light resistance test of the cured product is YI=8.3S 13, and it is judged to have light resistance. Moreover, the number of thermal shock tests is 5 times or more and 5 times, and it is judged to have thermal shock resistance. From the above results, the resin composition of Example 24 has fluidity and storage stability. Moreover, the cured product of the resin composition has light resistance and thermal shock resistance, and therefore it was judged to be acceptable. The resin composition is manufactured and evaluated according to the following steps. (1) Preparation. Set the circulating H tank to 5t: to return to the cooling tube. Also, place 8 (TC oil bath) on the magnetic stirrer. (2) According to the composition ratio of Table 1, the environment will be 25 艽. A mass corresponding to one-half of the total amount of the epoxy resin, the alkoxylated compound and the THF are added to the flask to which the stirrer has been added, and the mixture is stirred and mixed. Then, water and a hydrolysis condensation catalyst are added in one step, and the mixture is stirred and mixed. (3) Next, 'in the flask wire cooling tube, quickly dipped in the oil bath of the thief and began to mix, and reflux-surface reaction for 7 hours (reflow step). (4) After the completion of the reaction, the cold (four) hunger, the money is removed from the flask, and the sample solution (intermediate) is taken after the completion of the reflux step. (5) After the completion of the refluxing step, (4) H-NMR of the sample solution (intermediate), it is confirmed that (0R2) of the following formula (1) is hydrolyzed to (0H). (6) Add one-half of the amount of BlS-A oxygen-containing resin in the intermediate to the intermediate and mix it until it is evenly distributed, then place it on the evaporator Θ 'after 4 GG Pa, 5 『c. More progress - step, 〆Μ 5 cut '- face into the water condensation reaction (dehydration 1) 1 321346 201004993 condensation step). (7) After the completion of the reaction, the amount of the residual alkoxy group calculated from the resin composition and the internal standard material was 0% by weight of 5% until the resin composition was cooled to 25 °C. (8) The mixing index α 25 to ε 25 of the resin composition is shown in Table 3 〇 (9), and the epoxy equivalent (WPE) of the resin composition obtained in the above (6) is measured by the above method. Viscosity and preservation of viscosity. Also, the preservation safety index 0 25 is obtained, which is shown in Table 3. The epoxy equivalent (wPE) of the resin composition of the above Example 25 was 232 g / eq, which showed an appropriate value. Further, the initial viscosity = 11.8 Pa.s &lt; 1 〇〇〇 pa · s' and the 'preservation viscosity = 16 · 7 Pa · s &lt; l 000 Pa · s' are both liquids having fluidity. Further, the storage stability index (9 25 = 1.4224, which was determined to have a resin composition for preserving stability) was prepared in the same manner as in Example 1 to prepare a resin composition and a Q-cured material according to Table 2. The same method as in Example 1 was carried out. As a result of the evaluation, as shown in Table 3, the indicator of the light resistance test of the cured product YI=8.3.3^13, and it was judged to have light resistance. The number of 'hot and cold shock test times was 5〇0 times or more and 250 times, and it was judged as It is known from the above results that the resin composition of Example 25 has fluidity and storage stability, and the cured product of the resin composition has light resistance and thermal shock resistance, so it is judged as qualified by comprehensive judgment. [Example 26] The resin composition was produced and evaluated according to the following procedure: 321346 112 201004993 (1) Preparation. Set the circulating constant temperature water tank to 5 ° C to reflux to the cooling tube. Further, upload on a magnetic stirrer Set 8 (TC oil bath. (2) Remove the P-MS component, according to the composition ratio of Table 1, in a 25 ^ environment, the Bis-Al epoxy resin, alkoxy calcined compound and tjif ingredients have been added After stirring in a flask with a stirrer, Further, water and a hydrolysis condensation catalyst were added and mixed and stirred. (3) Next, 'cooling tube was attached to the flask', rapidly immersed in an oil bath and started to mix, and reacted for 7 hours while refluxing (reflow step). (4) After completion of the reaction, cool to 25 ° C ' and then remove the cooling tube from the flask, and then take the sample solution (intermediate) after the completion of the reflux step. (5) After the reflux step, the sample solution (intermediate) is measured. H-NMR, it was confirmed that (〇R2) of the following formula (1) was hydrolyzed to (0H). (6) The solution after the reflux step was completed, using an evaporator at 4 ° Pa, 50 ° C After 1 hour of lower distillation, 'further further', the dehydration condensation reaction (dehydration condensation step) was carried out for 5 hours at 80 ° C. q (7) After the reaction was completed, it was cooled to 25 ° C, according to the composition of Table 1. The amount of the equivalent amount of P-MS is mixed and the mixture is mixed until it is evenly mixed to obtain a resin composition. The amount of residual alkoxy group calculated from the resin composition and the internal standard material is 4 (8) The mixing index α 26 to 26 of the resin composition is shown in Table 3. (9) Further, the epoxy equivalent (WPE), the initial viscosity, and the storage point of the resin composition obtained in the above (7) were measured by the above method. Further, the storage stability index 0 26 was obtained, which is shown in Table 3. 321346 113 201004993 The epoxy equivalent (WpE) of the resin composition of the above Example 26 is 23 〇g / eq, which shows an appropriate value. Further, the initial viscosity = 14.5 Pa·s &lt; 1000 Pa · s 'and Preservation viscosity = 49. 3 Pa · s &lt; i〇〇〇pa · s, both are fluid liquids. Further, the storage stability index 0 26 = 3 4 $ 4 was judged to be a resin composition having a stable stability. In the same manner as in Example 1, a resin composition and a cured product were produced in accordance with Table 2. The results of the evaluation in the same manner as in Example 1 are shown in Table 3. The index of the time-test of the cured product was YI = 1〇. 6^13, and it was judged that there was a good light. Further, the number of thermal shock tests was 250 times 5 times, and it was judged that there was cold and thermal shock resistance. From the above results, it is understood that the resin composition of Example 26 has fluidity and storage properties, and the cured product of the resin composition has light resistance and thermal shock resistance. [Comparative Example 1] A resin composition was prepared in the same manner as in Example 1 according to Table 1. The amount of residual alkoxy groups calculated from the resin composition and the internal standard material was 17% &gt; 5%. The results of evaluation in the same manner as in Example 1, the mixing index α 27 to ε 27, and the storage stability index eg? are shown in Table 3. As shown in Table 3, the epoxy equivalent (wpE) pin g/N of the resin composition of Comparative Example 1 was shown to be an appropriate value. Further, the initial viscosity &gt; 1 〇 _ s, the preservation minus &gt; 1000 Pa· s ' is not motivated, and the stability index Θ 27 cannot be counted. Further, the above-mentioned resin compositions, the fineness of HOGOPa.s and 321346 114 201004993, have no fluidity, so that it is impossible to produce a cured product. From the above results, it was found that the resin composition of Comparative Example 1 had no fluidity, and it was impossible to calculate the storage stability, and since it was impossible to produce a cured product, the overall determination was unacceptable. [Comparative Example 2] A resin composition and a cured product were produced in the same manner as in Example 1 according to Tables 1 and 2'. The amount of residual alkoxy groups calculated from the resin composition and the internal standard material was 8% &gt; 5 Å / Torr. The results of evaluation in the same manner as in Example 1, the mixing index α 28 to ε 28 , and the storage stability index Θ 28 are shown in Table 3. As shown in Table 3, the epoxy equivalent (??) of the resin composition of Comparative Example 2 = 295 g/eq, and an appropriate value was shown. Further, the initial viscosity = 30. 5 Pa · s &lt; 1000 Pa · s, and the preservation viscosity = 45. IPa · s &lt; l〇〇〇pa · s, both of which are fluid liquids. In addition, the preservation stability index 0 13=1.48 $4 was identified as a resin composition with preservation stability. Q Further, the indicator of the photochemical test of the cured product YI=8. 4 S13 was judged to have light resistance. Further, the number of thermal shock tests was 0 times &lt; 5 times, and it was judged that there was no cold shock resistance. From the above results, the resin composition of Comparative Example 2 has a fluidity and storage stability. However, even if it has light resistance, it has no resistance to thermal shock resistance, so it is judged that it is not comprehensive. Qualified. [Comparative Example 3] A resin composition was prepared in the same manner as in Example 1 according to Table 1. The results of evaluation in the same manner as in Example 1, the mixing index α 29 to ε 321346 115 201004993 29, and the storage stability index θ θ 29 are shown in Table 3. As shown in Table 3, the epoxy equivalent (??) of the resin composition of Comparative Example 3 = 233 g/eq, which showed an appropriate value. Further, the initial viscosity was 3. 8 Pa . s &lt; 1000 Pa·s, and the viscosity was maintained at >1000 Pa·s, indicating no fluidity. Further, the storage stability index 0 28 = 263 or more &gt; 4 was found to be non-storage stability. Further, since the above-mentioned composition is known to have a viscosity of &gt; pa · s and no fluidity, it is not possible to produce a cured product by =*=*. From the above results, it was found that the resin composition of Comparative Example 3 had no flow enthalpy and storage stability, and it was impossible to produce a cured product, so that it was judged to be unacceptable. [Comparative Example 4] A resin composition was produced in the same manner as in Example 1 in accordance with the specifications. The results of the evaluation in the same manner as in Example 1, the mixing index α3〇 to ^30, and the storage stability index Θ 30 are shown in Table 3

As shown in Table 3, the epoxy resin of the resin composition of Comparative Example 4, g/eq, showed an appropriate value. Again, initial viscosity

Pa.s, and 'save viscosity> _ Pa.s, showing the benefit flow = again, save the stability index Θ 3 (four) or more &gt; 4, and find that there is no preservation. Further, since the above resin composition has a viscosity of &gt;1()()〇ρ& · s and no fluidity, it is impossible to produce a cured product. A 321346 116 201004993 failed. [Comparative Example 5] A resin composition was prepared in the same manner as in Example 1 according to Table 1. The same method as in Example 1 will be used to evaluate the 3 and the preservation index (4); the fruit and the mixture refers to the .31 to stone.. η table is not in Table 3. The 0 system cannot determine the epoxy equivalent (10) of the composition. The viscosity ΗΟΟΟΡ^, ^^·〆1000 1^, and O Λ Qn ^ 4 are not fluid. Also, save the ampere (four) 曰 Θ 30 = 4i or more > η two no preservation stability.益法动ϋ ά ^ Α成物#, because of the preservation of viscosity > 1GG () Pa · S and no transfer, the shirt may be made into a hardened object. In the case of the O, it is known that the resin of the comparative example 5 has no flow, and it is impossible to produce a cured product, so it is judged to be unqualified. [Comparative Example 6] 硬化 In the same manner as in Example 1, according to Table 2, a cured product was produced. The results of evaluation in the same manner as in Example 1 alone are shown in Table 3. The index of the light-resistant material of the cured product ΥΙ = 16 9 &gt; 13, judgment = light. Further, the number of thermal shock tests was 5 (10) times or more (10) times, and the thermal shock resistance was determined. The hitting property was judged by =:, !! The hardened material of Comparative Example 6 was resistant to cold and heat, and ρ had no light resistance, so it was judged to be unacceptable. [Comparative Example 7] The above-mentioned polysulfuric acid resin was mixed with eight liquids and 321346 317 201004993 B liquid in a mass ratio of 1:1, and the cured product was produced in the same manner as in Example 1 according to Table 2. Use a solution. The above-mentioned curing solution was poured into a molding jig and 10 substrates for the above-mentioned thermal shock test in the same manner as in Example 1, and one wafer was placed in each of the substrates. The forming jig and the substrate for the thermal shock test were placed in an oven, and subjected to a curing treatment at 70 ° C for 1 hour and further at 150 ° C for 5 hours to prepare a cured product.结果 The results of evaluation in the same manner as in Example 1 are shown in Table 3. The index of the light resistance test of the cured product was YI = 2. 0S13, and it was judged to have light resistance. However, the number of thermal shock tests was 0 times &lt; 50 times, and it was judged that there was no cold shock resistance. From the above results, it was found that the cured product of Comparative Example 7 had a light-resistance but was not resistant to thermal shock resistance, and was therefore judged to be unacceptable. [Comparative Example 8] 0 According to Table 1, epoxy resin Α2 and epoxy resin A3 were added to the reaction vessel, and the mixture was immersed in an oil bath at 85 ° C and stirred/dissolved, and further P-MTMS and DBTDL were added. And mixed. Further, while performing nitrogen purge, the oil bath temperature was raised to 105 ° C, and the dealcoholization reaction was carried out for 8 hours. Next, after cooling to 60 ° C, the pressure was reduced to 12000 Pa, and the dissolved alcohol was removed to obtain a resin composition. The amount of residual alkoxy groups thus calculated from the resin composition and the internal standard material was 11% &gt; 5%. The results of the evaluation in the same manner as in Example 1 and the preservation stability index 1] 8 321346 201004993 θ 32 are shown in Table 3. The epoxy equivalent (WPE) of the resin composition of Comparative Example 8 was 282 g/eq, which showed an appropriate value. Further, the initial viscosity is 0.15 Pa · s &lt; 1000 Pa · s, and the storage viscosity = 〇. 27 Pa · s &lt; 1000 Pa · s, both are fluid liquids. Further, the storage stability index θ 32 = 1.80S 4 was found to be a resin composition having a storage stability. Further, according to the blending method of Table 2, a cured product was produced in the same manner as in Example 1. When the evaluation was carried out, the number of times of the hot and cold impact test of the cured product of Comparative Example 8 was 〇50 times, and it was found that there was no heat and cold resistance. Impact. Further, in the production of the sample used in the light resistance test, minute cracks were generated and measurement was impossible. From the above results, it was found that the cured product of Comparative Example 8 was judged to be unacceptable. [Comparative Example 9] A resin composition was prepared in the same manner as in Example 1 according to Table 1. The results of evaluation in the same manner as in Example 1 and the mixing index α 33 to ε 33 ❹ are shown in Table 3. Further, (OR2) in the above formula (1) of the intermediate is not hydrolyzed in a large amount, and the hydrolysis reaction cannot be carried out normally. Therefore, the normal resin composition was not obtained, and it was judged to be unacceptable. The amount of residual methoxy groups derived from the resin composition and the internal standard material is 100% or more &gt; 5%. From the results of Tables 1 to 3, it is understood that the resin composition (Examples 1 to 26) obtained by mixing an epoxy resin with a specific alkoxydecane compound in a specific ratio and performing cohydrolysis condensation is excellent. Liquidity and preservation stability. Further, the cured product obtained by using the resin composition has excellent light resistance and thermal shock resistance. Π9 321346 201004993 ι&lt; χΐίί :3⁄4 孅 孅 ( 和 和 和 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 IU«期1 丨1 1 1 1 1 1 t 1 1 1 1 丨1 1 1 1 1 ! 1 1 I 1 1 1 1 lt 1 1 ! 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CO 5 1 27.9 II 20.3 I 1 27.6 I 35.3 ! eo 87.1 | 27.6 ?7.8(ί3.8ίΐα8) IA I 26.8 26.0 26.6 28.9 1 1 loo.o 1 I o Really fine 1 I f Gang 1 I solid foot | 1 Zi Na 1 1 Poor Na | 1 Shi Na 1 1 Shi Na i | Lean Liu | 1 Lean Liu | 1Example ii 1 | Bao Gang 2 I | Poverty _13 II Real W14 I | Remuneration 15 1 Really 16 Real _7 寅 Example 18 tnm Poor Benzoin solid pin 1 t &lt; W23 mm \ Rewards plant itm fc puncturing ratio _ I ΛϋίΗ2 mm TB Lion ratio correction W7 1 tb «lW9 120 321346 201004993 TABLE 2

Unit: mass % composition ratio resin composition Bis-Al epoxy resin polyoxyl resin hardener hardening accelerator Example 1 58. 3 — — 41. 6 0. 2 Example 2 58.4 One 41.4 0 2 Example 3 60. 6 - a 39. 3 0. 2 Example 4 55. 8 — — 44. 0 0· 2 Example 5 59.8 I—40. 0 0. 2 Example 6 57. 3 — — 42. 5 0· 2 Example 7 56. 9 - A 43. 0 0. 2 Example 8 56.4 I - 43.4 0. 2 Example 9 58. 8 I - 41. 0 0. 2 Example 10 56. 5 — — 43.4 0. 2 Example 11 58. 1 — — 41. 8 0· 2 Example 12 58. 3 — — 41. 6 0. 2 Example 13 60. 6 — — 39. 3 0. 2 Example 14 57. 8 — 42. 0 0. 2 Example 15 57.4 I—42. 5 0. 2 Example 16 57.4 — — 42. 4 0. 2 Example 17 58. 4 I—41. 4 0. 2 Example 18 59. 8 - 40. 0 0. 2 Example 19 58.4 - - 41. 4 0. 2 Example 20 58. 4 - 41. 4 0_ 2 Example 21 58.4 - - 41. 4 0. 2 Example 22 58 4 — — 41. 4 0. 2 Example 23 58.4 — — 41. 4 0. 2 Example 24 58.4 A — 41.4 0· 2 Example 25 58.4 I—41. 4 0· 2 Example 26 58.4 I—41.4 0. 2 Comparative Example 1 — — — — — Comparative Example 2 64. 1 — A 35. 7 0. 2 Comparative Example 3 — A - a comparative example 4 - - - - - Comparative Example 5 - one - one - Comparative Example 6 - 53. 2 - 46. 6 0. 2 Comparative Example 7 - 100. 0 A - Comparative Example 8 63. 7 - — 36. 1 0. 2 121 321346 201004993 co &lt; Capital Umbrella-: X, 鸯-f-: 9 ◎ <铋家> V f 〇〇o 〇〇〇〇〇〇Ο 〇〇〇〇〇〇〇〇〇〇〇〇〇〇〇〇XXXXXXXXXS ί i ** 5C ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ 〇 1 X ! 1 1 ◎ XXI old is 1 Λϋ § 爵 i i 1 i § S § § Gss 1 An 1 1 Λ» s 1 et 1 1 1 oo 1 tasting o 〇〇〇〇〇〇〇〇〇o 〇〇〇〇〇〇〇〇O 〇〇〇1 〇1 1 1 X 〇X 1 &gt;: a eo eo 04 α» in οό 〇0 ro OO CD 卜 o ed 〇〇 · · in OO OO OO OO OO oi oi oi oi oi oi oi oi oi oi oi oi oi oi oi oi 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 · OO 卜 · ed Dd ed O vi n οό eo 90 CO i call ad 1 1 IO) cd o ei w I } I % i 〇〇〇〇〇〇〇〇〇〇〇〇〇〇ο 〇〇〇〇〇 o 〇〇〇O 〇X 〇XXX 1 1 〇X m 2·5 ss ss ss s oi s SS wear eo* s ♦· 1 i 癸X ! 1 s 1 1 〇r-* CP 卜 CO CO eo CD iO CO (£3 «0 t— OO s I A ss OO wear · s rj S3 β&gt; in 〇&gt; tn different e*a 忒eo 8 K2 CD N CO ec t- CO eo per cloud 1 I 1 X 1 1 so' 1 stop 1 OO CO t- C4 e»5 rg οό eo e Sfi e eo Ed CM CO Γ— m F= CO 1 — e4 〇&gt; ed CQ ad CnJ CP CM CO 〇» c? ·«· eo eo ΙΛ 2! I m eo rJ in甴O 1 1 to G&gt; 1 笤1 Celluloid t- eo 53 § Fee father ^· N 赛 器 g B § 1 爵 s m. 1 l Pack! Raise « 1 fii «0 sss S s &amp S s & s S s &amp; s 茗2 sss S 8 lt&gt; s & 1 1 1 8 tsi *〇r- s 〇· eo s C9 t- § e&gt; 1- se» α» δ e 1 — § e&gt; OO s ea se δ δ eS t*- s CO s 卜 s § S s eo § nsii OO s β» s σ> 00 s OO s DO 8 I— I r — S β» iif — 1 ao 5 1 1 1 eo ci m e&gt; s es So e&gt; 宙 e» &amp; e» s eS 宙 e&gt; soseseses Sd smss 8 s S δ ss SS 2 e= S 1 1 ! s 〇· se* o' e&gt; e» 9 o 闵c» 9 e&gt; e 2J o 2j O so thinking S CO 55 s knot S s fee Ϊ 1 1 β 1 1 e: i 1 e&gt; I C3 i O i O 1 1 eIe$ 1 e&gt; 1 1 i e&gt; ie 运 e» 1 CD m es I 93 〇· § OO ΙΑ § S e&gt; i O 1 o 1 〇· iis fr S3 I oie CO soii 1 io' _ I jM s 丄*5 esa ( eg eo l CO si in 1 0 c〇i Q ε 1 00 Q&gt; i aa Φ iaee « s ΐ eo s Q e*ss ? PD 〇s «2* *5 ΙΛ sl CD s ? CD cr— 5 *5 eo Φ lee» } se lean Q&gt; i 宕c3 Φ 53 Q i i i S3 « ? « l φ } goods c & ie 闵i fee Q skin 8 l « eo Q> l β 1明 l路« 40 1 II CO I eo I 对 I m QD f 1« *»: t— 爹00 ea i 13⁄4 1 * &lt; DO 1 Ϊ i —: LA 1 * &lt;C £ I 1 r — i 00 1 V: 03 I 闵1 3 3 3 3 3 1 1 闵I 1 1 CO I ff* I LA I CD II QP i σ&gt; ! 122 321346 201004993 The condensation ratio of the alkoxysilane of the modified resin composition to the condensation ratio of the intermediate is specifically described in the examples and the comparative examples. First, the evaluation methods of the physical properties in Examples 27 to 35 and Comparative Examples 10 to 14 are shown below. Regarding the amount of residual alkoxy groups, epoxy equivalent (WPE), viscosity, and mixing index α to ? of the modified resin composition? ? , obtained in the same way as above. &lt;Calculation of Condensation Rate of Intermediate&gt; The condensation rate of the intermediate is determined by the following procedure after the completion of the refluxing step by the Si-NMR measurement of the sample solution (intermediate) taken. (1) Preparation of Cr solution: 3% by mass of acetonitrile (III) (manufactured by Sigma-Aldrich Co., Ltd.) was added to chloroform-d (manufactured by Wako Pure Chemical Industries, Ltd.), and dissolved. (2) In the sample bottle, weigh 200 mg of the sample solution after the end of the refluxing step, and add the above Cr solution to adjust to lg. (3) The solution of the above (2) was transferred to an NMR tube having a diameter of 5 mm p, and Si-NMR was measured under the following conditions. Fourier transform nuclear magnetic resonance apparatus: "α-400 type" manufactured by JEOL, Nuclear species: Si, cumulative number: 4000 times (4) According to the following formula, the condensation ratio K of the intermediate is obtained. Condensation rate (%MD1 xl + D2x2 + Tlxl + T2x2 + T3x3) / {(D0 + Dl + D2)x2+ (Τ0 + Τ1 + Τ2 + Τ3)χ3}χ100 ...(10) 123 321346 201004993 Here, DO : (1) The total of the integrated values of the signals derived from the D〇 structure represented by the following formula (11) derived from the alkoxydecane compound of n=l. D1 is a total of integral values of signals derived from the D1 structure represented by the following formula (12) derived from the η=ι alkoxydecane compound in the formula (1). D2 is a total of integral values of signals derived from the D2 structure represented by the following formula (12) derived from the alkoxydecane compound of n = 1 in the formula (1). 0 T〇 : Formula (1) 'Total value of the integrated value of the signal derived from the TO structure represented by the following formula (13) derived from the alkoxydecane compound of n=2. In the formula (1), the integral value of the signal derived from the T1 structure represented by the following formula (14) derived from the alkoxydecane compound of n=2 is altogether. T2: In the formula (1), the integral value of the signal derived from the T2 structure shown by the following formula 〇4) derived from n=2 alkoxydecane compound is a total. T3: In the formula (1), the integral value of the signal derived from the T3 structure represented by the following formula (14) derived from the alkoxydecane compound of n=2.

® OR

I R—Si—R η i)

I

OR DO structure In the formula (11), R is an arbitrary organic group or H. 124 321346 201004993

R R

I I HO—Si—O—Si—O— (12)

I I

R R D 1 structure D .2 structure In the above formula (12), R is an arbitrary organic group or hydrazine

OR 1 R —Si—OR (i 3) 〇

I

OR 丁 o structure In the above formula (13), R is an arbitrary organic group or hydrazine

R

R

R HO—Si—Ο—Si—Ο—Si—Ο (μ) OH τ 1 structure 01 D 3 structure OH T 2 structure In the above formula (14), R is an arbitrary organic group or H. &lt;Calculation of the condensation ratio of the alkoxydecane compound of the modified resin composition&gt; The condensation ratio of the alkoxydecane compound of the modified resin composition is the Si of the sample solution taken after the end of the dehydration condensation step The result of the measurement of Li R was determined by the same method as the calculation method of the condensation ratio of the intermediate, and the condensation ratio L (%) was obtained. &lt;Calculation of Storage Stability Index β and Storage Stability of Resin Composition&gt; The storage stability of the resin composition is expressed by the following formula (9), and is evaluated by storing 125 321 346 201004993 stability index 0. Preservation stability refers to (4) = (health viscosity) / (tapping degree)... (9) The container of the resin composition manufactured by Gu Rengang is sealed, and after adjusting the temperature for 25 hours, the viscosity in the step is measured, and this is regarded as "Starting viscosity". &lt;'''''''''''''' After saving, the measurement will be at 25

This is treated as "save viscosity." When the resin composition has fluidity (viscosity of 1 〇〇〇Pa·s or less) and the safety index of the ampere m is 6 or less, it is judged that the storage stability is determined, and it is determined as follows. 0^ Θ ^4 ◎ 4&lt; Θ S6 〇 &lt; Light resistance test of cured product&gt; The light resistance of the cured product of the resin composition was evaluated by the following method. Ο (1) The cured product prepared by the method described later was hardened with a solution to prepare a cured product having a thickness of 20 mm x 10 mm X 3 mm. (2) The cured product was covered with a black mask of 25111^15 mm x 1.2 mm thick having a diameter of 5. 5 mm as a sample for light resistance test. (3) Preparation device 'The UV light was irradiated from the UV irradiation device ("Spot Cure SP7-250DB", manufactured by Ushio Electric Co., Ltd.) to the above-mentioned test in a strange temperature oven set to a constant temperature of 50 °C via an optical fiber. kind. (4) The above sample was placed in an incubator at 321346 126 201004993 50 °C with the black mask covered. (5) UV light of 2 W/cm2 was irradiated from the upper part of the black mask for 96 hours in such a manner that the light was irradiated to the hole of 5. 5 imn. (6) A sample irradiated with UV was measured by a spectrophotometer ("SD5000" manufactured by Seiko Co., Ltd.) which has been modified into a diameter i〇min. (7) Yellowness (YI) is obtained according to "ASTM D1925-70 (1988): Test Method for Yellowness Index of Plastics". ® When this YI is 13 or less, it is judged to have light resistance. &lt;Cold and thermal shock test of cured product&gt; The thermal shock resistance of the cured product of the resin composition was evaluated by the following method. (1) Prepare the following substrate and germanium wafer. (1 1) Substrate. Made by Solvay Advanced Polymers, "AMODEL A-4122NL WH 905" (with a diameter of lOmmx depth of 1. 2mm in the center of a flat plate of 15mmxl5mmx ❹ thickness 2_) U -2) broken wafer (will The commercially available bite wafer is cut into 5 dirty and 5 face thicknesses 200 &quot; m) (2) Η) A solution for the hardened material produced by the method described later flows into the substrate and is placed in the front (four) crystals&gt; 5, it is hardened and used as a sample for the thermal shock test. (3) The above sample is placed in a thermal shock cracking (10) company (TSE 11 Α))" (--Qing to 12 ( Rc) / cycle: heat 321346 127 201004993 time 14 minutes, temperature rise and fall time 1 minute" conditions for thermal cycling. (4) The above sample was taken out at the time of 50 thermal cycles, the permeate (Κ0ΗΖΑΙ( The company's system, "MICRO-CHECK", was sprayed, and the presence or absence of abnormality (peeling or cracking) was visually observed under a magnifying glass, and the number was recorded. (5) The above-mentioned (4) was confirmed to be a sample without abnormality. Into the device, after the 50th thermal cycle, the same operation evaluation Then, the heat cycle was performed 100 times in the same way and evaluated. Repeat these ISO operations and evaluate them. (6) When you see that 2 out of 10 samples are abnormal, the evaluation is interrupted. The number of thermal shock resistance = (the number of thermal cycles interrupted) - (50 times). When the number of thermal shock resistance is 50 or more, it is judged to have practically sufficient thermal shock resistance. The raw materials used in 35 and Comparative Examples 10 to 14 are shown in the following (1) to (10). Q (1) Epoxy Resin (1-1) Epoxy Resin A: Poly(bisphenol A-2-hydroxypropane Base ether) (hereinafter, referred to as Bis-A epoxy resin) • Trade name: manufactured by Asahi Kasei Epoxy Co., Ltd., "AER2600" The epoxy equivalent (WPE) and viscosity measured by the above method are as follows. Oxygen equivalent (WPE): 187g/eq • Degree (25°C): 14. 3 Pa · s (1-2) Epoxy resin B : 3, 4-epoxycyclohexyl fluorenyl-3', 4'- Epoxy 128 321346 201004993 Cyclohexyl carboxylate (hereinafter referred to as alicyclic epoxy resin) • Trade name · Dai ce 1 Chemical Industry Co., Ltd. 'Ce 1 1 οχ ide 2021P” The epoxy equivalent (WPE) and viscosity measured by the above method are as follows: • Oxygen equivalent (WPE): 131g/ed • Degree (25°C): 227 mPa · s (2) Alkoxydecane compound Η : 3-glycidyloxypropyltrimethoxy-based decane (hereinafter referred to as GPTMS) • Trade name: Shin-Etsu Chemical Co., Ltd.'s "ΚΒΜ-403" (3) Alkoxy Base decane compound I: phenyltrimethoxy decane (hereinafter referred to as PTMS) • Trade name: "ΚΒΜ-103" manufactured by Shin-Etsu Chemical Co., Ltd. (4) Alkoxy decane compound j: dimercapto ruthenium Oxydecane (hereinafter referred to as DMDMS) ❹ • Trade name: Shin-Etsu Chemical Co., Ltd., “ΚΒΜ-22” (5) Alkoxydecane compound κ: tetraethoxy decane (hereinafter referred to as TEOS) • Product name: Shin-Etsu Chemical Co., Ltd., "ΚΒΕ-04" (6) Solvent (6-1) Tetrahydrofuran: manufactured by Wako Pure Chemical Industries Co., Ltd., without stabilizer (hereinafter referred to as THF) (6- 2) Tert-butanol: manufactured by Wako Pure Chemical Industries Co., Ltd. (hereinafter referred to as t-BuOH) (7) Hydrolysis condensation catalyst 3 21346 129 201004993 (7-1) Dibutyltin dimethoxide (hereinafter referred to as DBTDM): Sigma-Aldrich Co., Ltd. (7-2) Dioctyltin diacetate (hereinafter referred to as D0TDA): manufactured by Nitto Chemical Co., Ltd. "Neostann U-820" (7-3) Dibutyltin dilaurate (hereinafter referred to as DBTDL): manufactured by Wako Pure Chemical Industries Co., Ltd.

(8) Hardener: "4-methylhexahydrophthalic anhydride / hexahydrophthalic anhydride = 70/30" • Trade name: "RIKACID ® MH-700G" manufactured by Nippon Chemical and Chemical Co., Ltd. (9) Hardening promotion Agent: Amine-based hardener • Trade name: “U_CAT 18X” manufactured by San-apro Co., Ltd. (10) Polyoxynene resin: “SCR-1012 (A liquid and B liquid) manufactured by Shin-Etsu Chemical Co., Ltd. (11) Internal standard substance 1,1,2,2-tetrabromoethane: Q manufactured by Tokyo Chemical Industry Co., Ltd. [Example 27] A resin composition was produced by the following procedure. (1) Preparation · Set the circulating constant temperature water tank to 5. (:, return to the cooling tube. Further, place 8 〇 oil bath on the magnetic stirrer. (2) According to the composition ratio shown in Table 4, the above Bis~A ring is placed at 25 ° C. An oxygen resin, an alkoxydecane compound, and THF are added to a flask to which a stirrer has been placed, and mixed and stirred, and then water and a hydrolysis condensation catalyst are further added, and mixed and mixed. (3) Next, the flask is installed. Cool the tube and quickly pour it into 8 (TC oil bath 321346 130 201004993 and start stirring, react for 25 hours while refluxing (reflow step). (4) After the reaction is finished, cool to 25 ° C ' and then remove from the flask The lower cooling tube is taken to take the sample solution (intermediate) after the completion of the reflux step. (5) After the reflux step is completed, the si-NMR of the sample solution (intermediate) is measured, and the middle is obtained according to the above formula (10). The condensation rate of the body is K1. The condensation rate of the intermediate Kl (%) = 80. (6) The solution after the reflux step is distilled off at 400 pa, 50 ° C for 1 hour using an evaporator, and further Distilled at 80 ° C for 1 hour, while dehydration condensation reaction (7) After completion of the dehydration condensation reaction, the mixture is cooled to 25 ° C to obtain a resin composition, and a sample solution is taken. (8) After the dehydration condensation step is completed, Si-NMR of the sample solution is measured, according to the above formula (10) The condensation ratio L1 of the modified resin composition is obtained. The condensation ratio of the modified resin composition is Ll (%) = 86 · 6% 2 80%. Further, the amount of residual alkoxy groups of the modified resin composition is 〇%$ 5%. (9) The above-mentioned mixing index α 34 to ε 34 of the resin composition is shown in Table 6 below. (10) Further, the resin composition obtained in the above (6) is measured according to the above method. Epoxy equivalent (WPE), initial viscosity, and storage viscosity. Further, a storage stability index Θ 34 was obtained, which is shown in Table 6. The epoxy equivalent (wpE) of the resin composition of the above Example 27 was 220 g / eq. , showing the appropriate value. Again, the initial viscosity = 12. 7Pa · s &lt; lOOOPa · s, and the preservation viscosity = 32. 5Pa · s &lt; 1000 Pa · s, both are 131 321346 201004993 fluidity liquid. Also, 'preservation stability index 0 34 = 2. 4, excellent fluidity' is judged to be improved preservation stability Next, 'the resin composition was used, and the cured product was produced and evaluated by the following procedure. (11) The resin composition, the hardener, and the hardening accelerator were placed under the environment of 25 ° C. The composition ratios shown in Table 5 were mixed and stirred, and degassed under vacuum to obtain a solution for the hardened material. (12) A thickness of 3 mm; a 7-shaped stone etched rubber was applied to two coated release agents. A molding jig is produced to make the cured product produced by the molding jig into a thickness of about 50 mm x about 20 mm x 3 Å. (13) For the molding jig and one of the substrates for the above-described thermal shock test, the above-mentioned cured solution is injected, and one of the above-mentioned tantalum wafers is placed in each of the substrates. (14) The above-mentioned forming jig and the substrate for thermal shock test were placed in a baking oven, and hardened at 120 ° C for 1 hour, and further at 15 〇 ec # i hour to prepare a cured product. (15) After the internal temperature of the oven drops below 3 〇t, the cured product is taken out, and the sample for light resistance test and the sample for thermal shock test are prepared by the above method. (16) The results of the light resistance test and the hot and cold impact test by the above method using the above samples are shown in Table 6 below. The indicator of the light resistance test of the cured product, γ Ι = 113, was judged to have practically sufficient light resistance. Further, the number of thermal shock tests was 35 ^^5 〇2, and it was judged to have practically sufficient thermal shock resistance. From the above results, it is understood that the resin composition of Example 27 has a good flow 132 321346 201004993 motility and excellent preservation stability, and the resin β u ☆ 八 + I bait day, and the cured product of the product has a practical charge The light resistance and cold and thermal shock resistance of the knife, so comprehensive [Example 28] 疋马〇 inspection. In the same manner as in the above-mentioned Example 27, the resin composition and the cured product thereof were produced in accordance with the following paragraphs and Table 5. The resin composition and the cured product thereof were evaluated in the same manner as in the above Example ^. The evaluation results, the mixing index α such as to milk, and the storage stability index 0 35 are shown in Table 6 below. °。 The condensation rate of the intermediate Κ 2 (%) = 78. 2% ^ 78%. The condensation ratio L2 (%) of the modified resin composition = 8 l 8% g 8%. The amount of residual alkoxy groups of the modified resin composition was 〇%$5%. &gt; As shown in the following Table 6, the epoxy resin equivalent (WPE) of the resin composition of Example 28 was 233 g/eq, and showed an appropriate value. Further, the initial viscosity = 15.9 Pa·s &lt; 1000 Pa·s, and the storage viscosity = 53·8 Pa·s &lt; 1000 Pa·s, and good fluidity. Further, 'storage ◎ stability index (9 35=3·4S4, excellent fluidity, it is known that the resin composition has improved stability and stability. Also, the indicator of the light resistance test of the cured product YI=8. 1$ 13, It is judged that there is practically sufficient light resistance. The number of thermal shock tests is 250 times 2, 50 times, and it is judged that there is practically sufficient cold and thermal shock resistance. From the above results, it is understood that the resin composition of Example 28 is excellent in fluidity. Moreover, since the cured product of the resin composition has improved practical light resistance and thermal shock resistance, it is judged to be qualified as a whole. 0 133 32] 346 201004993 [Example 29] In the same manner as in Example 27, according to the following Tables 4 and 5, the resin composition and the cured product thereof were evaluated. The resin composition and the cured product thereof were evaluated in the same manner as in the above Example 2. The evaluation results and the mixed indexes were evaluated. α 36 to 36, storage stability index 0 36 is shown in Table 6. The condensation rate of the intermediate Κ 3 (%) = 85. 3% ^ 78%. The condensation rate of the modified resin composition L3 (%) = 86. 8 %^80%. The amount of residual alkoxy groups in the modified resin composition 0% each 5%. As shown in the following Table 6, the epoxy resin amount (WPE) of the resin composition of Example 29 was 242 g/eq, which showed an appropriate value. Further, 'starting viscosity=14·3 Pa· s<10〇〇Pa· s, save test sound = 41· 0 Pa · s &lt; 1000 Pa · s, both are liquid liquids. Also, preservation stability index 0 36=2. 9 S 4 'The fluidity is excellent, and it is known that the resin composition has been changed to maintain stability. The index of the light resistance test of the cured product is γι=8 9$13, which is judged to be practically sufficient light resistance. The number of thermal shock tests is 25 times. (4) It is judged that there is practically sufficient thermal shock resistance. It is known that the resin composition of Example 29 has fluidity f@ μ # =, the child is qualitative, and the cured product of the resin composition is practical. In addition to the resistance to cold and thermal shock resistance, it is determined that the combination is the same as the above-mentioned Example 27, according to the following Table 4 and Table 5, A resin composition and a cured product thereof were produced. The resin composition and the cured product thereof were the same as in the above Example 27. The evaluation results, the evaluation results α 37 to ε 37, and the storage stability index 0 37 are shown in Table 6. The condensation rate of the intermediate Κ 4 (° / 〇 = 87. 4% 2 78 ° / 〇. The condensation ratio of the resin composition is L4 (%) = 88.8% 280 ° / 〇. The amount of residual alkoxy groups of the modified resin composition is 0% by weight 5%. As shown in Table 6 below, Example 30 The epoxy equivalent (WPE) of the resin composition = 238 g/eq, showing an appropriate value. Further, the initial viscosity = 15.6? 8.5 &lt; 1000 ? 3.5, and the storage viscosity = 24. 9 Pa · s &lt; 1000 Pa · s, both of which are fluid liquids. In addition, the storage stability index Θ 37=1. 6S4 is excellent in fluidity, and it is known that the composition of the tree wax having improved stability is improved. The index YI of the cured product of the cured product YI=8. 8 S 13 ' was judged to be Q practically sufficient light resistance. The number of thermal shock tests was 150 times 2 50 times, and it was judged that there was a practically sufficient cold shock resistance. From the above results, the resin composition of Example 30 is excellent in fluidity and improved in storage stability, and the cured product of the resin composition has practically sufficient light resistance and thermal shock resistance, so that comprehensive judgment is made. To be qualified. [Example 31] In the same manner as in the above-mentioned Example 27, according to the following Table 4 and Table 5, 135 321346 201004993 was used as a resin composition and a cured product thereof. The resin composition and the cured product thereof were evaluated by the same method as in the above Example 27. The evaluation results, the mixing index α 38 to ε 38 , and the storage stability index 0 38 are shown in Table 6 below. The condensation rate of the intermediate Κ 5 (° / 〇 = 82.6 ° / 〇 2 78 ° /. The condensation rate of the modified resin composition L5 (« = 87.2% 280 ° / 〇. modified resin composition The amount of residual alkoxy group was 0% $ 5 ° / 〇. As shown in Table 6 below, the epoxy equivalent of the resin composition of Example 31 (WPE) = 245 g/eq, which showed an appropriate value. Viscosity = 17. 3Pa· s &lt; 1000 Pa·s, and preservation viscosity = 5 0. 2 Pa · s &lt; 10 0 0 Pa · s, both are fluid liquids. Also, preservation stability index Θ 38=2. 9^4, which is excellent in fluidity, and is known as a resin composition having improved storage stability. The index of the light resistance test of the cured product is YI=8. 2S 13, and it is judged that there is practically sufficient light resistance. The number of the thermal shock test was 150 times and 2,50 times, and it was judged that the thermal shock resistance was practically sufficient. From the above results, the resin composition of Example 31 was excellent in fluidity and improved in storage stability. Further, since the cured product of the resin composition has practically sufficient light resistance and thermal shock resistance, it has been judged to be acceptable as a whole. [Example 32] In the same manner as in Example 27, a resin composition and a cured product thereof were produced according to the following Tables 4 and 5. 136 321346 201004993 The resin composition and the cured product thereof were evaluated in the same manner as in the above Example 27. The mixing index α 39 to ε 39 and the storage stability index 0 39 are shown in the following Table 6. The condensation ratio of the intermediate K6 (° / 〇 = 82.8 ° / 2 78 ° / 〇. The modified resin composition The condensation ratio L6 (%) = 83. 2% 280%. The amount of residual alkoxy group of the modified resin composition was 0% '5%. As shown in Table 6 below, the epoxy equivalent of the resin composition of Example 32. (WPE) = 253 g / eq, showing the appropriate value. ^ Again, the initial viscosity = 24. 3Pa · s &lt; lOOOPa · s, and, save the viscosity = 86. 3Pa · s &lt; lOOOPa · s, both have Liquidity of liquidity. Further, the storage stability index is 0 39=3. 6S 4 , and the fluidity is excellent, and it is known that the resin composition has improved stability and stability. The indicator of the light resistance test of the cured product YI = 9. 7S 13 It is judged that there is practically sufficient light resistance. Moreover, the number of thermal shock tests is 250 times ^ 50 times, and it is judged to be practically sufficient. From the above results, it is understood that the resin composition of Example 32 is excellent in fluidity and has improved storage stability, and the cured product of the resin composition has practically sufficient light resistance and heat and cold resistance. In the same manner as in the above Example 27, the resin composition and the cured product thereof were produced in the same manner as in the above-mentioned Example 27, in the same manner as in the above-mentioned Example 27. The resin composition and the cured product thereof were evaluated in the same manner as in the above Example 27. The evaluation results, the mixing index α 40 to ε 137 321346 201004993 40, and the storage stability index 0 40 are shown in Table 6 below. The condensation rate of the intermediate K7 (%) = 83. 5 ° / 〇 278%. The condensation rate of the modified resin composition was L7 (%) = 84.4% 2 80%. The amount of residual alkoxy groups of the modified resin composition was 0% by weight of 5%. As shown in the following Table 6, the epoxy resin equivalent (WPE) of the resin composition of Example 33 was 210 g/eq, which showed an appropriate value. Further, the initial viscosity = 12. 8 Pa · s &lt; lOOOPa · s, and the storage viscosity = 39. 8 Pa · s &lt; lOOOPa · s, both are fluid liquids. In addition, the storage stability index Θ33=3.1$4 is excellent in fluidity, and it is known that the resin composition has been improved in stability. The indicator YI of the light resistance test of the cured product was judged to have practically sufficient light resistance. Further, the number of thermal shock tests was 350 times 2 50 times, and it was judged that there was practically sufficient cold shock resistance. From the above results, it is understood that the resin composition of Example 3 is excellent in fluidity and improved in storage stability, and the cured product of the resin composition has practically sufficient light resistance and thermal shock resistance. The overall judgment is qualified. [Example 34] A resin composition and a cured product thereof were produced in the same manner as in the above Example 27, according to the following Tables 4 and 5. The resin composition and the cured product thereof were evaluated in the same manner as in the above Example 27, and the evaluation results, the mixing indexes α 41 to ε 41 and the storage stability index 0 41 are shown in Table 6 below. The condensation rate of the intermediate Κ 8 (%) = 84. 2% 2 78%. 138 32] 346 201004993 The condensation rate of the modified resin composition L8 (%) = 84. 4% 280 ° / 〇. The amount of residual alkoxy groups of the modified resin composition was 0% $5 ° / Torr. As shown in the following Table 6, the epoxy resin equivalent (WPE) of the resin composition of Example 33 was 233 g/eq, which showed an appropriate value. Further, the initial viscosity = 13. 2 Pa · s &lt; lOOOPa · s, and the storage viscosity = 46. 8 Pa · s &lt; lOOOPa · s, both are liquid liquids. Further, the storage stability index 0 41 = 3.5 S 4 was excellent in fluidity, and it was found that the resin composition having improved stability was improved. ^ The indicator of the light resistance test of the cured product YI = 7. 3S 13, which was judged to have light resistance. In addition, the number of thermal shock tests was 150 times and 50 times, and it was judged as having ί thermal shock resistance. From the above results, it is understood that the resin composition of Example 34 is excellent in fluidity and has improved storage stability, and the cured product of the resin composition has practically sufficient light resistance and thermal shock resistance, so comprehensive judgment To be qualified. 5小时。 The hour of the dehydration condensation step at 80 ° C for 5 hours, the distillation time was changed to 2.5 hours. The rest of the conditions were the same as in Example 27, and a resin composition was produced according to Table 4, and evaluated in the same manner as in Example 27. The evaluation results, the mixing indexes α 42 to ε 42 , and the storage stability index 0 42 are shown in Table 6 below. The condensation rate of the intermediate Κ9 (%) = 78. 2%278%. The condensation rate of the modified resin composition was L9 (°/D) = 79. 0% &lt; 80%. The amount of residual alkoxy groups of the modified resin composition was 5%. 139 321346 201004993 As shown in the following Table 6, the resin composition of Example 35, /eq, shows an appropriate value. Also, the initial viscosity ^ oxygen ^ s &lt; HHH) Pam ' preservation viscosity = 68 both flow axis _ H stored mosquito pure (four) spit 5 'the modified resin condensation rate is not reached, but the fluidity Excellent, it is known that the resin composition has been improved in storage stability. The index of the light resistance test of the cured product YI = 8.1 $13 was judged to have light resistance. Further, the number of thermal shock tests was determined to be cold shock resistance by 25 ^ ^ 5 〇 times. &quot; From the above results, it is understood that the resin composition of Example 35 is excellent in fluidity and has improved storage stability, and the cured product of the resin composition has practically sufficient light resistance and thermal shock resistance. The overall judgment is qualified. [Comparative Example 10] The curing temperature of (14) shown in the above Example 27 was changed to ❹1HTC for 4 hours, and further 15 (rc, ! hours. Other conditions were the same as Example 27). Table 4 and Table 5, t as a resin composition and a cured product, were evaluated in the same manner as in Example 27. The evaluation results, the mixing index α 43 to ε 43 , and the storage stability index Θ 43 are shown in Table 6 below. The condensation ratio of the intermediate Κ10 (%) = 71. 1% &lt; 78%. The condensation ratio of the modified resin composition L10 (%) = 75.4 · 〇 % &lt; 8 〇 %. The residual amount of the antioxidant was as shown in the following Table 6. The epoxy equivalent of the resin composition of Comparative Example 10 was 321346 140 201004993 (WPE) = 200 g/eq, which showed an appropriate value. Further, the initial viscosity = 11.7 卩&.5&lt;1000?&*5. However, the viscosity is kept > 100OPa · s, showing no fluidity, the stability index is saved at 0 43 &gt; 85, and the stability is poor. As shown in Table 6, The cured product obtained by the resin composition of Comparative Example 10 has good light resistance and thermal shock resistance, but the storage stability of the resin composition is good. In the same manner as in the above-mentioned Example 27, a cured product was produced in the same manner as in Example 27 below. The cured product was evaluated in the same manner as in Example 27. The evaluation results are shown in the following Table 6. The index of the light resistance test of the cured product is YI = 16.9&gt; 13, and it is judged that there is no practically sufficient light resistance. Moreover, the number of thermal shock tests is 500 times or more and 250 times, and the judgment is made. In view of the above results, the cured product of Comparative Example 11 was resistant to cold and heat, but had no light resistance, and was judged to be unacceptable by comprehensive judgment. [Comparative Example 12] By using a polyoxyxylene resin ("SCR-1012 (A liquid and sputum)" manufactured by Shin-Etsu Chemical Co., Ltd.), the mixture of the A liquid and the B liquid is mixed at a mass ratio of 1:1, as follows. In the same manner as in Example 26, a solution for a cured product was prepared in the same manner as in Example 26. In the same manner as in Example 27, the molding jig and the above-mentioned substrate for the above-mentioned thermal shock test were injected. Hardened solution, again, in each One sheet of tantalum wafer was placed in each of the plates. 141 321346 201004993 The above-mentioned forming jig and the substrate for thermal shock test were placed in an oven, and hardened at 70 ° C for 1 hour and further at 150 ° C for 5 hours. The cured product was treated in the same manner as in Example 27. The evaluation results are shown in the following Table 6. The index of the light resistance test of the cured product was YI = 2. 0^13, and it was judged as It is practically full of light resistance. However, the number of thermal shock tests was 0 times &lt; 50 times, and it was judged that there was no practically sufficient cold shock resistance. From the above results, it was found that the cured product of Comparative Example 12 was not rich in thermal shock resistance, but was not judged to be unacceptable. [Comparative Example 13] The reflux step was changed to 7 hours, and the dehydration condensation step was carried out for 25 hours. Other conditions were the same as in Example 27, and a resin composition was produced according to Table 4, and evaluated in the same manner as in Example 27. The evaluation results, the mixing index α 44 to ε 44, and the storage stability index 0 Θ 44 are shown in Table 6 below. The condensation rate of the intermediate Kll (%) = 64. 8 ° / 〇 &lt; 78%. The condensation ratio of the modified resin composition was Lll (° / 〇 = 68. 0 ° / . &lt; 80%. The amount of residual alkoxy groups of the modified resin composition was 7% &gt; 5%. As shown in Table 6 below The epoxy equivalent (WPE) of the resin composition of Comparative Example 13 was 233 g/eq, which showed an appropriate value. Further, the initial viscosity = 15.2 Pa · s &lt; 10 0 0 Pa · s. However, the preservation viscosity &gt; 10 0 0 Pa · s, showing no fluidity, preservation stability index Θ 44 &gt; 66, the stability of storage is poor, so the comprehensive judgment is unqualified. 142 323346 201004993 As described above, even if the time of the dehydration condensation step is extended, Since the storage stability of the resin composition did not reach the acceptable line, it was found that the characteristics of the resin composition were largely dependent on the condensation ratio (chemical structure) of the intermediate in the reflux step. [Comparative Example 14] Reflow was performed. The oil bath temperature of the step was changed to 60 ° C. Other conditions were the same as in Example 27, and a resin composition was produced according to Table 4, and evaluated in the same manner as in Example 27. ® Evaluation result, mixing index α 45 to ε 45, storage stability index 045 is shown in Table 6 below. The condensation ratio Κ12 (%) = 63.6% &lt;78 ° / 〇. The condensation ratio of the modified resin composition L12 (%) = 65.4% &lt; 80%. The amount of residual alkoxy groups of the modified resin composition It is 12% &gt; 5%. As shown in the following Table 6, the epoxy equivalent of the resin composition of Comparative Example 14 (\^£) = 238 cliffs / 69, showing an appropriate value. Further, the initial viscosity = 16.4 卩&amp;· 0 s &lt; 1000 Pa · s. However, the storage viscosity &gt; 1000 Pa · s, showing no fluidity, preservation stability index 0 44 &gt; 61, preservation stability is bad, so the comprehensive judgment is unqualified As shown in Tables 4 to 6, it is understood that if the epoxy resin is mixed with a specific alkoxylated compound in a specific ratio, and the condensation ratio of the intermediate in the reflux step of the cohydrolysis condensation is specified, after that, The resin composition of Examples 27 to 35 which is produced by dehydrating condensation and imparting a specific condensation ratio of the modified resin composition, has excellent fluidity and storage stability, and the cured product of the resin composition All have excellent light fastness and cold resistance 143 321346 201004993 Thermal shock resistance. οο times £: uniform 钵 矽 矽1 1 1 i 1 1 1 1 1 1 1 ο 1 Hydrolysis condensation catalyst 1 1 1 1 1 1 1 I 1 1 1 1 1 0.64 DBTOM 0.24 0.15 S3 Ο 0.15 0.28 0.17 0.19 0.15 0.15 1 1 1 1 0.15 _Λ I 0.24 1 1 I 1 1 1 0.24 0.33 1 i 1 1 〇0 〇〇10.9 10.0 10.9 10.2 10.7 10.2 10.9 10.9 10.9 1 i 11.0 a&gt; t-BuOH 1 1 20.7 1 1 1 1 1 1 1 1 ii 16.5 20.3 1 20.4 ΙΛ CSI 20.6 20.4 20.4 20.3 20.4 1 1 20.2 20.4 Alkyl hydrazine 1 〇C&gt; ο d 〇o ΙΛ CD C&gt; 〇o Ο Ο 〇c&gt; Ο Ο ο CD c&gt; oo c&gt; CD CD 兮' 〇ΙΛ ο Id o to CO CO CO CS3 ο trf o LfS ο uri ! I 〇iri o iri 1 eo 05 11.8 CO t 11.9 «1 19.7 m Bu · 11.9 OO 11.9 i 1 11.8 11.9 1 19.3 23.9 24.3 23.9 22.3 I 05 oo 31.2 05 CO CM 23.9 23.9 1 1 OO CO 03 23.9 Alicyclic ring fine grease 1 i 1 1 1 ( 1 OO csi 1 27.7 ! 1 i 1 i ! Bis-A ring IUH fat 1 CO *_丨&lt; 27.7 od CM 27.7 25.9 cc&gt; 28.3 25.0 27.7 1 100.0 1 27.6 L 2u_ Composition ratio Example 27 1 Example 28 1 Example 29 丨 Example 30 I Example 31 Example 31 Example 33 Example 34 Example 35 \kMM 10 Comparative Example 11 Comparative Example 12 Comparative Example 13 Comparative Example 14 144 321346 201004993 Table 5 Unit: % by mass Composition ratio Resin composition Bis-A Epoxy resin polyoxyl resin hardener hardening accelerator Example 27 57. 2 — 42. 6 0. 2 Example 28 58. 6 — — 41. 2 0. 2 Example 29 59. 5 — — 40. 3 0. 2 Example 30 59. 1 — — 40. 7 0. 2 Example 31 59. 8 — — 40 0. 2 Example 32 60. 6 — — 39. 3 0. 2 Example 33 56. 1 — — 43. 8 0. 2 Example 34 58. 6 — — 41. 2 0. 2 Example 35 58. 6 — — 41. 2 0. 2 Comparative Example 10 54. 9 — — 45. 0 0. 2 Comparative Example 11 — 53. 2 — 46. 6 0. 2 Comparative Example 12 — — 100. 0 — —

145 321346 201004993 9 &lt;ο❹ 55 Umbrella ± : χ, 鸯 Umbrella: 9 ◎ <^家〉 Comprehensive judgment 〇〇〇〇o 〇〇〇〇XXXXX Hard recording cold-resistant touch determination 〇〇〇〇〇〇〇〇〇〇 〇X 1 1 times S CO S ρα S CO ggg S CO S i 2500 o 1 1 Light resistance determination 〇〇〇〇〇〇〇〇〇〇X 〇1 11.9 οο σ» οό οο od 00 卜 ai LO CO 卜· CO 16.9 S i Resin composition storage stability % ◎ ◎ ◎ ◎ ◎ ◎ ◎ ◎ 〇 X 1 .1 1 Index 0 ee οί CO 03 CO 〇&gt;c&lt;i CD co :· tn n ΙΛ — 臣/s 1 1 s viscosity retention viscosity 32.5 53.8 41.0 50.2 86.3 39.8 46.8 68.0 gelation (&gt;1000) 1 1 (&gt;1000) (&gt;1000) initial viscosity 12.7 15.9 14.3 , 15.6 17.3 24.3 12.8 13.2 LO — 2 1 1 CQ Isi 16.4 1 1 i CSI CM 1 Lft s eo LO O CO § I 1 1 CO DO οο Convergence rate when upgrading trees (X) 86.6 81.8 86.8 i 88.8 87.2 83.2 84.4 84.4 79-0 1 75.4 i 1 68.0 65.4 Intermediate Jtt condensation rate {%) Μ 80.1 78.2 85.3 87.4 82.6 82.8 83.5 84.2 78.2 1 1 QO 63.6 Washing index (〇 1 .07 1.07 ο gg SS 1 1 1.08 1.07 *〇0.018 0.0018 0.0014 1 0.0009 0.0018 I 0.001 0.0012 0.0014 0.0018 0.013 1 1 0.0018 0.0009 1.26 1.26 0.69 0.68 0,67 1 0.67 0.69 0.68 1.26 0.B8 1 1 0.68 0.68 0.26 0.26 0.26 0.26 .0.25 0.11 «μ O 0.26 0.26 0.26 1 1 0.26 0.26 « 0.5914 0.5914 0.5716 I 0.5914 I 1 0.5914 I 1.2423 0.2858 I 0.5914 0.5914 0.5914 1 1 0.5894 0.5914 Evaluation of dryness indicators compilation a34~034, in, Ll | α35~ 035, K2, L2 | α36 ~ 036, K3 'L3 cz37 ~ 037, K4, L4 a38 ~ 038, K5, L5 a39 ~ 039, K6, L6 Real case 33 | a40 ~ a41 ~ 6M Bu K8, L8 ~ 042 , K9, L9 a43~043, KlO, LlO ! i Z3 ψ • ta a45~0舫, K12, L12 Practical example / Comparative example 27 | Example 28 1 1 Example 29 1 | Example 30 I | Example 31 | Example 32 Remuneration 34 Real Example 35 tb Comparative Example 10 Comparative Example 11 Comparative Example 12 tbfe Example 13 146 321346 201004993 Next, regarding the addition of oxetane to the modified resin composition of the present embodiment The resin composition of the alkane compound is added by way of examples and comparative examples. To specify. The epoxy equivalent (WPE), viscosity, and mixing index &lt;2 to 7/ were obtained in the same manner as above. The evaluation of the physical properties in Examples 36 to 38 and Comparative Examples 15 to 16 was carried out as follows. &lt;Measurement of viscosity of composition&gt; ^ The container immediately after the composition was sealed, and the temperature was adjusted at 25 ° C for 1 hour, and then the viscosity at 25 ° C was measured. When the viscosity is below 100 OPa·s, it is judged to have fluidity. <Cured Property Test of Hardened Material> The light resistance of the cured product was evaluated by the following method. (1) The cured product prepared by the method described later is cured with a solution to prepare a cured product of 20 mm x 10 mm x 3 mm thick. 0 (2) The hardened material was covered with a black mask of 25 mm x 15 mm x thickness of 1.2 mm which had been punched with a hole of 5. 5 mm in diameter, and was used as a sample for the test of the viscous light. (3) The preparation device was used to irradiate the UV light from the UV irradiation device ("Spot Cure SP7-250DB" manufactured by Ushio Electric Co., Ltd.) to the above-mentioned sample in an incubator set to a constant temperature of 50 °C via an optical fiber. (4) The above sample was placed in an incubator at 50 ° C in a state where the black mask was placed on the top. (5) UV light of 2 W/cm2 was irradiated for 96 hours from the upper portion of the black cover 147 321346 201004993 by irradiating UV light to a hole having a diameter of 5.5 mm. (6) A sample irradiated with UV was measured by a spectroscopic color meter ("SD5000" manufactured by KK Electronics Co., Ltd.) which has been modified into a diameter of 10 mm. (Ό Yellowness (YI) is obtained according to "ASTM D1925-70C1988: Test Method for Yellowness Index of Plastics". When the YI was 11 or less, it was judged to have light resistance &lt;breaking test of cured product&gt; The presence or absence of cracking of the cured product was evaluated by the following method. (1) Prepare the substrate as shown below. • Substrate: manufactured by Solvay Advanced Polymers, "AM0DEL A-4122NL WH 905" (in the center of a flat plate of 15mm x l5mm x 2mm, with a diameter of 1 Ommx, a depth of 1. 2, 1). (2) Making 5 methods to be described later The prepared hardened material solution flows into the above substrate, and the hardened person is used as a test for a crack test. (3) For the above sample, a permeate ("MICR0-CHECK" manufactured by K0HZAI Co., Ltd.) was sprayed.] The presence or absence of cracking was visually observed under a magnifying glass, and the number was recorded. (4) When four of the five samples did not show cracking, it was judged to have crack resistance. &lt;Surface adhesion test of cured product&gt; The surface adhesion of the cured product was evaluated by the following method. (1) The cured product prepared by the method described later was hardened with a solution to prepare a cured product having a thickness of 20 mm x 10 mm x 3 mm. (2) The surface of the obtained cured product was pressed with a thumb of a latex glove 148 321346 201004993, and when the adhesion was not confirmed, the surface adhesion was judged to be good. The raw materials used in Examples 36 to 38 and Comparative Examples 15 to 16 are shown in the following (1) to (12). (1) Epoxy Resin (1-1) Epoxy Resin A: Poly(bisphenol A-2-hydroxypropyl ether) (hereinafter, referred to as Bis-A epoxy resin) • Trade name: Asahi Kasei Epoxy Co., Ltd. Company system, "AER" In addition, the epoxy equivalent (WPE) and viscosity measured by the above method are as follows

• Epoxy equivalent (WPE): 187 g/eq • Viscosity (25 ° C): 14. 3 Pa · s (1-2) Epoxy resin B: 3, 4-epoxycyclohexylmethyl-3', 4'-epoxycyclohexyl carboxylate (hereinafter referred to as alicyclic epoxy resin) • Trade name: manufactured by Daicel Chemical Industry Co., Ltd., "Celloxide 2021P" 0 Further, the epoxy equivalent measured by the above method ( WPE) and viscosity are as follows. • Epoxy equivalent (WPE): 131g/eq • Viscosity (25°C): 227 mPa · s (2) Alkoxydecane compound Η : 3-glycidoxypropyltrimethoxy decane (hereinafter referred to as GPTMS) • Trade name: Shin-Etsu Chemical Co., Ltd., "ΚΒΜ-403" (3) Alkoxydecane compound I: Phenyltrimethoxydecane (hereinafter referred to as PTMS) 149 321346 201004993 • Trade name: Shin-Etsu Chemical Industry Co., Ltd., "ΚΒΜ-103" (4) Alkoxydecane compound J: dimethyl dimethoxy decane (hereinafter referred to as DMDMS) • Trade name: Shin-Etsu Chemical Co., Ltd. "KBM-22" (5) Alkoxylated cerium compound κ: tetraethoxy shixiyuan (hereinafter referred to as TE0S) • Trade name: Shin-Etsu Chemical Co., Ltd., "KBE-04" (6) Solvent (6-1) Tetrahydrocide: manufactured by Wako Pure Chemical Industries Co., Ltd., without ampoules (hereinafter referred to as THF) (ΌHydrolytic condensation catalyst: dibutyltin dilaurate (Wako Pure Chemical Industries Co., Ltd.) Company system, hereinafter referred to as DBTDL) (8) Heterocyclic butyl compound: 3-ethyl-{[3-ethyloxetan-3-yl]曱Oxime methyl}oxetane (manufactured by Toagosei Co., Ltd., "Aron oxetane OXT-221") (9) Cationic polymerization initiator ❹ • Trade name: Sanshin Chemical Industry Co., Ltd. , "San-aid

Si-100L" (10) Hardener: "4-Mercaptohexahydrophthalic anhydride / hexahydrophthalic anhydride = 70/30" • Trade name: New Japan Physical and Chemical Co., Ltd., "RIKACID MH-700G" (11 ) Hardening accelerator: Amine hardener • Trade name: San-apro Co., Ltd., “U-CAT 18X” (12) Polyoxyn resin • Trade name: Ding Yi 1' &amp; 7.0 Daisy (: 〇1_1^叩(share) company, "£〇6301 (eight 150 321346 201004993 liquid / B liquid)" (Synthesis Example 1) Resin composition A: tree furnace such as a, this * tree 曰 composition A The steps are manufactured and evaluated. (1) Preparation: The Lai Xinxin water tank is set to 5t: to return to the cooling pipe. Further, the mixer is placed on the 8 (TC oil bath. (2) According to Table 7 In the environment, in the environment, the alicyclic (four) resin, the alkoxy compound, and the person who has already invested in the search flask are mixed and stirred, m step is added water and hydrolysis condensation catalyst, and Mix and mix. (3) Next, install a cooling tube in the flask, quickly immerse it in an oil bath of 8 ° C and start stirring, and react for 8 hours while refluxing. (4) After the reaction is over Cool to 25 ° C, then remove the cooling tube from the flask, after the reflux step, take the sample solution. (5) The solution after the end of the reflux step, using the evaporator, at 4 〇〇 Pa, P 50 ° C After distilling for 1 hour, the mixture was further subjected to dehydration condensation reaction at 8 hours (TC was distilled off for 5 hours. (6) After completion of the reaction, the mixture was cooled to 25 ° C to obtain a resin composition a. (7) The resin composition was The mixing index α46 to ε 46 is shown in Table g. (8) Further, the epoxy equivalent (WPE) of the resin composition A obtained in the above (6) is measured according to the above method. The epoxy equivalent of the above resin composition ( WPE) = 158 g/eq, which showed an appropriate value. (Synthesis Example 2) 321346 151 201004993 Resin composition B: Resin composition B was synthesized and evaluated in the same manner as in Synthesis Example 1 according to the composition ratio of Table 7. The mixing index α 47 to ε 47 is shown in Table 9. The epoxy resin equivalent (WPE) of the above resin composition was 163 g/eq, which showed an appropriate value. (Synthesis Example 3) Resin composition C: According to Table 7 The composition ratio was the same as in Synthesis Example 1, and the resin composition C' was synthesized. The evaluation of the mixing index ® a 48 to ε 48 is shown in Table 9. The epoxy equivalent (WPE) of the above resin composition C = 160 g / eq ' shows an appropriate value. (Example 36) Composition 1 The product was produced and evaluated according to the following procedure: (1) 75 mass% of the resin composition A of the above Synthesis Example 1 and 25 mass% of the oxetane compound were mixed and scrambled, and further dried under vacuum. Degas and treat it as composition 1. The viscosity of the composition 1 was 1.82 Pa·s, which was a liquid excellent in fluidity. (2) In a composition of 99.2% by mass, 阳离子8 mass% of a cationic polymerization initiator is added and mixed, and degassing treatment is carried out under the same conditions as (丨) to prepare a solution for hardening. (3) The thickness of 3 mm: 7-shaped 矽 rubber 挟 is made between two sheets of coated steel sheet to form a forming fixture, so that the cured product made by the forming fixture becomes about 5 mm. About 20mmx thickness 3〇ππη. (4) It is prepared to inject the 321346 152 201004993 hardened solution described above into the forming jig and the five substrates for the above fracture test. In the hour of the experiment, the substrate was placed at 85t for 1 hour and further at 15 inches. 〇 Processed with 3 to make a cured product. (6) The results of the light resistance test and the surface adhesion test by the above method were the results of the light resistance test of the cured product, and the index of the light resistance test of the cured product was γι=6 8^'.

Financial property. Further, all of the five samples were not determined to have crack resistance. Moreover, the adhesion was not confirmed, but the crack was good and the sex was good. The double-surface adhesion was obtained by the above results. The composition of Example 36, the cured product of the composition was light-resistant and good, and was judged to be acceptable. Surface properties (Example 37) Composition 2 was produced by the following procedure and evaluated. (1) 7 parts by mass of the resin composition b of the above-mentioned Synthesis Example 2, and (for example, mass% of the azetidinium compound) were mixed (IV), and degassed in the same manner as in Example %, and was used as a composition. Object 2. The viscosity of the composition 2 was 2.78 Pa·s, which was a liquid excellent in fluidity. (2) In 99.4% by mass of the composition 2, 6% by mass of a cationic polymerization initiator was added and mixed, and a degassing treatment was carried out under the same conditions as in (1) to prepare a solution for hardening. (3) Using the above-mentioned solution for a cured product, a hardening treatment was carried out in the same manner as in Example , to prepare a cured product. 321346 153 201004993 The indicator of the photochemical test of this hardened material YI = 7. 9 S 11. It is judged to be light and light. Further, none of the five samples was cracked, and it was judged to have crack resistance. Further, since the adhesion was not confirmed, the surface adhesion was also good. From the above results, it was found that the composition 2 of Example 35 had fluidity, and the cured product of the composition had good visibility and cracking property, and the surface tackiness was also good. (Example 38) Composition 3 was produced by the following procedure and evaluated. (1) 80% by mass of the resin composition C of the above Synthesis Example 3 and 20% by mass of an oxetane compound were mixed and stirred, and degassed in the same manner as in Example 36, and was treated as Composition 3. The viscosity of the composition 3 is 2.27 Pa · s, which is a liquid excellent in fluidity. (2) In the composition 3 of 99.3% by mass, 0.7% by mass of a cationic polymerization initiator was added and mixed, and degassing treatment was carried out under the same conditions as in (1) to prepare a solution for hardening. (3) Using the above-mentioned solution for a cured product, a hardening treatment was carried out in the same manner as in Example 36 to prepare a cured product. The indicator of the light resistance test of the cured product YI = 8. 8S 11, which was judged to have light resistance. Further, four of the five samples did not undergo cracking, and it was judged to have crack resistance. Further, since the adhesion was not confirmed, the surface adhesion was also good. From the above results, it was found that the composition 3 of Example 38 had fluidity, and the cured product of the composition had good visibility, cracking property, and surface adhesion, and was judged to be acceptable. (Comparative Example 15) 154 321346 201004993 In the above-mentioned Bis-A epoxy resin and alicyclic epoxy resin, a hardener and a hardening accelerator were added in accordance with the composition ratio of Table 8 to replace the cationic polymerization initiator and mixed and stirred. Then, it was degassed under vacuum and used as a solution for hardening. Then, in the same manner as in Example 36, the above-mentioned cured solution was injected into the molding jig and the five fracture test substrates, and the cured product was cured at 110 ° C for 4 hours to produce a cured product. The results of evaluation in the same manner as in Example 36 are shown in Table 9. ❹ When the index of the light resistance test of the cured product is YI = 13.9 &gt; 11, it is judged that there is no light resistance. Further, four of the five samples were not cracked, and the crack resistance was steep, and the adhesion was not confirmed, and the surface adhesion was good. From the above results, it was found that the cured product of Comparative Example 15 was not light-resistant, and was judged to be unacceptable. (Comparative Example 16) The above-mentioned polysulfide resin was mixed with the mash and the mash at a mass ratio of i: i, and mixed (4) and used as a cured solution. Then, in the same manner as in Example 36, the above-mentioned cured solution was injected into the molding jig and the five substrates for the fracture test, and hardened at (10) C for 1 hour to prepare a cured product. The results of evaluation in the same manner as in Example 36 are shown in Table 9. The index of the light resistance test of the cured product was judged to be rich in light. In addition, 5 of the 5 samples were not confirmed to be broken, and (4) cracking. However, it was confirmed that there was a feeling of adhesion, so the surface adhesion was poor. From the above results, the cured product of Comparative Example 16 had light resistance and crack resistance, and 321346 155 201004993, but the surface adhesion was poor, so that the overall judgment was unacceptable. As shown in Tables 7 to 9, a resin composition system in which a ring-= substance is mixed at a specific ratio and co-hydrolyzed with a S3 composition and an oxetane compound is contained. The cured product of the resin composition is excellent in light resistance, crack resistance, and surface adhesion.

Unit: mass X composition ratio alicyclic epoxy resin Bis-A epoxy resin alkyl decyl decane compound THF water hydrolysis condensation catalyst DBTDL 0. 33 polyoxyl resin GPTMS PTMS 8. 6 DMDMS TEOS synthesis example 1 47. 1 — 17. 4 3. 6 — 14. 9 8. 0 Synthesis Example 2 45. 8 3.4 15. 7 7.8 2. 9 17. 1 7. 2 0. 29 Synthesis Example 3 IIU4 Comparative Example 15 46. 1 - 13. 0 13. 6 1.7 0. 4 17. 5 7. 5 0. 36 60. 0 40. 0 — 0. 0 One — _ Comparative Example 6 6 — — — 0. 0 *~~ — — 100. 0

Table 8 Unit: mass% Composition ratio composition alicyclic epoxy resin Bis-A epoxy resin polyxanthene resin ionic polymerization initiator hardening 剤 hardening promotion 剤 Example 36 Composition I 99. 2 — — — 0 8 - - Example 37 Composition 2 99. 4 - - __ 0. 6 - - Example 38 Composition 3 99. 3 - - - 0. 7 A comparative example 15 - 29. 0 19. 3 - 51. 6 0. 1 Comparative Example 16 一一—100. 0 — — 一156 321346 201004993 .-ΧΊ.όΛίν Comprehensive judgment 〇〇〇 XX hard ΊΜ 表面; surface adhesion judgment 〇〇〇〇X crack resistance t 〇〇〇〇〇 Light resistance judgment 〇〇〇X 〇〇〇CD Oi 卜·〇〇〇0 13.9 丨CO Composition viscosity determination 〇〇〇1 ! Initial viscosity 1_ 1.82 2.78 2.27 1 I Resin composition washing index 1〇1.07 Η 1 1 0.0013 0.0012 0.0014 1 1 ! 1.59 1 1.87 1 1 0.26 0.22 0.11 ' 1 0.5914 α47~ε47 |〇.5918 α48~ε48 | 1.2423 1 1 1 1 Evaluation result index number 1_α46 to ε46 Example / Comparative Example 3 (3 Example 37 Example 38 ratio Example 15] Comparative Example 16 157 321 346 201 004 993 Next, on joining the light of the present embodiment form a modified resin composition

The photosensitive resin composition obtained by the Ssc generating agent will be specifically described by way of examples and comparative examples. The epoxy equivalent (WPE), viscosity, and mixing index α to π were obtained in the same manner as above. The physical property evaluations of Examples 39 to 41 and Comparative Examples π to 19 were carried out as follows. Ο 鬌 &lt;Measurement of viscosity of photosensitive resin composition&gt; The container in which the composition immediately after the production was placed was sealed. After adjusting the temperature at 25 ° C for 1 hour, the viscosity in 25X: was measured. When the viscosity is 1 OOOPa·s or less, it is judged to have fluidity. &lt;Production Method of Coating Film a&gt; A coating film was produced under the following conditions in the air, at a temperature of 23 t: and a humidity of 55 % RH. (1) Prepare the following substrates and wipe the surface with ethanol (99.5%, manufactured by Wako Pure Chemical Industries, Ltd.) to dry. Substrate: Polyethylene terephthalate resin (hereinafter abbreviated as PET) Polycarbonate resin (hereinafter referred to as PC) Polydecyl acrylate resin (hereinafter referred to as pmma) (2) Photosensitive composition of the examples The composition of the object or the comparative example was coated on the above substrate using a bar coater (#3). (3) The substrate was placed in a UV curing device (manufactured by Fusion uv Systems Co., Ltd., Japan), and was repeatedly operated three times under the following conditions to be hardened. Light source and amount of light: High-pressure mercury lamp (120 W/cm2) 321346 158 201004993 Conveyor speed: l〇m/min (4) Further, the substrate was heat-treated at 1〇〇1 for 1 hour to perform post-hardening. &lt;Production Method of Coating Film b&gt; A coating film was produced under the conditions of air, temperature 23 ° C, and humidity 55% RH in the following procedure. (1) The following substrates were prepared, and the surfaces were wiped with ethanol (99.5% manufactured by Wako Pure Chemical Industries, Ltd.) to dry them.

Substrate: PET (2) The photosensitive composition of the example or the composition of the comparative example was applied onto the above substrate using a bar coater (#3). (3) The above substrate was placed on a UV curing device (manufactured by Fusi〇n uv Systems Co., Ltd., Japan), and the operation was repeated five times according to the following conditions to harden the light source and the amount of light: a high-pressure mercury lamp (120W/CH12; φ Conveyor speed: 5 m/min &lt;Photos hardenability of the coating film&gt; The above coating film is applied [Jis K 5600H. 1999 Coating General Test Method - Part 5: Mechanical Properties of Coating Film - Chapter 4 The upper stroke method)] measured, when it is 3Β to 6Η, it is judged as * W strength (ship <adhesion of coating film> is good °

The above coating film was measured in accordance with [JIS K 5600-5-6: lQ test method - part 5: mechanical properties of the coating film - 6 r. 9 cross cut test). ~Sexuality (Loose cut 321346 159 201004993 The results were evaluated in the following three stages: 〇: almost no peeling was observed Δ: partial peeling X: almost all peeling When the result was shown to be better than the standard, it was judged that the adhesiveness was good. &lt;Comprehensive Judgment&gt; When the photosensitive resin composition has fluidity and the photocurability and adhesion of the coating film are good, it is judged to be acceptable in general. ® For use in Examples 39 to 41 and Comparative Examples 17 to 19 The raw materials are expressed in the following (1) to (9). (1) Epoxy Resin U-1) Epoxy Resin A: Poly(bisphenol A-2-hydroxypropyl ether) (hereinafter, referred to as Bis- A epoxy resin) • Trade name: manufactured by Asahi Kasei Epoxy Co., Ltd., "AER" The epoxy equivalent (WPE) and viscosity measured by the above method are as follows. • Epoxy equivalent (WPE): 187g/eq • Viscosity (25°C): 14. 3 Pa · s (1-2) Epoxy resin B: 3, 4-epoxycyclohexylmethyl-3', 4 '-Epoxycyclohexyl carboxylate (hereinafter referred to as alicyclic epoxy resin) • Trade name: manufactured by Daicel Chemical Industry Co., Ltd., "Celloxide 2021P" Further, the epoxy equivalent (WPE) measured by the above method And the viscosity is as follows. 160 321346 201004993 • Epoxy equivalent (WPE): 131g/eq • Viscosity (25°C): 227 mPa · s (2) Alkoxydecane compound Η : 3-glycidoxypropyltrimethoxy decane ( Hereinafter referred to as GPTMS) • Trade name: Shin-Etsu Chemical Co., Ltd., “KBM-403” (3) Alkoxydecane compound I: Phenyltrimethoxy decane (hereinafter referred to as PTMS) • Trade name: "SKM-103" ® (4) alkoxy decane compound J: dimethyl decyloxy decane (hereinafter referred to as DMDMS) • Trade name: Shin-Etsu Chemical Co., Ltd. "KBM-22" (5) Alkoxydecane compound K: tetraethoxy decane (hereinafter referred to as TEOS) • Trade name: Shin-Etsu Chemical Co., Ltd., "KBE-04" (6) Solvent (6-1) Tetrahydrofuran: manufactured by Wako Pure Chemical Industries Co., Ltd., does not contain An Q formula (hereinafter referred to as THF) (7) Hydrolysis condensation catalyst: Dibutyltin dilaurate (Wako Pure Chemical Industries Co., Ltd.) System, hereinafter referred to as DBTDL). (8) Photoacid generator: (8-1) Triisopropyl sulfonium hexafluorophosphate mixture • Trade name: manufactured by Union Carbide, "UV1-6990" (hereinafter referred to as UVI-6900) (8-2) Aromatic sulfur hexafluoroantimonate • Trade name: Sanshin Chemical Industry Co., Ltd., “San-Aid 161 321346 201004993 SI-80L” (hereinafter referred to as “si~8〇l”) (9) Oxygen heterocycle Butane compound (9 1) 3-ethyl-3-(p-oxymethyl) oxetane quotient, made by East Asia Synthetic Co., Ltd., "0XT-211" (hereinafter, abbreviated as Ρ0Χ) Synthesis Example 4) Tree sputum, and D. Resin oxime was produced and evaluated according to the following procedure. ® 0) Preparation: Set the temperature control bath to 5t to return to the cooling tube. Step-by-step on the magnetic stirrer to place 8 (TC oil bath. (2) According to the group 1G table ratio, in the environment of the alicyclic epoxy tree, oxyalkyl compound, and After adding the flask that has been thrown into the disturbing basket and mixing and mixing, further add water and hydrolysis condensation catalyst, and mix and mix. (3) Secondly, install the cooling tube in Wei, quickly dipped in 8 generations. In the oil bath 并 and start the Lin's surface reflux-surface reaction for 8 hours. (4) After the reaction is finished, 'cool down to 25t', then remove the cooling tube from the flask and take the solution. (5) Use the above-mentioned Lok solution After distilling off at 4 〇〇pa and 5 〇〇c for 1 hour, the hydrazine was subjected to a dehydration condensation reaction at 5 hours. (6) After the reaction was completed, it was cooled to 25 Torr to obtain a tree (four) compound (7). The mixing index α 49 to ε 49 of the composition is shown in Table 12. 321346 162 201004993 (8) Further, according to the above method, the epoxy equivalent (WPE) of the composition D of the above-mentioned (6) is determined. The composition had an epoxy equivalent weight (WPE) = 193 g/eq, which showed a suitable value of 2. Further, the viscosity U2.7Pa.s &lt;1()(K)Pa.s showed good (Synthesis Example 5) Resin composition E: The resin composition E was synthesized and evaluated according to the composition ratio of Table 10 in the same manner as in Synthesis Example 4. The mixing index "〇 to ε50 is expressed in In the above-mentioned resin composition, the epoxy equivalent (WPE) of the resin composition was 152 g/eq, which showed an appropriate value. Further, the viscosity was 0.93 Pa.s &lt; 1_pa.s, which showed good fluidity. 39) The photosensitive resin composition 1 and its coating film were produced and evaluated according to the following procedure: © () Using the resin composition D of the above Synthesis Example 4, mixing and stirring according to the blending method of Table 11, and further removing under vacuum The gas is used as a photosensitive resin composition. The photosensitive resin composition has a viscosity of 12·6 Pa · s &lt; i〇〇〇pa · s, which is a liquid excellent in fluidity. (2) According to the above [coating In the method for producing a film a], the photosensitive resin composition i is applied to the above-mentioned three types of substrates (PET, PC'PMMA), and a coating film is formed using a uv curing device. (3) The coating film is [JIS K5600- 4: General test methods for i999 coatings - Part 5: Mechanical properties of coatings - Section 4: Scratch resistance (lead 163 321346 201004993 Stroke)] The results of the measurement are shown in Table 12. (4) The above coating film is applied [JIS K5600-5_6: 1999 Coatings - General Test Method - Part 5: Mechanical Properties of Coating Films - Section 6 Adhesiveness (crosswise = the results of the measurement are shown in Table 12. As described above, the photosensitive resin composition 1 is excellent in fluidity, and the photocuring property of the coating film is good, and compared with the comparative example as a standard. , its program is better, so the comprehensive judgment is qualified. (Embodiment 40)

In the same manner as in Example 39, a glazing resin composition 2 was produced in the same manner as in Example 39. However, the conveyor speed of the 'UV hardening device is set to l〇m/min. The evaluation results are shown in Table 12. Further, sighs 3. 2Pa · s &lt; l〇〇〇pa · The viscosity of the photosensitive resin composition 2 is s ' is a liquid excellent in fluidity. As described above, the photosensitive resin composition 2 is excellent in fluidity, and is excellent in light hardenability due to coldness, and is more excellent in comparison with the comparative example as a standard. (Example 41) A photosensitive resin composition 3 was produced according to the blending method of Table 11, and evaluated in the same manner as in Example 39. The sticking property of the photosensitive resin composition 3 a 1.0 Pa· S &lt; l〇〇〇 Pa.s is a liquid excellent in fluidity.疋 Next, using the above-mentioned photosensitive resin composition 3, the m-plate is produced according to the above-mentioned f-coating film. The result is shown in ^2. As described above, the photosensitive resin composition 3 has excellent fluidity, and the film 321346 164 201004993 has good photocurability, and the adhesion is better than that of the comparative example 19' which is the standard. (Comparative Example 17) A photosensitive resin composition 4 was produced in the same manner as in Example 39 according to the blending method of Table 11. The evaluation results are shown in Table 12. The viscosity of the photosensitive resin composition 4 is 13.8 Pa·s &lt; 1 〇〇〇 Pa·s, which is a liquid excellent in fluidity. However, as shown in Table 12, the photosensitive resin composition 4 was excellent in fluidity ®, but the adhesion of the coating film was poor, so that it was judged to be unacceptable. (Comparative Example 18) A photosensitive resin composition 5 was produced in the same manner as in Example 39, according to the blending method of Table 11. GPTMS was used as the decane coupling agent. The results of the evaluation are shown in Table 12. The viscosity of the photosensitive resin composition 5 is 12.1 Pa · s &lt; 1 〇〇〇 Pa • s, which is a liquid excellent in fluidity. ◎ However, as shown in Table 12, the photosensitive resin composition 5 was excellent in fluidity, but the effect of improving the adhesion of the coating film was not observed, so that it was judged to be unacceptable. (Comparative Example 19) A photosensitive resin composition 6 was produced in the same manner as in Example 39, according to the blending method of Table 11. The evaluation results are shown in Table 12. The viscosity of the photosensitive resin composition 6 is pa. 3 pa · s &lt; 1 〇〇〇 Pa · s, which is a liquid excellent in fluidity. However, as shown in Table 12, the photosensitive resin composition 6 was excellent in fluidity 165 321 346 201004993, but it was judged to be unacceptable because of the poor adhesion of the coating film. From the results of Tables 10 to 12, it is understood that the resin composition obtained by co-hydrolyzing and condensing an epoxy resin with a specific alkoxydecane compound and the photosensitive resin composition of the photoacid generator have excellent fluidity. The coating agent and the coating film which are obtained by using such a photosensitive resin composition are excellent in photocurability and adhesion. Table 10

Unit: mass! 3⁄4 composition ratio Bi sA epoxy resin alicyclic epoxy resin alkoxy decane compound THF water hydrolysis condensation catalyst GPTMS PTMS DMDMS TEOS DBTDL Synthesis Example 4 46. 7 — 24. 6 2. 6 1.6 — 17 . 2 7. 0 0. 33 Synthesis Example 5 — 47. 8 22. 5 5.4 1. 6 0. 2 14. 8 7. 4 0. 30 166 321346 201004993 II嵴οο Light Contact Agent SI-80L 1 1 1 1 1 1 UVI-6990 〇CO 〇CO Ln 〇CO 〇CO LTD (ms 1 1 1 1 〇cJ 1 secret ring butaneization § 1 40.0 1 1 1 1 alicyclic ring decanted i 1 1 1 1 1 ΙΩ U Bis-A ring tilt 1 1 1 97.0 1 95.0 1 Resin composition E 1 1 1 1 1 1 Resin composition D 〇〇1 1 1 l Composition ratio Photosensitive resin composition 1 Photosensitive resin composition 2 1 Photosensitivity Resin Composition 3 Photosensitive Resin Composition 4 Photosensitive Resin Composition 5 Photosensitive Resin Composition 6 Example 39 Example 40 Example 41 Comparative Example 17 Comparative Example 18! Comparative Example 19 167 321346 201004993 o zl&lt;&quot; X - *E^S« &quot;&lt;&lt; - OA^^V Comprehensive judgment〇〇〇«r X 跻m\Jh pure M4 t 〇〇〇% X «- i 〇〇1 XX 'd 〇〇1 X &Lt;1 1 g 〇〇〇X Ο-Δ 0 i 练 bfi t 〇〇〇〇〇〇i - i = 1 目 g 1 臣 = 1 1 = mg S g 剤 剤 composition determination 〇〇 0 〇〇〇 t Initial viscosity i 12.7 CO 0.93 13.8 CO cj Resin composition i?L combination finger u&gt; 1 1.03 I 1.02 1 1 1 ί〇0.0014 0.0012 1 1 1 κ CO CO S 1 1 ! Free·« ψ^· ο 0.11 1 1 1 e 0.125 0.2857 1 1 W Ancient result i index edit % 03 TP i〇l α» es (ϋ is « 1 1 1 Example / Comparative Example 1 Resin composition tree temple touch D tsS im 1 1 1 *光酬物1 Weiwei W grease "a product 2 \- * optical tearing agent composition 3 Weiguang resin knows L product 4 Weiguang resin composition 5 Weiguang surface S New product 6 Example 39 Vibration Example 40 Example 41 Comparative Example 17 -1 Comparative Example 18 Comparative Example 19 168 321346 201004993 Next, the examples and comparative examples are given, and the phosphors are added to the modified resin composition of the present embodiment. The luminescent tree 2 was carried out under the evaluation of the physical properties of Examples 42 to 44 and Comparative Examples 20 to 23.

The epoxy equivalent (WPE), viscosity 'mixing index ^ to ^ the same method as above was obtained.

<Calculation of the preservation of the sputum and the preservation stability of the resin composition &gt; The preservation stability of the sapphire composition is evaluated by the storage stability index P shown by the following general formula (9). Preservation stability index preservation viscosity) / (starting viscosity)... (9) Seal the container of the resin composition immediately after manufacture, and adjust the temperature at 25 ° C for 2 hours, then measure 25 〇 c The viscosity is taken as [initial viscosity]. ◎ In addition, the container of the resin composition was sealed, and then stored in an incubator at a constant temperature of 25 ° C for 2 weeks. After storage, the viscosity at 25 ° C was measured, and this was taken as [preservation viscosity]. When the resin composition has fluidity (viscosity of 1000 Pa·s or less) and the storage stability index 0 is 4 or less, it is judged to have storage stability. &lt;Dispersion stability test of fluorescent resin composition&gt; After the production of the fluorescent resin composition, it was placed in a 50 ml glass bottle and sealed, and stored in an incubator kept at a constant temperature of 25 ° C for 5 hours. After storage, the appearance was observed to visually confirm the precipitation or uniformity of the phosphor. When the phosphor 169 321346 201004993 was not seen and the phosphor was uniformly dispersed, the dispersion stability was judged to be acceptable. &lt;Light resistance test of cured product (cured product of resin composition)> The cured product in which solid matter (fluorescent body) is dispersed is yellow. Therefore, a cured product was produced from a resin composition to which no phosphor was added by the following method, and the evaluation results were evaluated as light resistance. (1) The cured product prepared by the method described later is hardened with a solution to prepare a cured product having a thickness of 3πππ of min xl Omni X. ❹ (2) The hardened material was covered with a black mask of 25 mm x 15 mm x thickness of 1.2 mm which had been punched with a diameter of 5. 5 mm, and used as a test sample for light resistance test. (3) Preparation device The UV light was irradiated from the UV irradiation device ("Spot Cure SP7-250DB" manufactured by Ushio Electric Co., Ltd.) to the above-mentioned sample in an incubator set to a constant temperature of 50 °C via an optical fiber. (4) The above sample was placed in an incubator at a constant temperature of 50 ° C in a state where the black mask was placed on the upper surface. ❹ (5) UV light of 2 W/cm 2 was irradiated for 96 hours from the upper portion of the black mask so that the UV light was irradiated to the hole having a diameter of 5. 5 mm. (6) A sample irradiated with UV was measured by a spectroscopic color meter ("SD5000" manufactured by KK Electronics Co., Ltd.) which has been modified into a diameter of 10 mm. (Ό Yellowness (YI) is based on "ASTM D1925-70 (1988): Test

Here, when YI is 13 or less, it is judged as pass. <LED luminescence test> 170 321346 201004993 LED is lit to visually confirm the color tone, relative to undoped LED with phosphor "When the hue changes from blue to white, it is considered to be luminosity. &lt;Luminescence test of light-storing material (measurement of afterglow time)&gt; For sample use [JIS Z9107: 2008 Safety Marking - Performance Classification 'Performance Benchmarks and Test Methods' The commonly used light source fluorescent lamp D65 'is irradiated with 200 lux (iux) for 2 〇 minutes. After irradiation, the brightness of the residual light is measured by the brightness meter ^ The time until 0 mcd/m2 or less is regarded as the afterglow time. When the afterglow time is 12 〇 or more, the luminescence is judged to be acceptable. <The reliability test of LED (i) (continuous operation test: Referred to as [l test]) &gt; 10 LED' according to [MIL-STD-750E (Test Methods For Semiconductor Devices)] METHOD 1026·5 (Steady-State Operation) 〇Life)) and [M IL-STD-883G (Microcircuits)] METHOD 1005. 8 (Steady-State Life), evaluated under the following conditions: [IF = 20 mA ' Ta = 25 ° C ' 960 hours Turn on the light and measure the full beam (lin) before and after the lighting. Also 'Get the full beam maintenance rate (%) = (full beam after lighting) / (full beam before lighting) xl〇 〇], when the lowest value of the total beam maintenance ratio (%) of the full LED is 90% or more, it is judged as qualified. <LED reliability test (2) (thermal shock test: hereinafter referred to as [TS test] &gt; 171 321346 201004993 10 LEDs, according to [EIAJ ED-4701/300 (Test Method for Soil and Long-Term Test Methods for Semiconductor Devices (Strength Test I)) 3 0 7 (thermal shock test), The following conditions are evaluated. Take [-10 ° C (5 minutes) to 100 ° C (5 minutes)] as one cycle, after performing 100 cycles of thermal shock, confirm the number of LED lights, when 10 all When it is lit, it is judged as qualified. <LED reliability test (3) (temperature cycle test: hereinafter referred to as [TC] test) &gt; ❹ 10 LEDs, according to [EIAJ ED-4701/100C semiconductor Test Method 10 5 (Temperature Cycle Test) of the device's grief and durability test method (Faith Test I)) was evaluated under the following conditions. [40 ° C (30 minutes) to 85 ° C (5 minutes) to 100 ° C (30 minutes) to 25 ° C (5 minutes)] as a cycle, after performing 100 cycles of temperature cycle, It is confirmed that the number of LEDs is lit, and when all 10 are lit, it is judged as pass. ◎ In the evaluation of the above LEDs, when the light resistance and reliability tests (1) to (3) are all qualified, the overall judgment is qualified. The raw materials used in Examples 42 to 44 and Comparative Examples 20 to 23 are shown in the following (1) to (10). (1) Epoxy Resin (1-1) Epoxy Resin A: Poly(bisphenol A-2-hydroxypropyl ether) (hereinafter, referred to as "Bis-A Epoxy Resin") • Trade Name: Asahi Kasei Epoxy ( Company), "AER" In addition, the epoxy equivalent (WPE) and viscosity measured by the above method are as follows: 172 321346 201004993 Description • Epoxy equivalent (WPE) ·· 188 g/eq • Viscosity (25°C): 14. 8 Pa · s U-2) Epoxy Resin B: 3, 4-epoxycyclohexyldecyl-3',4'-epoxycyclohexylcarboxylate (hereinafter referred to as "alicyclic epoxy resin" ") Product name: "Del cel Chemical Industry Co., Ltd.", "Cel loxide 2021P" In addition, the epoxy equivalent (WPE) and viscosity measured by the above method are as follows: • Epoxy equivalent (WPE) · 131g/ Eq • Viscosity (25 ° C): 227 mPa · s (2) alkoxydecane compound (2-1) alkoxylated compound H: 3-glycidoxypropyltrimethoxy decane (below) It is called GPTMS) • Product name: Shin-Etsu Chemical Co., Ltd., "KBM-403" 〇 (2-2) alkoxy decane compound I: phenyl trimethoxy decane (hereinafter referred to as PTMS) • Goods Name: Shine Manufactured by Industrial Co., Ltd., "KBM-103" (2-3) Alkoxydecane Compound J: Dimercaptodimethoxydecane (hereinafter referred to as DMDMS) • Trade Name: Shin-Etsu Chemical Co., Ltd. , "KBM-22" (2-4) alkoxydecane compound K: tetraethoxy decane (hereinafter referred to as TEOS) • Trade name: Shin-Etsu Chemical Co., Ltd., "KBE-04" 173 321346 201004993 (3) Solvent: tetrahydrofuran: manufactured by Wako Pure Chemical Industries Co., Ltd., does not contain a stabilizer (hereinafter referred to as "THFj" (4) Hydrolyzed condensation catalyst: Dibutyltin dilaurate (Wako Pure Chemical Industries Co., Ltd.) 'hereinafter referred to as "DBTDL") (5) Hardener: [4-methylhexahydrophthalic anhydride/hexahydrophthalic anhydride 40/30] • Trade name: New Japan Physical and Chemical Co., Ltd. 'RIKACID leg ~7〇 〇〇" ❹ (6) Hardening accelerator: Amine compound • Trade name: San-apro Co., Ltd., "U_CAT 18X" (7) Reactive diluent: r丨, 2: 8, 9 epoxide Limonene" • Trade name: "Celloxide 3000" manufactured by Daicel Chemical Industry Co., Ltd. (8) Polymerization initiator: aromatic sulfonium salt Product Name: Sanyo Chemical Industry Co., Ltd. 'SanAidSI-lOOL' (9) Phosphor © (9-1) Phosphor A: "YAG: Ce3+ Phosphor" (Chemistry & Ptnics Co., Ltd.) (9-2) Phosphor b (light-storing phosphor): "SrAhO4: EU, Dy phosphor" (manufactured by Basic Specialty Chemicals Co., Ltd.) (10) Polyoxyl resin • Trade name: Toray · Dow Corning Co., Ltd.' "EG6301CA Liquid/B Liquid" [Synthesis Example 6] The resin composition was produced by the following procedure. 321346 174 201004993 () Prepare the 水槽 j j 温 温 温 温 温 温 温 温 温 温 温 温 温 温 温 温 温Further, an 8 〇t oil bath was placed on a magnetic stirrer. (2) According to the ratio of the composition of the gas 13 in the environment of 25 ° C, the above A1 € oxy resin, the oxime compound, and the THF # into the flask which has been mixed with the stirrer are mixed and disturbed. Further, water and a hydrolysis condensation catalyst are added and mixed. (3) Next, install a cooling tube in the flask, quickly soak the oil bath in the 8 〇 art and start stirring. Respond to the back of the 20-b b (return step). (4) After the reaction was completed, it was cooled to 25 ° C, and then the cooling tube was removed from the flask. (5) The solution after the completion of the refluxing step is distilled off at 4 Torr, 5 ° C for 1 hour using an evaporator, and further subjected to dehydration condensation reaction (dehydration condensation) while being distilled at 8 rc for 1 hour. Step (6) After the completion of the dehydration condensation reaction, the mixture was cooled to 25 ° C to obtain a resin composition. ❹ (Ό The mixing indexes α 51 to ε 51 of the resin composition are shown in Table 16 below. Further, the epoxy equivalent (WPE), the initial viscosity, and the storage viscosity of the resin composition obtained in the above (6) were measured by the above method. Further, the storage stability index Θ51' was obtained and shown in Table 16. The epoxy equivalent (WPE) = 228 g / eq' of the resin composition of the above Synthesis Example 6 shows an appropriate value. Further, the initial viscosity is 38.2 Pa.s &lt; 1000 Pa·s, and the storage viscosity = 61 1 Pa · s &lt; 1000 Pa · s, both are fluid liquids. Also, the storage stability index θ 51 = 1. 6S4, judged as 175 321346 201004993 has a fine composition for preservation stability. Example 7] shows that the step of returning W is changed to 6 hours, and the rest is in the same manner as in Synthesis Example 65. Tables 13 and 14 produce a resin composition, which is shown in Table 16 as a result of the same method as the synthesis = the mixed index α52 to e 52, and a storage stability index Θ52. 〇φ, for example, 16 is not 'synthesized. The epoxy equivalent (WPE) of the resin composition of Example 7 was 1 g eq , which was an inappropriate value. Further, the initial viscosity = Ha.s < 1 〇〇〇 Pa s and 'preservation degree = 3.1 Pa.s &lt; I〇〇〇pa.s, both are fluid liquids. Further, the storage stability index Θ 52=1. 72^4, and it was judged that there was a resin composition for preserving stability. [Example 42] After the resin composition of the above Synthesis Example 6 was stored at 25 C for 2 weeks, a cured product was produced and subjected to a Nike test. The results are shown in Table 16. (1) In the muscle environment, the above-mentioned (four) substance was hardened. Agent and hardening accelerator, mixed with Lin according to the composition ratio of Table 14, degassed under vacuum' as a solution for hardening. (2) Kicking the thickness of 3mm (4) into two stainless steel coated with release agent Between the plates, a forming jig is produced. (3) The above-mentioned solution for hardening is injected into the U to harden at 150 ° C for 1 hour. (4) After the temperature in the furnace is lowered to 3 (TC or less, the cured product is taken out, and the sample for light resistance test is prepared according to the above method. 321346 176 201004993 (5) Using the above sample' The results of the light resistance test conducted in the above manner are shown in Table 16. The index of the light resistance test of the cured product ΥΙ = 7.5 $13, and it was judged that the light resistance was acceptable. (6) Next, '90% by mass of the resin composition of Synthesis Example 6 was blended with 1% by mass of phosphor A' by a planetary mixer (manufactured by Inoue Seisakusho Co., Ltd.) and stirred for 10 minutes. The defoaming treatment was carried out, and this was regarded as a fluorescent resin composition. ❹ (?) The above fluorescent resin composition was poured into a 50 mL sample bottle and stored at 25 C for 5 hours. (8) After the storage, it was confirmed that there was no precipitation when the side surface and the bottom surface were visually observed, and the phosphor was uniformly dispersed. Therefore, the dispersion stability of the fluorescent resin composition was judged to be acceptable. The results of the evaluation are shown in Table 16. Further, the above-mentioned fluorescent resin and the resultant after storage for 2 weeks at 25 ° C were used, and a cannonball type LED was produced in the following procedure, and reliability tests (1) to (3) were performed. The results are shown in Table 16. The structure of the color-elastic LED has two lead frames, one of which (two forms a cup for mounting the LED chip. More progress, the above-mentioned fluorescent resin composition, hardener and hardening The agent is mixed and stirred according to the composition ratio of Table 15, and degassed under vacuum as an LED sealing material. (1〇) In the cup portion of the 5 mm diameter cannonball type mold frame, the LED sealing material of (9) is injected. An LED chip having an emission wavelength of 4 〇〇 nm was bonded by silver paste, and a bonding wire (copper wire) was connected to 321 346 177 201004993 to immerse the lead frame. (12) Take off the gun in a vacuum. . (: 5 hours, 隹, at 90 (: Η, hour, and further operation at 110. (13) Also, as the outer drawer resin, add /4R to the mass of 53·2. /° BiS_A ring The gas promoter and 6% by mass of the hardener and 6% by mass of the hardener, the bismuth &amp; agitating, degassing under vacuum, and injecting it into the mold to p-r hard C for 1 hour, Further, it was treated at 150 ° C for 6 hours to obtain a shot type led. The evaluation results are shown in Table 16 and the results of the above [luminescence test] were carried out, and the LED of Comparative Example 20 as a reference was It AA . ^ The light of the color of the horse, the LED of Example 42 is white light' is judged to be qualified. As a result of the above [confidence test (1) (L test)], the lowest value of the full LED is the total beam maintenance rate ( % )=9 4 % 2 9 0 % , judged to be qualified. Secondly, 'the above-mentioned [confidence test (2) (TS test)] is carried out, and after the implementation of 100: under-cycle thermal shock, all The LEDs are all lit and judged to be qualified. In addition, the result of the above [credibility test (3) (TC test)] is performed at a temperature of 100 cycles. After the cycle, all of the LEDs were lit and judged to be acceptable. From the above results, the fluorescent resin composition of Example 42 was subjected to a dispersion stability test, a light resistance test, a luminosity test, and a reliability test ( 1) to (3) are all acceptable, and the overall judgment is acceptable. [Example 43] 32] 346 178 201004993 The resin composition of Synthesis Example 6 was replaced with the resin composition of Synthesis Example 7 and Example 41 was 3), (12) The curing treatment temperature was changed to 110 ° C for 4 hours, and further 150 ° C for 1 hour, and the same procedure as in Example 40 was carried out to prepare a resin composition, a cured product, and a firefly according to Tables 13 to 15'. The photoreceptor composition and the LED were evaluated in Table μ. The index of the light resistance test YI=6.8S13, and it was judged that the light resistance was acceptable. Further, the fluorescent resin composition after storage at 25 ° C for 5 hours There is no precipitation, and the phosphor is uniformly dispersed, so it is judged that the dispersion stability is acceptable. Next, the result of the [luminescence test] of the LED is white light emission, and it is judged as pass. Further [confirmation test (1) (L test)] results, full led The lowest value is the total beam maintenance ratio (%) = 95% 290%, and it is judged as pass. Next, the result of the above [confidence test (2) (TS test)] is performed, after performing 100 cycles of thermal shock All the LEDs are lit, and the judgment is qualified. Then, the above-mentioned [confidence test (3) (TC test)] is carried out, after performing the 100-cycle temperature cycle, all the LEDs are From the above results, it was found that the fluorescent resin composition of Example 43 is a dispersion stability test, a light resistance test, a luminosity test, and a credibility test (1) to (3). All are qualified, so the comprehensive judgment is qualified. [Example 44] In 60% by mass of the resin composition of Synthesis Example 7, 4 G% by mass of phosphor B was blended in the same manner as in Example 42 179 321 346 201004993 to prepare a fluorescent resin composition'. Flat estimate. The fluorescent resin composition of Example 44 was subjected to dispersion stability, and it was judged to be acceptable when the test was carried out without saying that it was a uniform sentence. Therefore, the fluorescent resin composition was mixed with the reaction diluent and the polymerization initiator at the ratio shown in Table 17, and defoamed under vacuum, and further in the following steps in the working gas, the temperature was 23 ° C, and the humidity was 55. Under the conditions of Shan, a light-storing material (coating film) is produced. ❹ (1) The size of the slide glass (slideGlass) was prepared, and the surface was wiped with ethanol (99.5%, manufactured by Wako Pure Chemical Industries, Ltd.) and allowed to dry. (2) The above fluorescent resin composition was applied onto the carrier glass using a bar coater (#3). (3) The above-mentioned carrier glass was cured at 14 〇t: for 1 minute to form a coating film. In the luminosity test of the above-mentioned light-storing material (coating film), the residual light time was measured by the above method to be 600 minutes or longer, and it was judged to be acceptable. From the above, it was found that the dispersion resin composition of Example 44 had passed the dispersion stability test and the luminescence test, and was judged to be acceptable. This result is shown in Table 18. [Reference Example] The resin composition of Synthesis Example 6 was used in place of the fluorescent resin of Example 42, and the product was produced in accordance with Tables 13 to 15, and the results of the evaluation are shown in Table 16. . The light resistance test index YI=7. 5^13, and the light resistance was judged to be acceptable. Next, as a result of performing the [luminescence test] of the LED, the blue light was 180 321346 201004993, and it was judged that the luminosity was unacceptable.

Further, as a result of the [confidence test (1) (L test)], the lowest value of all the LEDs was 90% of the total beam maintenance ratio (%) = 95%, and it was judged as pass. Next, the results of the above-mentioned [confidence test (2) (TS test)] were carried out, and after the thermal shock of 100 cycles was performed, all of the LEDs were turned on, and it was judged as pass. Then, as a result of the above-mentioned [confidence test (3) (TC test)], all of the LEDs were turned on after the temperature cycle of 100 cycles, and it was judged as pass. [Comparative Example 20] A resin composition of Synthesis Example 6 was replaced with an alicyclic epoxy resin to prepare a fluorescent resin composition, and the results of the evaluation are shown in the table. The fluorescent resin composition of Comparative Example 20 was stored at 25 Torr for 5 hours, and the phosphor was precipitated to be uneven, and the dispersion stability was judged to be unacceptable. Therefore, since the normal fluorescent resin composition could not be produced, the comprehensive evaluation of the cured product and the LED was not acceptable. [Comparative Example 21] A resin composition, a cured product, a fluorescent resin composition, and the like were prepared in the same manner as in Example 42 except that the resin composition of Synthesis Example 6 was replaced with a Bi sA epoxy resin. LEDs, the results of the evaluation are shown in Table 16. The indicator of the photometric test γ Ι = 17.2 &gt; 13, and it was judged that the light resistance was unacceptable. ° Further, the fluorescent resin composition after 5 hours of storage at 25 C was not immersed in 321346 181 201004993, and the phosphor was uniformly dispersed, and the dispersion stability was judged to be acceptable. Next, as a result of performing the [luminescence test] of the LED, it was white light emission, and it was judged as pass. Further, as a result of the [confidence test (1) (L test)], the lowest value of all the LEDs was the total beam maintenance ratio (%) = 97% ^ 9 %, which was judged to be acceptable. Next, the results of the above-mentioned [confidence test (2) (TS test)] were carried out, and after 100 cycles of thermal shock, all the LEDs were turned on, and it was judged to be acceptable.继 Then, as a result of the above-mentioned [confidence test (3) (TC test)], after the temperature cycle of 100 cycles was performed, all of the LEI) were lit and judged as pass. From the above results, the fluorescent resin composition of Comparative Example 21 was qualified in the dispersion stability test, the luminosity test, and the reliability test (1) to (3), but the light resistance was poor, so the overall judgment was Not qualified. [Comparative Example 22] 树脂 The resin composition of Synthesis Example 6 was replaced with a polyfluorene oxide resin by mixing and stirring the liquid A and the liquid B at a mass ratio of 1:1. A resin composition was produced in the same manner as in Example 42 except that the curing temperature of the cured product of the cured product and the LED was changed to 7 (TC 1 hour, and further 150 ° C for 5 hours). The cured product, the fluorescent resin composition, and the LED were evaluated in Table 16. The light resistance test index ΥΙ=2·0^13, and the light resistance was judged to be acceptable. Next, the LED [luminescence test] was performed. As a result, the white light emission was judged as pass. 182 321346 201004993 The result of the above [confidence test (1) (L test)] was performed. 'Three of the 10 LEDs were not lit, and the full beam could not be measured. The maintenance rate (%) was judged to be unsatisfactory. _ Next, the result of the above [confidence test (2) (TS test)] was performed, and after performing 100 cycles of thermal shock, 'only 4 out of 10 LEDs. When the lighting is judged to be unacceptable, the result of the above [confidence test (3) (TC test)] is performed, and after the temperature cycle of one cycle is performed, only 10 of the 10 LEDs are used. Six of them were lit and judged to be unacceptable. From the above results, the fluorescence of Comparative Example 22 was known. Although the resin composition test was satisfactory in the dispersion stability test, the light resistance test, and the luminosity test, the results of the reliability tests (1) to (3) were unacceptable, so the overall judgment was: Grid. ", ° [Comparative Example 23] A fluorescent resin composition and a light-storing material were produced in the same manner as in Example 44 except that the alicyclic epoxy resin was used instead of the resin composition 合. (Coating film), the dispersion test and the luminescence test were carried out. The results are shown in Table 18. In the case of the comparative example 23, the optical resin shattering was caused to be uneven and was judged to be unacceptable. In the luminosity test of the material (coating film), the above method measures the residual light % for 6 〇〇 minutes or more, and it is judged to be acceptable. The luminescent fruit shows that the composition of the glory tree of Comparative Example 23 is The test was a stone grid, but the dispersion stability was unsatisfactory, so it was judged to be 321346 183 201004993. The results of Tables 13 to 18 show that the fluorescent resin compositions of Examples 42 and 43 have excellent dispersion stability. Light resistance of the cured product Further, 'the LED system using the fluorescent resin compositions of Examples 42 and 43 as the sealing material was excellent in the luminosity test, and was also excellent in the reliability test. Further, the fluorescing property of Example 44 The resin composition was excellent in dispersion stability. The light-storing material was excellent in luminosity test. On the other hand, the fluorescent resin compositions of Comparative Examples 20 and 23 were poor in dispersion stability. Further, light resistance when a cured product was produced At least one of the luminescence test and the flammability test of the LED used as the sealing material is defective. The above shows that the fluorescent resin composition of the present embodiment is excellent in dispersion stability. The sealing material made of the fluorescent resin composition is excellent in reliability. The light-storing material is excellent in luminescence. Table 13 Unit: mass % Composition ratio Bis-A epoxy resin alicyclic. Epoxy resin alkoxy decane compound THF Hydrolysis condensation catalyst DBTDL Polyoxyl resin GPTMS PTMS DMDMS TEOS Example 42 (Synthesis Example 6) 27.7 — 24. 8 12. 5 2. 7 1.2 20 10. 6 0.5 Example 43 (Synthesis Example 7) 47. 1 17. 4 8. 6 3. 6 0. 0 14. 9 8. 0 0. 3 — Reference Example (Synthesis Example 6) 27.7 - 24.8 12. 5 2.7 1.2 20 10. 6 0.5 A Comparative Example 20 100. 〇一一一一—— _ Η A Comparative Example 2] 100. 〇----一—一— — 一———一__ A comparative example 22 One-one-one-one-100. 0 321346 184 201004993 Table 14

Table 15 0 Composition ratio luminescent resin composition Resin composition Example 42 (Synthesis Example 6) 60. 4 Example 43 (Synthesis Example 7) 60. 1 Reference Example (Synthesis Example 6) - 58.3 Comparative Example 20 - Comparative Example 21 a comparative example 22 a Bis-A epoxy resin

Unit: mass X alicyclic epoxy resin polyoxyn resin hardening 剤 hardening promotion 剤 39. 7 41. 5 53. 2 46. 5 100. 185 321346 201004993 ΐέ ^κ·:χ -1 &quot; ΟΛ^^ν 91 &lt;Qο 13⁄4 〇〇XXXX i credibility amm 〇〇〇1 〇X slave after the soil shines earned \ 9 9 〇〇 \ *6&quot; single mold 〇 〇 〇» t 10锢 / 10 6 / 10 t (2) lSim 〇〇〇i 〇X lighting number \ ^ 9 single S 2 霣隳Ο 〇 \ *6&quot; Single Ξ S 1 10佃 / 10 锢 4 / 10镧中(1)L冢冢' 〇0 〇1 〇X ·« «-4! $ S? ^ * 1 Unable to measure illuminance micro X 1 〇〇«} • Φ *) • ffi 簸 (base) 1 « 0 «S3 Lightfastness 〇0 〇1 X Ο m 卜' 00 CD ITS _ _ 17.2 s 鳌 街 街 组成 组成 组成 组成 〇 〇 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 均匀 均匀 均匀 均匀 均匀 均匀 均匀Rogue) Evenly split (no ship) Uneven (with sinking) 1 t _ shouting system 触0 〇f ί 1 Finger 搮0 cs&gt; — CC 1 1 1 Viscosity (Pa-s) IS 〇〇〇 Starting viscosity 〇〇13.8 CO O m (g/ Eq) CM S 1 1 t ift phase combination k&gt; 1.07 1 1.07 1 1 1 &lt;〇,0.0018 1 1- :0.0013 0.0018 ! I 1 0.69 1.59 0.69 1 1 ! ^ 1 Ξ 1 0.26 1_ 0. Η 1 1 1 « 0.59Θ6 0.5914 0.5996 I 1 Results refers to 檩 % % 1 C α52 〜 eS2 α51 ～ e51 1 f 1 tmw 峨 Example 4 (Synthesis Example 6) Example 43 (Synthesis Example 7) Example (Synthesis m) Comparative Example 20 Comparative Example 21 Comparative Example 22 186 321346 201004993 Table 17 Unit: % by mass Composition ratio Fluorescent resin composition Reaction diluent Polymerization initiator Example 44 (Synthesis Example 7) 80. 0 16. 0 4. 0 Comparative Example 23 80. 0 16. 0 4. 0

187 321346 201004993 ο ο 001&lt; 'Tour Φ: 〇&lt; to ## gt; Comprehensive judgment 1 〇X Luminescence test of light-storing material 〇〇 Remnant time (fine 600 or more 600 or more fluorescent resin composition record stability determination 〇X Uniform dispersion (no fine unevenness (with fine resin reduction and preservation stability) 1 finger 1 1.72 viscous (Pa · s) preservation viscosity 〇 initial viscosity 〇〇 CO WPE (g/eq) 1 mixed index 40 1.07 1 £〇0.0013 1 1.59 1 0.26 1 0.5914 1 Evaluation result index number i_α53 ～ε53 | Example / Example Example 44 (Synthesis Example 7) Comparative Example 23 188 321346 201004993 Its-person's change in this embodiment An insulating resin composition in which an insulating property is added to the resin composition is specifically described by way of examples and comparative examples. The evaluation of the physical properties in Examples 45 to 48 and Comparative Examples 24 to 25 was carried out as follows. For the morning oxygen equivalent (WPE), viscosity, mixing index α to ??, according to the same method as above. 平均H oxygen cut average particle size measurement> Using laser diffraction particle size distribution measurement The apparatus ([HEL0S system] manufactured by SYMPATEC Co., Ltd.) measures the average particle diameter in a dry mode. <Measurement of viscosity of resin composition> The container in which the composition immediately after the production is placed is sealed at 25 (: 1) After adjusting the temperature for an hour, the viscosity at 25 ° C was measured. When the viscosity was 1 〇〇〇pa · s or less, it was judged to have fluidity. &lt;Measurement of volume resistivity of the insulating resin composition &gt; Ο On the slide The insulating resin composition was applied to a thickness of 40/zm by a bar coater on a glass, and heated at 2 Torr (TC for 6 minutes to form a coating film. Using a resistivity meter (Dia Instruments Co., Ltd., "Loresta") When the volume resistivity is 1χ1〇ι«·Ω·cm or more, the insulation property is judged to be good. &lt;Measurement of adhesion strength and adhesion of insulating resin composition&gt; Step 'Measure the adhesion strength before and after the moisture absorption treatment. (1) Apply an insulating resin composition to the die pad portion (9 mm x 9 mm) of the copper lead frame. 189 321346 201004993 (2) Next, the silicon wafer (8mmxl6mm) mounted on the die pad, 2〇 °C X1 hour heating in an oven (sample before moisture absorption treatment) (3) The sample prepared in (2) is hygroscopic for 72 hours in a constant temperature and humidity machine set to a temperature of 85 ° C 'humidity 85%> (sample after moisture absorption treatment). (4) The above [pre-moisture-preventing sample] and [moisture-absorbing sample] are heated on a hot plate of 250X: for 2 seconds in a state where the stone substrate is placed below, and the lead frame is pulled up. The wire was measured using a push-pull gauge (manufactured by IMADA Co., Ltd.) to measure the adhesion strength when the chip and the die pad were peeled off. (5) When the residual strength residual ratio represented by the following formula is 8〇% or more, it is determined that the adhesion is good. Then, the residual rate of strength (%M after the moisture absorbing treatment) / (the strength after the moisture absorbing treatment) xl 〇〇 ' &lt; void evaluation of the insulating resin composition > The above-mentioned crystal grains in the copper lead frame The lining portion was coated with an insulating resin to form a crucible, and a glass wafer (8 mm x 8 nini) was mounted and heated in an oven at 2 Torr {rCx i hours. Visually confirm the presence or absence of voids in the sample under a magnifying glass. In the insulating resin composition of the examples and the comparative examples, when the insulating properties and the adhesion were good, and it was confirmed that no voids were formed, the overall judgment was qualified. The raw materials used in the examples and comparative examples are shown in the following (1) to (10). (1) Epoxy Resin (Bu 1) Epoxy Resin A: Bisphenol A type epoxy resin (hereinafter, referred to as 321346 390 201004993

Bis-A epoxy resin) • Trade name: manufactured by Asahi Kasei Epoxy Co., Ltd., “AER” The epoxy equivalent (WPE) and viscosity measured by the above method are as follows. • Epoxy equivalent (WPE): 187 g/eq • Viscosity (25 ° C): 14. 3 Pa · s (1-2) Epoxy resin F: Bisphenol F type epoxy resin (hereinafter, referred to as "Bis- F epoxy resin)) • Trade name: manufactured by Nippon Epoxy Resin Co., Ltd., "jER807" The epoxy equivalent (WPE) and viscosity measured by the above method are as follows. • Epoxy equivalent (WPE): 169 g/eq • Viscosity (25 ° C): 3. 2 Pa · s (2) Alkoxydecane compound Η : 3-glycidoxypropyltrimethoxy decane ( Hereinafter referred to as GPTMS) Q • Trade name: Shin-Etsu Chemical Co., Ltd., “ΚΒΜ-403” (3) Alkoxydecane compound I: Phenyltrimethoxy decane (hereinafter referred to as PTMS) • Trade name · Shin-Etsu Chemical Co., Ltd., "ΚΒΜ-103" (4) Alkoxydecane compound J: dimethyldimethoxy decane (hereinafter referred to as DMDMS) • Trade name: Shin-Etsu Chemical Co., Ltd. Company system, "ΚΒΜ-22" (5) Alkoxy decane compound Κ : Tetraethoxy decane (hereinafter referred to as TEOS) • Trade name · Shin-Etsu Chemical Co., Ltd., "ΚΒΕ-04" 191 321346 201004993 (6) Solvent (6-1) Tetrahydrofuran: Manufactured by Wako Pure Chemical Industries Co., Ltd., without stabilizer (hereinafter referred to as THF) (7) Hydrolyzed Condensation Catalyst: Dibutyltin dilaurate (Wako Pure Chemical Industries, Ltd.) Shares) Company system, hereinafter referred to as dbtdl) (8) Hardener: dicyandiamide (Maruzen Pharmaceutical Industry Co., Ltd.) (9) · cre cre cre 缩 缩 cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre cre s) (10) Insulating powder (1〇1) melted cerium oxide (manufactured by Toshinagawa Kasei Co., Ltd., average particle size 6. ΙβΜ) (1〇_2) Hydrophobic sulphur dioxide eve (Australian chemical WACKER Silic 「ne (share) company's 'H18') (Synthesis Example 8) ◎ 丨 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 (1) Preparation: : The circulating constant temperature water was again mixed and placed on a magnetic stirrer. (2) According to the composition ratio of Table 19, the mixture was stirred and mixed with the alkoxydecane compound, and further stirred and stirred. The increase was set to 5 ° C to return to the cooling tube. Set 80t oil bath. In a 25 C environment, epoxy resin and THF were added to the flask to which the stirrer was placed, and water and hydrolysis condensation catalyst were further added. (3) Secondly, a cold tube was installed in the flask and rapidly immersed in the 801. In the oil bath 321346 192 201004993, stirring was started, and the reaction was carried out for 10 hours while refluxing. (4) After the completion of the reaction, 'cooled to 25 ° C' and then the cooling tube was removed from the flask, and after the refluxing step was completed, the sample solution was taken. (5) The solution after the completion of the refluxing step was distilled off at 400 Pa and 50 ° C for 1 hour using an evaporator, and further distilled at 80 ° C for 5 hours to carry out a dehydration condensation reaction. (6) After completion of the reaction, the mixture was cooled to 25 ° C to obtain a resin composition F. (7) The mixing index α 54 to ε 54 of this resin composition is shown in Table 21. (8) Further, the epoxy equivalent (WPE) of the resin composition F obtained in the above (6) was measured by the above method. The epoxy resin equivalent (WPE) of the above resin composition = 195 g/eq, showing an appropriate value. Also, the viscosity is 12·7 Pa · s, which is a liquid with fluidity. (Synthesis Example 9) Resin composition G: According to the composition ratio of Table 19, the resin composition G was synthesized and evaluated in the same manner as in Synthesis Example 8. The mixing index Ο α55 to ε 55 is shown in Table 21. The epoxy equivalent (WPE) of the above resin composition = 228 g/eq, showing a suitable value. Further, the viscosity is 13.8 Pa · s, which is a liquid having fluidity. (Synthesis Example 1) The resin composition H was evaluated according to the composition ratio of Table 19 in the same manner as in Synthesis Example 8 'synthetic resin composition Η '. The mixing index α 56 to ε 56 is shown in Table 21. ^ The epoxy resin equivalent (WPE) of the above resin composition = 206 g / eq, which shows a suitable viscosity and a viscosity of 18.2 P a · s ' is a liquid having fluidity. 193 321346 201004993 (Synthesis Example 11) Resin composition I: According to the composition ratio of Table 19, the resin composition I was synthesized in the same manner as in Synthesis Example 8 and evaluated. The mixing index α 57 to £ 57 is shown in Table 21. The epoxy equivalent (WPE) of the above resin composition = 208 g/eq, showing an appropriate value. Further, the viscosity is 10·2 Pa·s, which is a liquid having fluidity. (Example 45) 0 The insulating resin composition 1 was produced by the following procedure and evaluated. The evaluation results and the mixing indexes α 54 to e 54 are shown in Table 21. Using the resin composition f of the above-mentioned Synthesis Example 8, the raw materials were blended according to the composition of Table 20, and uniformly kneaded by a three-roll mill (manufactured by Inoue Co., Ltd.). Further, it was defoamed at 400 Pa for 30 minutes using a vacuum chamber, and this was regarded as the insulating composition 1. The insulating resin composition 1 was applied to a carrier glass by a bar coater to a thickness of 40/zm, and heated at 20 (rc for 6 minutes to form a coating film. With a ❹ resistivity meter (DiaInstru deleted ts ( The company's system, "seven (four) gamma" measures the volume resistivity of this coating film. When the volume resistivity is ΐχΐ〇1 () Ω • (10) or more, 'the insulation is judged to be good. The insulating resin composition is followed by The strength residual ratio was obtained by the following procedure: (1) Four insulating resin compositions were applied to the die pad portion (9 mjnx9 inm) of the copper lead frame. (2) Next, the germanium wafer (8 mm x 16 inm) Mounted in the die pad portion and heated in an oven at 200 C for 1 hour. 321346 194 201004993 (3) In the sample prepared in (2), two were used as "pre-hygroscopic treatment samples". 4) The remaining two pieces of the matte made in (2) are set in the machine with the temperature resistance and humidity of 85% for 72 hours, and these are used as the "sample after moisture absorption treatment". (5) Using the above "sucking "Pre-wet treatment sample" and "moisture-receiving sample", so that the crucible wafer is hung below - on the 25 (rc hot plate for 2 seconds, Pull the lead wire of the lead frame and use a push-pull meter (manufactured by Seiko Co., Ltd.) to measure the adhesion strength of the tantalum wafer and the die pad. The measurement was performed at n = 2 11 to obtain an average value. (6) The average value of the subsequent strengths of the "pre-hygroscopic treatment sample" and the "moisture-absorbing sample" obtained above was substituted into the following equation to determine the residual strength residual ratio, and the adhesion was evaluated. Residual rate (% 接着 adhesion strength after moisture absorption treatment) / (adhesion strength before moisture absorption treatment) χ 100 = 95% 280%, and the adhesion property of the insulating resin composition 1 was judged to be good. ❹ Secondly, in the copper lead frame The die pad portion was coated with an insulating resin composition 1 'Women's glass wafer (8 mm x 8 mm), and heated in an oven for 2 ° C for 1 hour. Under the magnifying glass, it was visually confirmed that the sample did not generate voids. Insulating resin composition 1 was excellent in insulation and adhesion, and did not cause voids. Therefore, it was judged to be acceptable by comprehensive judgment. (Example 46) The composition of the composition of Table 20 was used, and the resin composition g described above was used. 45 the same method to make insulation The lipid composition 2 was evaluated and evaluated. The evaluation results and the mixing index α 55 to ε 55 are shown in Table 21. 195 321346 201004993 The volume resistivity of the insulating resin composition 2 is lxl 〇 1 () Q · (10) or more The insulation property is determined to be good. The average value of the adhesion strength between the "pre-hygroscopic treatment sample" and the "moisture absorption-treated sample" of the insulating resin composition 2 is substituted into the following equation to obtain the residual strength residual ratio. Next, the strength residual ratio (%) = (the strength after the moisture absorption treatment) / (the adhesion strength before the moisture absorption treatment) x l 〇〇 = 92% 280%, and the adhesion of the insulating resin composition 2 It was judged to be good. 〇 ^ ^ Eight-person' was coated with an insulating resin composition 2' on the die pad portion of the copper lead frame to mount a glass wafer (8 mm x 8_), and heated in an oven for 2 〇〇〇 C x 1 hour. It was visually confirmed under a magnifying glass that no void was generated in this sample. As a result of the above, it was found that the insulating resin composition 2 was excellent in insulation and adhesion, and no void was formed. (Example 47) The insulating resin composition 3 was produced and evaluated in the same manner as in Example 45, except that the resin composition of the above-mentioned composition was used. The results of the evaluation and the mixing index are shown in the table. The volume resistivity of the insulating resin composition 3 is judged to be good at 1 χ 101 (ιΩ · cm or more. The insulating resin composition 3 is used. The average value of the subsequent strengths of the "sample before moisture absorption treatment" and the "sample after moisture absorption treatment" was substituted into the following equation, and the residual strength ratio was evaluated to evaluate the adhesion. Then, the residual ratio of strength (%) = (hygroscopicity) The strength after the treatment) / (the strength before the moisture absorption treatment) x l 〇〇 = 89% 280%, the insulating resin composition 321 346 196 201004993 The adhesion of the material 3 was judged to be good. Second, the grain in the copper lead frame The insulating resin composition 3 was applied to the pad portion, and a glass wafer (8 mm x 8 inm) was attached and heated in an oven at 200 ° C for 1 hour. Under the magnifying glass, it was visually confirmed that the sample did not generate voids. From the above results, it was found that the insulating resin was composed. The material 3 was excellent in insulation and adhesion and did not cause voids. Therefore, it was judged to be acceptable by comprehensive evaluation. (Example 48) The resin composition I described above was used according to the composition of Table 20, and the same method as in Example 43 was carried out. The insulating resin composition 4 was produced and evaluated. The evaluation results and the mixing index α 57 to ε 57 are shown in Table 21. The volume resistivity of the insulating resin composition 4 was 1 χ 1 〇 1 () Ω · cm or more. The insulation property is determined to be good. The average value of the adhesion strength between the "pre-hygroscopic treatment sample" and the "moisture-absorbing sample" of the insulating resin composition 4 is substituted into the following equation to determine the residual strength residual ratio. Evaluation of adhesion. 0 Next, the residual rate of strength (%) = (the strength after the moisture absorption treatment) / (the strength after the moisture absorption treatment) x l 〇〇 = 86% 28% by weight, followed by the insulating resin composition 4 The determination was good. Secondly, a glass wafer (8 mm x 8 mni) was attached to the die pad portion of the copper lead frame by applying an insulating resin composition 4', and heated in an oven at 200 ° C for 1 hour. The sample was visually confirmed under a magnifying glass. As a result of the above, it was found that the insulating resin composition 4 was excellent in insulation and adhesion, and did not generate voids, so it was judged to be acceptable by comprehensive judgment. (Comparative Example 24) 197 321346 201004993 According to the composition of Table 20, use Bis_A epoxy tree The insulating resin composition 5 was produced in the same manner as in Example 45, and was evaluated in the same manner as in Example 45. The results are shown in the table. The volume resistivity of the insulating resin composition 5 is (10) or more. 'The insulation is good. The average value of the adhesion strength of the sample before moisture absorption treatment and the sample after moisture absorption treatment of the insulating resin composition 5 is substituted into the following formula to obtain the residual strength of the adhesive strength. , evaluate the adhesion. $ &quot; 着 $strength of the residual rate (%) = (the strength after the moisture absorption treatment) / (the strength before the moisture absorption treatment) x l 〇 G = 63% &lt; 8Q%, insulation The adhesion determination of the fat composition 5 is poor. Next, the insulating resin composition 5 was coated on the die lining of the copper lead frame, and a glass wafer (8 mm x 8 mm) was mounted and heated in an oven for 2 hours. It was visually confirmed under a magnifying glass that no void was generated in this sample. From the above results, it is understood that the insulating resin composition 5 is

Well, there is no void, but because of poor adhesion, the synthesis is not qualified. (Comparative Example 25) According to the composition of Table 20, Bis-A epoxy oxime was used -

The insulating resin composition 6 was produced and evaluated in the same manner as in Example 43 except that the resin composition F was replaced with GPMS, GPMS, and PTMS. The results are shown in Table 21. The volume resistivity of the insulating resin composition 6 was 1 χ 1 〇 1 () Ω · (10) or more, and it was judged that the insulation property was good. The average strength of the subsequent strength of the "pre-hygroscopic treatment sample" of the insulating resin composition 6 and the "sample after wet treatment of 321346 198 201004993" was determined, and the adhesive strength residual ratio was determined to evaluate the adhesion. Then, the strength residual ratio (%) = (the strength after the moisture absorption treatment) / (the degree before the moisture absorption treatment), x (10) = 89%, and the adhesion of the impurity-free resin composition 6 was judged to be good. Next, 'insulating resin composition 6' women's glass wafer (8 mm x 8 mm) was applied to the die pad portion of the copper lead frame, and heated by an oven for 20 (TC x 1 hour). This sample was visually confirmed to have voids under a magnifying glass. As a result of the above, the insulating resin composition 6 was excellent in insulation property and adhesion, but it was confirmed that voids were formed, and it was judged that it was not combined. As shown in Tables 19 to 21, the epoxy resin was contained. The insulating resin composition of the resin composition, the insulating powder, and the curing agent which are obtained by mixing and hydrolyzing a specific alkoxydecane compound in a specific ratio is excellent in insulation and adhesion, and does not occur. Table 19 Unit: mass % Composition ratio Bis-A epoxy resin Bis-F epoxy resin alkoxy decane compound ΤΗΓ Water hydrolysis condensation catalyst GPTMS PTMS DMDMS TE0S DBTDL Synthesis Example 8 37.5 — 31. 6 3. 1 0· 9 a 17.9 8. 5 0. 40 Synthesis Example 9 43. 5 — 10. 2 14. 3 3. 5 — 20.4 7. 8 0. 36 Synthesis Example 10 48. 0 6. 9 11.8 5. 9 2· 5 0.3 18.9 5.4 ......– — 0. 32 Synthesis Example 1 | 72. 4 — 1.8 6. 0 4. 6 a 10.8 4. 1 0. 24 199 321346 201004993 Table 20 Unit: mass%

Composition Bifeng resin composition Bi sA Epoxy resin Bis-F Epoxy resin hardening 剤GPTMS PTMS Diluent molten cerium oxide hydrophobic bismuth bismuth Hydroxide Example 45 Resin composition F 53. 8 - 6. 0 2_ 0 - A 18.2 15. 0 5. 0 Example 46 Resin-composition G 51.0 - 6. 0 2. 0 - - 20. 0 13. 0 5. 0 Example 47 Resin composition Η 59. 8 - - 2 0 — - 18. 2 15. 0 5. 0 Example 48 Resin Composition I 51.8 - 8. 0 2. 0 - - 18. 2 15. 0 5. 0 Comparative Example 24 A 53. 8 6. 0 2 0 - 18.2 15. 0 5. 0 Comparative Example 25 - 45. 8 6. 0 2. 0 4. 0 4. 0 18. 2 15. 0 5. 0 200 321346 201004993

Iz&lt; .· X ^ $ .. OAW^V Comprehensive judgment ί_ 〇〇〇〇 XX scale earning fat composition a 1 Judging 1___ 〇〇〇〇〇X Then strength residual ratio (%) 1 〇〇〇〇X 〇 Remaining Rate SS Short-term resistivity (Ω · cm) Determine the resistivity of 〇〇〇〇〇〇Zhao product xlOw or more • Μ S xlO1. Above xlOw or more - Μ 〇 xlOw above resin composition mixing index CNI 〇 1.05 1.20 1 1 0.0014 0.0014 0.0017 0.002 1 1 1.05 1.56 2.67 5.82 1 1 0.05 0.25 0.25 1.00 1 1 0.1177 1.6666 0.5914 4.0000 1 1 Evaluation result index number α54~ Ε54 α55 to e55 cr56 to e56 α57 to ε57 1 1 Embodiment, Comparative Example 45 Example 46 Example 47 Example 48 Comparative Example 24 Comparative Example 25 20 321346 201004993 Semi-guided 有关 2 The composition of the resin composition is specifically described by way of examples and comparative examples. The evaluation of the physical properties in only the domains 49 to 58 and the comparative examples 26 to 3 was carried out as follows. (10)), viscosity, mixed finger - the same as the above = storage stability index Θ calculation, and resin 纟 reduction of the preservation of the stability of the resin composition of the line of deposits, the wire according to the following - the preservation and stability Sex indicators Θ assessment. () Preservation stability index θ = (preservation viscosity) / (The initial viscosity will be placed in the container of the resin composition immediately after manufacture: after adjusting the temperature for 2 hours, measure the viscosity in the scratch, and start from ^5 The initial viscosity". 啊一田作❹. Also, put the resin composition in a container and seal it, then store it in the 温C strange incubator for 2 weeks. After storage, measure it as a q in the stick. Viscosity. τ viscosity, when the resin composition has fluidity (viscosity is 1 〇〇〇Pa·s or less and the storage stability index is 0 or less, it is judged to have preservation stability and &lt; LED (hardened material) (Light resistance test) It is difficult to cut the sample after the LED is manufactured. Therefore, the cured product is obtained by the following method, and the evaluation result is substituted for the light resistance evaluation of the LED. (1) Hardening prepared by the method described later. The material is hardened with a solution to make a cured product of 20 mm x 10 mm x 3 mm thick. 321346 202 201004993 (2) The hardened material is covered with a black mask having a diameter of 5 5 mm and a thickness of 1.5 mm π χ 15 mm x 1.2 mm as a light-resistant property. Test sample. (3) Preparation device The UV light was irradiated from the UV irradiation device ("Spot Cure SP7-250DB" manufactured by Ushio Electric Co., Ltd.) to the above-mentioned sample in an incubator set to a constant temperature of 50 ° C via an optical fiber. In the state where the black mask is placed on the top, it is placed in an incubator at a constant temperature of 50 ° C. (5) In such a manner that the UV light is irradiated to the hole having a diameter of 5. 5 mm from the upper portion of the black mask, The UV light of 2 W/cm 2 was irradiated for 96 hours. (6) The uv irradiation test was carried out by using a spectrophotometer ("SD5000" manufactured by Sakamoto Electric Co., Ltd.) which has been modified into a diameter of 10 mm. (7) Yellowness (YI) is determined according to "ASTM D1925-70 (1988): Test Method for Yellowness Index of Plastics,&gt;." When this YI is 13 or less, it is judged as pass. Credibility test (1) (continuous action test: hereinafter referred to as [l test]) &gt; 10 LEDs, according to "MIL-STD-750E (Test Method for Semiconductor Devices)" METHOD 1026. 5 (steady state) Operating life) and "MIL-STD-883G (microcircuit)" METHOD 1005.8 (steady state life), using the following conditions Estimate with a forward current (IF) = 20 mA, ambient temperature (TA) = 25 t:, 960 hours, and measure the full beam (LM) before and after lighting. Also, ask 203 321346 201004993 for each LED "Total beam maintenance rate (%) = (total beam M0G before the lamp is turned on), and when the lowest value of the total beam maintenance rate (%) of the entire LED is 90% or more, it is judged as pass. &lt;LED reliability test (2) (thermal shock test: hereinafter, abbreviated as [Ts test]) &gt; 10 LEDs, according to [EIAJ ED-4701/30〇 (Solution and Environment Test Method for Semiconductor Devices) (Intensity test 1}) Test method 3〇7 (thermal shock test), evaluated by the following conditions: ❹ [_10 ° C (5 minutes) to 100 ° C (5 minutes)] as the i-cycle, in the implementation After 100 cycles of thermal shock, it is confirmed that the LED is lit, and when all 10 are lit, it is judged as qualified. <LED reliability test (3) (temperature cycle test: hereinafter referred to as [Tc] test) &gt; 10 LEDs were evaluated according to the following test conditions [EIAJ ED-4701/100 (Environmental and Financial Test Method for Semiconductor Devices (Life Test I)) ❹ (Temperature Test). Take [-40 ° C (30 minutes) to 85 ° C (5 minutes) to 1 〇〇. (: (30 minutes) to 25 ° C (5 minutes)] as a cycle, after 10 cycles After the temperature cycle, the number of LEDs of the LEDs is confirmed, and when all of the LEDs are lit, it is judged as pass. In the evaluation of the above LEDs, the light resistance and reliability tests (1) to (3) are combined. In the case of the above, the raw materials used in Examples 49 to 59 and Comparative Examples 26 to 3 were expressed in the following (1) to (12). 321346 204 201004993 (1) Epoxy resin (1-1) ring Oxygen Resin A1: Poly(bisphenol A-2-hydroxypropyl ether) (hereinafter, referred to as "Bis-Al Epoxy Resin") • Product name: Asahi Kasei Epoxy Co., Ltd., "AER2600" The epoxy equivalent (WPE) and viscosity determined by the method are as follows: 0 • Epoxy equivalent (WPE): 188 g/eq • Viscosity (25 ° C): 14. 8 Pa · s 0-2) Epoxy resin A2: Poly(bisphenol A-2-hydroxypropyl ether) (hereinafter, referred to as "Bis-A2 epoxy resin") • Product name: Asahi Kasei Epoxy Co., Ltd., "AER2500" Further, the ring measured by the above method The oxygen equivalent weight (WPE) and viscosity are as follows: • Epoxy equivalent (WPE): 186 g/eq • Viscosity (25t:): 10. 2 Pa · s (1-3) Epoxy resin A3: Poly (bisphenol) A-2-hydroxypropyl ether (hereinafter, abbreviated as "Bis-A3 epoxy resin") • Trade name: manufactured by Asahi Kasei Epoxy Co., Ltd., "AER6071" In addition, the epoxy equivalent (WPE) measured by the above method ) The viscosity is as follows. However, since the epoxy resin A3 is solid at 25 ° C, the viscosity cannot be measured. • Epoxy equivalent (WPE): 470 g/eq (2) Alkoxydecane compound Η : 3-shrinkage Glyceryloxypropyltrimethoxydecane (hereinafter referred to as "GPTMS") 205 321346 201004993 • Trade name: Shin-Etsu Chemical Co., Ltd., "ΚΒΜ-403" (3) Alkoxydecane compound L: 2 -(3,4-epoxycyclohexyl)ethyltrimethoxydecane (hereinafter referred to as "ECETMS") • Trade name: Shin-Etsu Chemical Co., Ltd., "KBM-303" (4) Alkoxydecane Compound I: phenyltrimethoxy decane (hereinafter referred to as "PTMS") • Trade name: Shin-Etsu Chemical Co., Ltd., "KBM-103" (5) Alkoxydecane compound J: trimethyl group曱 矽 矽 ( (hereinafter referred to as "DMDMS") • Trade name: Shin-Etsu Chemical Co., Ltd., "KBM-22" (6) Alkoxy decane compound K: tetraethoxy decane (hereinafter referred to as " TE0S") • Trade name: Shin-Etsu Chemical Co., Ltd., "KBE-04" (7) Solvent (7-1) Tetrahydrofuran: It is manufactured by Wako Pure Chemical Industries Co., Ltd., and does not contain a stabilizer (hereinafter referred to as "THF"). (7-2) Tert-butanol: Wako Pure Chemical Industries Co., Ltd. Stabilizing dosage form (hereinafter referred to as "t-BuOH") (8) Hydrolysis condensation catalyst (8-1) Dibutyltin dilaurate (manufactured by Wako Pure Chemical Industries, Ltd., hereinafter referred to as "DBTDL") (8- 2) Dibutyltin dioxide (manufactured by Sigma-Aldrich Co., Ltd., hereinafter abbreviated as "DBTDM") (9) Hardener: [4-methylhexahydrophthalic anhydride/hexahydrophthalic anhydride = 70/30] 206 321346 201004993

• Product name: New Japan Physicochemical Co., Ltd., "RiKACID MH-700G" (10) Hardening accelerator: Amine compound • Trade name: San-apro (share) company, "u CAT 18χ" (11 Polyoxyl resin • Trade name: manufactured by Toray·Dow Corning Co., Ltd., “EG6301 (A liquid/B liquid)” [Synthesis Example 12] ® The resin composition was produced by the following procedure. (1) Preparation: Set the circulating constant temperature water tank to 5. (:, return to the cooling tube. Further, place a 80 ° C oil bath on the magnetic stirrer. (2) According to the composition ratio shown in Table 22, the above Bis-Al epoxy was used in the environment of 25. The resin 'Oxygen-casting compound was added to the flask to which the stirrer was placed and mixed with thf, and then water and a hydrolysis condensation catalyst were further added and mixed and stirred. Q (3) Secondly, the flask was installed and cooled. The tube was rapidly immersed in an oil bath of 8 (TC) and started to stir while reacting for 20 hours while refluxing (reflow step). (4) After the reaction was completed, it was cooled to 25 ° C. Then, the cooling tube was removed from the flask. (5) The solution after the completion of the refluxing step was subjected to a dehydration condensation reaction (dehydration condensation step) while distilling off at 80 ° C for 50 hours using an evaporator at 400 Pa, 50. (6) After the completion of the dehydration condensation reaction, 'cooling to 25 ° C to obtain a resin composition. 207 321346 201004993 (7) The mixing indexes α 58 to ε 58 of the resin composition are shown in Table 24, respectively. Further, the resin group obtained in the above (6) was measured by the above method The epoxy equivalent of the material (WPE) 'initial viscosity and preservation viscosity. Further, the storage stability index 0 is obtained. It is shown in Table 24. The epoxy equivalent of the resin composition of the above Synthesis Example 12 ( Wpj;) = 230 g / eq, showing the appropriate value. Again, the initial viscosity is 33 7Pa.s &lt; 1 〇〇〇 Pa · s ' and the preservation viscosity = 47 · 0 Pa · s &lt; 1000 Pa · s, two In addition, the storage stability index 0 58 = 1. 39 g 4 , and it is judged that there is a resin composition for preservation stability [Synthesis Example 13] In the same manner as in Synthesis Example 12, 23. A resin composition was produced. The results of evaluation in the same manner as in Synthesis Example 12, the mixing index α 59 to ε 59, and the storage stability index θ 59 are shown in Table 24. As shown in Table 24, the resin of Synthesis Example 13 The composition has an epoxy equivalent weight (WPE) 〇 = 231 § / called, showing an appropriate value. Again, the initial viscosity = 13. 2 Pa · 1000 Pa s, and the preservation viscosity = 19 ! pa · s < pa · $, Both have a fluid liquid. Also, the storage stability index is 0 59=1. 45$4, which is judged to have a stable resin composition. [Synthesis Example 14] A resin composition was produced in the same manner as in Synthesis Example 12 according to Tables 22 and 23. The results of the evaluation in the same manner as in Synthesis Example 12, the mixing index α 60 to ε 60, and the preservation stability were observed. The index θ 6 〇 is shown in Table 24. As shown in Table 24, the epoxy resin of Synthesis Example 14 was *(WPE) 208 321346 201004993 = 242 g/eq, and an appropriate value was shown. Also, the initial viscosity = 145p ? &amp; 4, and the preservation viscosity = 16.2 匕 1 &lt; 1 〇〇〇 ^, rain is a liquid with fluidity. Further, the storage stability index 06 〇 =1 was judged to have a resin composition for preserving stability. [Synthesis Example 15] A resin composition was produced in the same manner as in Synthesis Example 12 in accordance with Tables 22 and 23. The results of the evaluation in the same manner as in Synthesis Example 12, #: α 61 to ε 61, and the storage stability index 061 are shown in Table 匕.曰 曰 ◎ As shown in Table 24, the ring gas equivalent ((iv)) of the resin composition of Synthesis Example 15 = 245 g/eq, which showed an appropriate value. Further, the initial viscosity = 14.8 匕 2 (10) Pa·s, and the storage viscosity = 21.0 Pa·s &lt; 1 〇 (9) d s , both of which are fluid liquids. Further, the storage stability index Θ 61 = 1 was determined, and it was judged that there was a resin composition for preserving stability. [Synthesis Example 16] A resin ruthenium composition was produced in the same manner as in Synthesis Example 12 in accordance with Tables 22 and 23. The results of evaluation in the same manner as in Synthesis Example 12, mixing = α 62 to ε 62, and storage stability index 062 are shown in Table 2: As shown in Table 24, the epoxy equivalent (wpE) = 228 g / eQ' of the resin composition of Synthesis Example 16 showed an appropriate value. Also, the initial viscosity = 44. Two &lt; ι〇(9)

Pa · s, and 'save viscosity = 61. 1 Pa · s &lt; l〇〇〇 pa · s, both are liquids with fluidity. Further, the storage stability index Θ 62 = 1 邡 was determined, and it was judged that there was a resin composition for preserving stability. [Synthesis Example 17] A resin composition was produced according to the same procedure as in Example 12 of 321346 209 201004993 except that the time of the turbulent flow step was set to 7 hours. The results of evaluation in the same manner as in Synthesis Example 12, the mixing index α 63 to ε 63 , and the storage stability index 0 63 are shown in Table 24. As shown in Table 24, the epoxy resin equivalent (WPE) of the resin composition of Synthesis Example 17 was 214 g/eq, which showed an appropriate value. Further, the initial viscosity = 4. 9 Pa · s &lt; 1000 Pa · s, and the storage viscosity = 9. 4 Pa · s &lt; 1000 Pa · s, both of which are fluid liquids. Further, the storage stability index Θ 63=1. 91 S4 was determined to have a resin composition for preserving stability.合成 [Synthesis Example 18] A resin composition was produced in the same manner as in Synthesis Example 12 in accordance with Tables 22 and 23. The results of the evaluation in the same manner as in Synthesis Example 12, the mixing index α 64 to ε 64 , and the storage stability index 0 64 are shown in Table 24. As shown in Table 24, the epoxy equivalent (WPE) of the resin composition of Synthesis Example 18 = 214 g/eq, which showed an appropriate value. Also, the initial viscosity = 15. 9 Pa · s &lt; 1000 ? 3 * 3, and the preservation viscosity = 15.9? 3 * 8 &lt; 1000 ? & * 5, Q Both are fluid liquids. Further, the stability index 0 7 = 1. 21 S4 was stored, and it was judged that there was a resin composition for preserving stability. [Synthesis Example 19] A resin composition was produced in the same manner as in Synthesis Example 12 in accordance with Tables 22 and 23. The results of evaluation in the same manner as in Synthesis Example 12, the mixing index α65 to ε 65, and the storage stability index Θ 65 are shown in Table 24. As shown in Table 24, the epoxy resin equivalent (WPE) of the resin composition of Synthesis Example 19 = 238 g/eq, which showed an appropriate value. Also, the initial viscosity = 18. 9 Pa · s &lt; 1000 ? 3.5, and the preservation viscosity = 28.7? & * 5 &lt; 1000 ? 3 * 5, both 210 321346 201004993 are liquids having fluidity. Further, the storage stability index θ 65=1. 52 S 4 was determined to have a resin composition for preserving stability. [Synthesis Example 20] A resin composition was produced in the same manner as in Synthesis Example 12 in accordance with Tables 22 and 23. The results of evaluation in the same manner as in Synthesis Example 12, the mixing index α66 to ε66, and the storage stability index 066 are shown in Table 24. As shown in Table 24, the epoxy equivalent (WPE) of the resin composition of Synthesis Example 20 = 213 g/eq, which showed an appropriate value. Further, the initial viscosity = 11.2 Pa · s &lt; ® 1000 Pa·s, and the storage viscosity = 16.1 Pa·s &lt; 1000 Pa·s, both of which are fluid liquids. Further, the stability index 0 66=1.44 S 4 was stored, and it was judged that there was a resin composition for preserving stability. [Synthesis Example 21] A resin composition was produced in the same manner as in Synthesis Example 12 in accordance with Tables 22 and 23. The results of the evaluation in the same manner as in Synthesis Example 12, the mixing index 〇: 67 to ε67, and the storage stability index 067 are shown in Table 24. Q As shown in Table 24, the epoxy equivalent (WPE) of the resin composition of Synthesis Example 21 = 253 g/eq, which showed an appropriate value. Further, the initial viscosity = 26.8 Pa·s &lt; 1000 Pa·s, and the storage viscosity = 39.1 Pa·s &lt; 1000 Pa·s, both of which are fluid liquids. Further, the stability index θ 67 = 1.46 S 4 was stored, and it was judged that the resin composition having the stability was stored. [Comparative Synthesis Example 1] A resin composition was produced in the same manner as in Synthesis Example 12 in accordance with Tables 22 and 23. The results of evaluation in the same manner as in Synthesis Example 12, the mixing index α 68 to ε 68, and the storage stability index Θ 68 are shown in Table 24. 211 321346 201004993 As shown in Table 24, the epoxy equivalent (WPE) = 295 g / eq ' of the resin composition of Comparative Synthesis Example 1 was shown to be an appropriate value. Further, the initial viscosity = 33. 4Pa · 5 &lt; 1000 ? & * 5' and the 'preservation viscosity = 48.2? & .5 &lt; 1000 ? 3. s ' are both liquids having fluidity. Further, the storage stability index 0 68 = 1. 44S4 ' was determined to have a resin composition for preserving stability. [Comparative Synthesis Example 2] A resin composition was produced in the same manner as in Synthesis Example 12 in accordance with Tables 22 and 23. The results of evaluation in the same manner as in Synthesis Example 12, the mixing index α 69 to ε 69, and the storage stability index 0 69 are shown in Table 24. As shown in Table 24, the epoxy equivalent (WPE) of the resin composition of Comparative Example 2 was compared to 295 g/eq, and an appropriate value was shown. Further, the initial viscosity = 29. 〇pa · s &lt; 1000 Pa·s, which is a fluid liquid, but the storage viscosity &gt; 1 〇〇〇 Pa · s is no fluidity. Since the stability index 0 69 &gt; 35 was saved, it was judged that the resin composition of the synthesis example 2 was poor in storage stability, and it was impossible to prepare a sample for evaluation of ED. ❹ [Comparative Synthesis Example 3] Add epoxy resin A2 and epoxy resin A3 to the reaction vessel according to Table 22', impregnate in an oil bath at 85 ° C, stir and dissolve, and further add P-MS and DBTDL. Mix it. Then, the surface was purged with nitrogen, and the temperature of the oil bath was raised to 105 ° C, and the dealcoholization reaction was carried out for 8 hours. Next, after cooling to 60 C, the pressure was reduced to 12 ° Pa, and the dissolved alcohol was removed to obtain a resin composition. The results evaluated in the same manner as in Synthesis Example 12 and the storage stability index 70 0 70 are shown in Table 24. 321346 212 201004993 The epoxy equivalent (wpE) of the resin composition of Comparative Example 3 was changed to 282 g / hr. Further, the initial viscosity is 1.89 Pa.s &lt; lG〇〇pa·s' and the 'preservation viscosity = 2. G3 Pa.s &lt; i_ Pa.s, both of which are fluid liquids. Further, the storage stability index (4) = ι 〇 (5) was determined as a resin composition having a storage stability. [Example 49] A resin composition of the above Synthesis Example 12 was used for 2 weeks, and a cured product was produced to carry out a light resistance test. The results are shown in Table 24. 0 (1) 5 % of C. The resin composition, the curing agent and the hardening accelerator described above were mixed and mixed according to the composition ratio of Table 23, and deaerated under vacuum to obtain a solution for the cured product. (2) A thickness of 3 mm of the character rubber is placed between two stainless steel sheets coated with a release agent to prepare a molding jig. (3) The above-mentioned hardened solution is injected into the forming jig at 12 Torr. The hardening treatment was carried out in an hour after i hours and further at 15 〇t: a i hours. 0 (4) After the internal temperature of the oven was lowered to 3 rc or less, the cured product was taken out, and the sample for light resistance test was prepared by the above method. (5) The results of the light resistance test conducted by the above method using the above sample ' are shown in Table 24. The indicator of the light resistance test of the cured product γι = 10· 1 S 13, and it was judged that the light resistance was acceptable. Next, using the resin composition of Synthesis Example 12, a bullet-type LED having the structure shown in Fig. 1 was produced by the following procedure, and reliability tests (1) to (3) were carried out. The results are shown in Table 24. 321346 213 201004993 (6) A solution for the cured product of (1) as a sealing resin is injected into the cup portion of the mold frame of the diameter of 5 nm. (7) Here, an LED wafer having an emission wavelength of 4 〇〇 nm is crystal-bonded with a silver paste, and a bonding wire (gold wire) is connected to impregnate the lead frame. (8) After defoaming in a vacuum, the hardening treatment was carried out at 90 ° C for 1 hour and further at 11 ° C for 5 hours. (9) Further, in the case of the outer layer resin, 46.6% by mass of the Bis_A1 cyclic oxime oxy-resin is added with 46.6 mass% of a hardener, 〇·2 mass% of a hardening accelerator and stirred under vacuum. Degassing, and injecting it into the mold frame, at 13 (TC for 1 hour, and further at i5 (TCh 6 hours hardening treatment, to obtain a bullet type led.

As a result of the above-mentioned "credibility test (1) α test), the lowest value of all the LEDs was the total beam maintenance ratio (%) = 94% ^ 9 %, and was judged to be acceptable. Next, the result of the above-mentioned "credibility test (2) (TS test)" was carried out, and after 100 cycles of thermal shock, all of the LEDs were turned on, and it was judged that it was acceptable. In addition, as a result of the above-mentioned "credibility test (3) (TC test)", after performing the temperature cycle of 100 cycles, all the LEDs are lit, and the sentence is qualified. From the above results, it is known that The LED light resistance test of Example 49 and the test of the 彳s degree (1) to (3) were all qualified, and the comprehensive judgment was qualified. [Example 50] The resin composition of Synthesis Example 13 was used instead of the resin composition of Synthesis Example 12, and a cured product and an LED were produced in the same manner as in Example 49, and the light resistance test and reliability were carried out in 214 321346 201004993. Tests (1) to (3). The results are shown in Table 24, Time Index Test Index YI = 8.1^13, and it was judged that the light resistance was acceptable. : The result of the above-mentioned test (1) (L test) was carried out, and the lowest value of all up was the total beam maintenance ratio (%) = 96% ^ 9 %, which was judged to be acceptable. Next, the result of the above-mentioned "trustworthiness test (2) (TS test)" was carried out, and after the thermal shock of one cycle was performed, all the LEDs were turned on, and it was judged as pass. Further, as a result of the above-mentioned "credibility test (3) (TC test)", after performing the temperature cycle of 100 cycles, all the LEDs were turned on, and it was judged as pass. From the above, it can be seen that the LED-based photochemical test and the reliability test (1) to (3) of Example 50 are all acceptable, and the overall judgment is acceptable. [Example 51] A resin composition of Synthesis Example 14 was used instead of the resin composition of Synthesis Example 12, and a cured product and an LED were produced in the same manner as in Example 49, and the light resistance test and the reliability test (1) were carried out. ) to (3). The results are shown in Table 24, and the index of γ lightness test γι = 8·9^13, and the light resistance was judged to be acceptable.

: As a result of the above-mentioned "confidence test (1) (L test)", the lowest value of all the LEDs was the total beam maintenance ratio (%) = 95% 29%, and it was judged as pass. Next, the results of the above-mentioned "trustworthiness test (2) (TS test)" were carried out, and after all the thermal shocks of one cycle were applied, all the LEDs were turned on and judged to be acceptable. Further, the results of the above-mentioned "credibility test (3) (TC test)" were performed. 215 321346 201004993 After the temperature of 100 cycles was performed, all the LEDs were turned on, and it was judged as pass. It can be seen that the economical test of the embodiment 51 and the seven-dollar (1) to (3) are all acceptable, and the comprehensive judgment is qualified. [Example 52] The resin composition of i] 15 was replaced with the resin composition of Synthesis Example 12 in the same manner as in Example 49, and a cured product and an LED were produced, and a light resistance steepness test was carried out: and reliability tests (1) to (8). The results are shown in Table 。. The index 3S13 of the resistance type is judged to be qualified. The result of the above-mentioned reliability test (1) (L test) of the lamp, the most = I beam maintenance rate (%) of all LEDs = 92 % ^9〇%, judged to be qualified. As a result of the above-mentioned "trustworthiness test (2) (TS test)", the implementation of the "1" - after the person's thermal shock, all the LEDs were lit and judged to be qualified. Further, as a result of performing the above-mentioned "confidence test (3) (TC test)", it was judged that the "all LEDs were turned on" after the temperature cycle of 1 G0 cycles was performed. From the above results, it was found that all of the LEDs of Example 52, the light resistance test and the reliability test (1) to (3) were qualified, and the overall judgment was a pass. [Example 53] A resin composition of Synthesis Example 16 was used instead of the resin composition of Synthesis Example 12 to produce a cured product and an LED in the same manner as in Example 49, and the light resistance test and the reliability test (1) were carried out. (3). The results are shown in Table 24. 216 321346 201004993 Index of light resistance test ΥΙ = 7. 5S 13, judged that light resistance is acceptable. As a result of the above-mentioned "confidence test (1) (L test)", the lowest value of all the LEDs was the total beam maintenance ratio (%) = 96% 2 90%, and it was judged as pass. Next, the result of the above-mentioned "trustworthiness test (2) (TS test)" was carried out, and after 100 cycles of thermal shock, all of the LEDs were turned on and judged to be acceptable. Further, as a result of performing the above-mentioned "confidence test (3) (TC test)", after performing the temperature cycle of 100 cycles, all the LEDs were turned on, and the judgment was determined to be acceptable. From the above results, it was found that the LED light resistance test and the reliability test (1) to (3) of Example 53 were all acceptable, and the overall judgment was a pass. [Example 54] Except that the resin composition of Synthesis Example 17 was used instead of the resin composition of Synthesis Example 12, and the curing temperature of the cured product and the sealing resin of the LED was changed to 110 ° C for 4 hours, In the same manner as in Example 49, the cured product and the LED were fabricated, and the light resistance test and the reliability test (1) to (3) were carried out. The results are shown in Table 24. The index of the light resistance test YI=8. 8S 13, and the light resistance was judged to be acceptable. As a result of the above-mentioned "confidence test (1) (L test)", the lowest value of all the LEDs was the total beam maintenance ratio (%) = 96% 29%, and it was judged as pass. Next, the result of the above-mentioned "trustworthiness test (2) (TS test)" was carried out, and after 100 cycles of thermal shock, all of the LEDs were turned on and judged to be acceptable. Further, the results of the above-mentioned "credibility test (3) (TC test)" were performed, and 217 321346 201004993, after performing the temperature cycle of 100 cycles, all the LEDs were turned on, and it was judged as pass. From the above results, it was found that the LED light resistance test and the reliability test (1) to (3) of Example 54 were all acceptable, and the overall judgment was acceptable. [Example 55] A resin composition of Synthesis Example 18 was used instead of the resin composition of Synthesis Example 12 to produce a cured product and an LED in the same manner as in Example 49, and the optical resistance test and the reliability test (1) were carried out. To (3). The results are shown in Table 24. The light resistance test index Π = 12.4$13, and the light resistance was judged to be a combination.

As a result of the above-mentioned "confidence test (1) (L·test)", the lowest value of all the LEDs was the total beam maintenance ratio (%) = 97% ^ 90%, and it was judged to be conjugated. Next, the results of the above-mentioned "credibility test (2) (TS test)" were carried out, and after the thermal shock of one cycle was performed, all the LEDs were turned on, and it was judged as pass. © In addition, the results of the above-mentioned "confidence test (3) (TC test)" were carried out, and after all the cycles of 100 cycles were performed, all the LEDs were turned on, and it was judged as pass. From the above results, it was found that the LED light resistance test and the reliability test (1) to (3) of Example 55 were all acceptable, and the overall judgment was acceptable. [Example 56] A resin composition of Synthesis Example 12 was used instead of the resin composition of Example 19, and a cured product and an LED were produced in the same manner as in Example 49, and the light resistance test and the reliability test were carried out (1). ) to (3). The results are shown in Table 24 218 321346 201004993. The indicator of the fiscal test fiber ΥΙ=7·2^13, and it is judged that the light resistance is acceptable. : As a result of performing the above-described reliability test (1) (L test), the lowest value of all the LEDs was the total beam maintenance ratio (%) = 92% ^ 9 %, and was judged to be acceptable. - Next, the result of the "trustworthiness test (2) (TS test)" was carried out. After the thermal shock of 100: under-reduction ring, all the LEDs were lit and judged as qualified. In addition, as a result of the above-mentioned Γ credibility test (3) (TC test), all of the LEDs were turned on after the temperature cycle of 100 cycles of the ring was applied, and it was judged as pass. From the above results, it was found that the LED light resistance test and the reliability test (1) to (3) of Example 56 were all acceptable, and the overall judgment was acceptable. [Example 57] A resin composition of Synthesis Example 20 was used instead of the resin composition of Synthesis Example 12 to produce a cured product and an LED in the same manner as in Example 49, and the light resistance test and the reliability test were carried out (1). ) to (3). The results are shown in Table 24. For the light test index YI=7. 8^13, it was judged that the light resistance was acceptable. As a result of the above-mentioned "confidence test (1) (L test)", the lowest value of all the LEDs was the total beam maintenance ratio (%) = 93%, and it was judged as pass. Next, the results of the above-mentioned "Trustworthiness Test (2) (TS Test)" were carried out. After 100 thermal shocks of the Judah, all the LEDs were lit and judged as qualified. Further, the results of the above-mentioned "credibility test (3) (TC test)" were performed, and 219 321346 201004993, after performing the temperature cycle of 100 cycles, all the LEDs were turned on, and it was judged as pass. From the above results, it was found that the LED light resistance test and the reliability test (1) to (3) of Example 57 were all acceptable, and the overall judgment was acceptable. [Example 58] 'The resin composition of Synthesis Example 21 was used instead of the resin composition of Synthesis Example 12, and a cured product and an LED were produced in the same manner as in Example 49, and the light resistance test and the reliability test were carried out (1). To (3). The results are shown in Table 240. The index of the light resistance test YI = 9.2S13, and the light resistance was judged to be acceptable. As a result of the above-mentioned "confidence test (1) (L test)", the lowest value of all the LEDs was the total beam maintenance ratio (%) = 92% 2 90%, and it was judged as pass. Next, the results of the above-mentioned "confidence test (2) (TS test)" were carried out, and after 100 cycles of thermal shock, all of the LEDs were turned on and judged to be acceptable. @ Further, as a result of the above-mentioned "trustworthiness test (3) (TC test)", after performing the temperature cycle of 100 cycles, all the LEDs were turned on, and it was judged as pass. From the above results, it was found that the LED-based chemiluminescence test and the reliability test (1) to (3) of Example 58 were all acceptable, and the overall judgment was a pass. [Example 59] Using the resin composition of Synthesis Example 13, an SMD type LED having a structure shown in Fig. 2 having a size of 2. 5 mm x 2.5 mm was produced by the following procedure, and it was confirmed that the LED was turned on. 220 321346 201004993 (1) A metal pattern is formed, and a silver paste is applied on a glass epoxy substrate to bond the LED wafers. (2) The substrate is placed in an electric furnace to be hardened. (3) A circuit is formed after the bonding wires (gold wires) are connected to the die-bonded LED wafer. (4) The substrate was placed on the mold, and the resin composition of the synthesis example 13 was poured into a hardening treatment at 90 ° C for 1 hour and further at not: for 5 hours. (5) Separate and cut each LED on the substrate to manufacture an SMD type LED. From the above results, it was found that the LEDs of Examples 49 to 59 were excellent in light resistance and reliability, and were judged to be acceptable as a whole. [Comparative Example 26] A resin composition of Comparative Synthesis Example 1 was used instead of the resin composition of Synthesis Example 12, and a cured product and an LED were produced in the same manner as in Example 49, and light resistance test and reliability test were carried out (1). To (3). The results are shown in Table q 24. The light resistance test index YI=8.4S13, and it was judged that the light resistance was acceptable. The results of the above-mentioned "confidence test (1) (L test)" were performed. "Two of the 10 LEDs did not light up." The total beam maintenance rate (%) could not be measured, and it was judged to be unacceptable. Next, as a result of the above-mentioned "trustworthiness test (2) (TS test)", after performing 100 cycles of thermal shock, only 6 of the 10 LEDs were lit, and it was judged to be unacceptable. Further, as a result of the above-mentioned "credibility test (3) (TC test)", 221 321346 201004993, after performing a temperature cycle of 100 cycles, only 6 of the 10 LEDs were turned on, and it was judged to be unacceptable. As a result of the above, it was found that the LED of Comparative Example 26 had a good light resistance, but the reliability tests (1) to (3) were all unacceptable, so that the overall judgment was unacceptable. [Comparative Example 27] A resin composition of Comparative Synthesis Example 2 was used instead of the resin composition of Synthesis Example 12 to produce a cured product and an LED in the same manner as in Example 49, although an attempt was made to perform a light test and a tooth reliability. Tests (1) to (3) 'But the storage stability of the resin composition was poor, and it was impossible to produce a cured product and an LED. Therefore, the silk stitching was judged to be unacceptable. [Comparative Example 28] A resin composition of Synthesis Example 12 was replaced with a Bis-Al epoxy resin, and a cured product and an LED were produced in the same manner as in Example 49 to carry out a light resistance test and a reliability test 〇) to (3). ). The results are shown in Table 24. ΥΙ The index of the light resistance test ΥΙ = 17. 2 &gt; 13, and the light resistance is judged to be unqualified. As a result of the above-mentioned "confidence test (1) (L test)", the lowest value of all LEDs was determined to be acceptable by the total beam maintenance ratio (%) = 97% 2 90%'. Next, the results of the above-mentioned "confidence test (2) (TS test)" were carried out, and after 100 cycles of thermal shock, all of the LEDs were turned on and judged to be acceptable. Further, as a result of performing the above-mentioned "confidence test (3) (TC test)", after performing the temperature cycle of 100 cycles, all the LEDs were turned on, and 222 321346 201004993 was judged as pass. As a result of the above, it was found that the reliability of the LED of Comparative Example 28 was excellent but the light resistance was poor, so that the overall judgment was unacceptable. [Comparative Example 29] The resin composition of Synthesis Example 12 was replaced with the above-mentioned polyoxyl resin' in which the mixture of the liquid A and the liquid B was mixed at a mass ratio of 1:1. The cured product and the LED were produced in the same manner as in Example 49 except that the curing temperature of the cured resin and the sealing resin of the lED was changed to 7 (TC 1 hour, more advanced / 150 ° C for 5 hours). The light resistance test and the reliability test (1) to (3) were carried out. The results are shown in Table 24. However, the index of the preliminary test γι=23, and the light resistance was judged to be acceptable. The above-mentioned "confidence test (1) α As a result of the test), only 3 of the 10 LEDs were lit. 'The total beam maintenance rate cannot be determined to be unacceptable.

Next, as a result of the above-mentioned "credibility test (2) (TS test)", after the thermal shock of 100 cycles of the clothes, only four of the one LEDs were light and thin, and it was judged to be unacceptable. 'U, the result of the above-mentioned "confidence test (3) (TC test)" was carried out, and after performing a temperature cycle of 100 cycles, only 6 of the 10 LEDs were judged to be unacceptable. From the above results, it was found that the LED of Comparative Example 29 was excellent in light resistance, but the reliability tests (1) to (3) were all unacceptable. , pb, Comparative Example 30] 321346 223 201004993 The resin composition of Comparative Synthesis Example 3 was used instead of the resin composition of Synthesis Example 12, and a cured product and an LED were produced in the same manner as in Example 49, and light resistance test and reliability were performed. Tests (1) to (3). As a result, although the cured product for the light resistance test was produced at 24 °, the crack was formed and the measurement was impossible, so that the light resistance was judged to be unacceptable. As a result of the above-mentioned "confidence test (1) (L test)", only four of the ten LEDs were turned on, and the total beam maintenance ratio (%) could not be measured, and the judgment was determined to be unacceptable. Next, as a result of the above-mentioned "trustworthiness test (2) (TS test)", after performing 100 cycles of thermal shock, only five of the ten LEDs were lit, and it was judged to be unacceptable. Further, as a result of the above-mentioned "confidence test (3) (TC test)", after performing a temperature cycle of 100 cycles, only 7 of the 10 LEDs were turned on, and it was judged to be unacceptable. From the above results, it is understood that the LED of Comparative Example 32 has excellent goodness of light, but the reliability tests (1) to (3) are all unacceptable, so the overall judgment is unacceptable. From the results of Tables 22 to 24, it is understood that the LEDs of Examples 49 to 59 are excellent in terms of the light transmittance, the L test, the TS test, and the TC test. On the other hand, in Comparative Examples 26 to 30, at least one of storage stability, light resistance, L test, TS test, and TC test was defective. According to the above, it is shown that the LED manufactured by using the modified resin composition of the present embodiment is excellent in financial property and reliability. 224 321346 201004993 ο ο ΧΪ* : 念聚矽氡 resin 1 1 1 1 1 1 1 1 1 1 1 1 1 100.0 1 Hydrolysis tank with catalyst DB1DM 1 1 Ο i ! 1 1 1 I ί 1 1 1 1 ί 1卜CO 1 卜ΙΛ C&gt; ΙΑ 〇CO c=&gt; CO o CO d oo o σ&gt; ο 1 1 - 〇〇〇〇LO CD Ο oo oo ea o to G 12· 9 ΙΑ » 1 1 1 t-BuOII [ 1 20.7 1 1 1 1 1 1 1 I 1 1 1 I 20.5 20.2 1 20.2 20.0 20.4 σ> 2· 20.5 1 20.2 ! 20.5 § 28.0 1 1 1 P-HS ! 1 1 1 1 1 1 1 1 I 1 i 1 27.5 Alk mt* 夕坑化1 〇〇〇〇〇O ο o CD O o 〇oooo ο ο 〇〇〇〇ο ο 〇〇 LT3 〇iri 卜 o LA GS CO 03 — cJ Oi G ο» CD 1 1 ί 1 CO 〇〇〇〇〇warn CO ΙΑ oS oo «m 60 eo oo o CO ai 28.0 CO CD 1 1 ί i 1 1 1 1 i ! CO CO 1 1 I i 1 1 1 1 22.2 23.8 24.3 S Οο s 23.8 20.8 s oo oo 32.9 1 1 1 alicyclic ring (10) hire 1 1 1 1 .IO CO 1 I 1 1 I 1 1 1 .I B1&amp;-A3 ring contact 1 1 1 I 1 1 [ 1 1 1 I l 1 1 ο Ζί Bis-A2 氡 氡 酯 1 1 1 1 1 1 1 1 i 1 I 1 1 1 58.4 City ratio 丨 27.9 '27.6 1_ 28.2 27.2 2 7.7 14.6 27.9 27.7 1 27.5 j 1 I loo.o 1 1 Real vibration example 49 (Synthesis Example 12) Example 50 | (Synthesis Example 13) 1 Example 51 B (Synthesis Example) I Actual operation example 52 (Synthesis example) 15) /-N co «〇ΙΛ - Example 54 (Synthesis Example 17) Example 55 (Synthesis Example 18) Example 56 (Synthesis Example 19) Example 57 (Synthesis Example 20) Example 58 (Synthesis Example 21) Comparative Example 26 (• Taste Synthesis Example 1) Comparative W27 (Comparative Synthesis Example 2) tb Example 28 Comparative Example 29 Comparative Example 30 (tb is more synthetic than Example 3) 225 321346 201004993 Table 23 Unit: mass% Composition ratio|tree Composition of Bis-Al epoxy resin polyoxyl resin hardener hardening accelerator Example 49 (Synthesis Example 12) 58.3 — — 41.6 0. 2 Example 50 (Synthesis Example 13) 58. 4 — — 41.4 0. 2 Example 51 (Synthesis Example 14) 59. 5 - 40. 3 0. 2 Example 52 (Synthesis Example 15) 59. 8 - a 40. 0 0. 2 Example 53 (Synthesis Example 16) 58. 1 — 41. 8 0. 2 Example 54 (Synthesis Example 17) 57. 4 — — 42. 5 0. 2 Example 55 (Synthesis Example 18) 57. 4 — — 42. 4 0. 2 Example 56 ( Synthesis Example 19) 58. 4 - a 41.4 0. 2 Example 57 (Synthesis 20) 56. 4 — — 43. 4 0. 2 Example 58 (Synthesis Example 21). 60. 6 — — 39. 3 0. 2 Comparative Example 26 (Comparative Synthesis Example 1) 64. 1 — A 35. 7 0. 2 Comparative Example 27 (Comparative Synthesis Example 2) — — — — — Comparative Example 28 53. 2 46. 6 0. 2 Comparative Example 29 — — 100. 0 — — 226 321346 201004993 § Way U-K-:x |:〇&lt;slave&gt; 〇〇〇〇〇〇〇〇〇〇合〇〇〇〇〇〇〇〇〇〇〇〇〇〇〇〇〇〇〇〇XXXXX § Confidence 峨(3)TC Record 1 〇〇〇〇〇〇〇〇〇〇X 1 〇1 〇3L4 The number of bright spots behind the ring is 10锢/10, 10 of 10, 10 of 10, 10 of 10, 10 of 10, 10 of 10, 10 of 10, 10 of 10, 10 of 10, 10 of 10 10 / Ί 0 out of 10 / 〗 0 out of 10 /10 of 6 /10 of 1 10 /10 悃 6 /10 t 7 锢 10 (2) TSIft «t judgment 〇〇〇〇〇〇〇〇〇〇X 1 〇XX After the thermal shock, the light enters 10 /10« t 10 /10 梱 10 /10 in 10 |10 /10 锢f 10 / 10 out of 10 / 10 out of 10 / 10 out of 10 / 10 out of 10 / 10 of 10 / 6 of 6 / 10 of 1 1 10 / 10 悃 4 » / !0« t 5 /10 锢 mum 妄〇〇〇〇〇〇〇〇〇〇X 1 〇 XX Minimum total beam maintenance rate (X) σ» g CO Od Unmeasured 1 & Unmeasurable Unmeasured anterior Ϊ 〇 〇〇〇〇〇〇〇〇〇〇1 X 〇X - «Μ σ&gt; od CO tso LO _ 〇0 〇〇ej C&gt;3 Bu·CO 1 c&lt;r cannot determine the qualitative determination of the rouge composition 〇〇〇〇〇〇〇〇〇〇Ό XI 1 〇 indicator 0 σ> CO ΙΛ DO 1.42 •«H Ο) c&lt;i Τ—' CO 5 Aluminium 1 1 1.07 Viscosity (Pa*s) 47.0 03 16,2 21.0 S σί Ο» LA 28.7 CO 48.2 &gt;1000 1 1 2.03 33.7 Osl CO 14.5 oo 44.0 α&gt; CO 18.9 PO Two V»1 26.8 33.4 29.0 1 1 Two WPE (g/eq) οα CO Csl ΙΛ 〇〇LO S CO in C^3 m σ&gt;C&lt;3 Unable to measure 1 1 i Washing index (〇gg «ih4 S 5 T—Η 1.08 1.07 〇二 SS 2 1.07 1 1 «〇0.0017 0.0018 0.0017 0.0019 0.0018 i 0.0018 0.0013 0.0012 - 1 0.0014 0.0017 0.0019 0.0018 1 1 1 0.68 0.68 0.67 0.67 0.69 0.68 is 0.68 0.45 1 0.67 0.64 0.00 1 1 1 0.00 0.26 0.11 1 0.43 0.14 0.26 0.26 0.25 0.26 «·* *4 o 0.62 0.26 1 1 1 1.0023 0.5894 1.2423 0.7494 0.5996 0.5894 0.5914 0.5999 0.5914 1.Z423 23.71 0.5916 1 1 Index % 1 , α 58 ～058 ι_ a59 ～059 j A60 ~060 a61 ~061 ot 62 ~062 of 63 ~063 S l Ξ da 65 ~065 a66 ~066 a 67~e 67 «υ iea 69 ~069 1 1 a70 ~070 | Example / I (Synthesis Example 12) \ Example 50 (Synthesis Example 13) Example 51 (Synthesis Example 14) Example 52 (Synthesis Example 15) Example 53 (Synthesis Example 16) Example 54 (Synthesis Example 17) /-N 1S2 Benzene Example 56 (Synthesis Example 19) Example 57 (Synthesis Example 20) Example 58 (Synthesis Example 21) Comparative Example 26 (峨 Synthesis Example 1) Comparative Example 27 (tb is more Comparative Example 2) Comparative Example 28 Comparative Example 30 Comparative Example 30 (Comparative Synthesis Example 3) 227 321346 201004993 Next, an optical lens manufactured using the modified resin composition of the present embodiment will be specifically described by way of examples and comparative examples. The evaluation of the physical properties in Examples 60 to 63 and Comparative Examples 31 to 35 was carried out as follows. &lt;Preservation of the virginity index, and preservation of the resin composition&gt; The preservation stability of the resin composition is evaluated according to the preservation stability index (9) of the following general formula (9). Preservation of female sex index 0 = (storage point) / (starting viscosity) (9) Seal the container of the resin composition immediately after manufacture, at 25 °. After adjusting the temperature for 2 hours, measure 25 ° The viscosity in C is regarded as the "starting viscosity". It is also sealed in a container of resin composition and stored in an incubator at a temperature of 2 5 °C for 2 weeks. After storage, it is measured at 25 °. The viscosity in C is regarded as the "preservation viscosity." ❹ When the resin composition has fluidity (viscosity is lOOOPa·s or less) and the storage stability index 4 is 4 or less, it is judged to have preservation stability. Light resistance test of optical lens (cured material)&gt; Since it is difficult to cut the sample after manufacturing the optical lens, the cured product is produced by the following method, and the evaluation result is evaluated as the light resistance of the optical lens. (0 for the hardened material prepared by the method described later) The liquid was hardened to make a cured product of 20 mm x 10 mm x 3 mm thick. (2) The hardened material was covered with a 25 rom x 228 321 346 2010 04 993 15 ram x 1 x 2 mm black mask covered with a hole having a diameter of 5.5 mm. (3) The preparation device is configured to irradiate UV light from the UV irradiation device (manufactured by Ushio Electric Co., Ltd., [Spot Cure SP7-250DB]) to the above-mentioned oven set to a constant temperature of 50 ° C via an optical fiber. The 5mm hole is immersed in a hole having a diameter of 5. 5mm. In the upper part of the black mask, the UV light of 2W/cm2 is irradiated for 96 hours. (6) The spectroscopic color meter (10% by diameter) has been transformed into a 10mm diameter spectrometer (manufactured by Sakamoto Electric Industries Co., Ltd.). [SD5000]) The sample irradiated with UV is measured. (7) The yellowness (YI) is determined according to "ASTM D1925-70 (1988): Test Method for Yellowness Index of Plastics". When the YI is 13 or less, It is judged as qualified. u &lt;Cold thermal shock test of optical lens> (1) Will be described later The 10 optical lenses manufactured by the method are installed in a thermal shock device ("TSE-11-A", manufactured by Espec Co., Ltd.) at "(-40 芄 to 120 °C) / cycle: exposure time 14 minutes, lifting The heating cycle was carried out under the conditions of a temperature of 1 minute. (2) The sample was taken out after 100 cycles of heat, and sprayed with a permeate ("MicroCheck", manufactured by 公司0ΗΖΑΙ), in a magnifying glass. Next, visually observe whether there is an abnormality (peeling or cracking) and record the number. 229 321346 201004993 (3) The above-mentioned (4) sample confirmed as no abnormality was placed in the apparatus again, and after 100 cycles of thermal cycling, it was evaluated in the same manner. Repeat these operations for evaluation. (4) When one of the 10 samples is abnormal, the evaluation is aborted, and the number of times of thermal shock resistance = (the number of thermal cycles aborted is M100 times) is obtained. When the number of cold shock resistance is 200 or more, the thermal shock resistance is judged to be acceptable. ® <Surface Adhesion Test of Optical Lens> The surface of the optical lens manufactured by the method described later was lightly pressed with a thumb wearing latex gloves, and when the adhesion was not confirmed, the surface adhesion was judged to be acceptable. &lt;Void Test of Optical Lens&gt; Ten optical lenses manufactured by the method described later were visually confirmed under a magnifying glass, and when all of the ten optical lenses were void-free, it was judged to be acceptable. Q When the above-mentioned light resistance test, cold shock resistance test, surface adhesion test, and void test are all qualified, the overall judgment is acceptable. The raw materials used in Examples 60 to 63 and Comparative Examples 31 to 35 are shown in the following (1) to (7). (1) Epoxy Resin (1-1) Epoxy Resin A: Poly(bisphenol A-2-hydroxypropyl ether) (hereinafter, referred to as Bis-A epoxy resin) • Trade name: Asahi Kasei Epoxy Co., Ltd. Company system, "AER" In addition, the epoxy equivalent (WPE) and viscosity measured by the above method are as follows 230 323346 201004993. • Epoxy equivalent (WPE): 187 g/eq • Viscosity (25 ° C): 14. 3 Pa · s (1-2) Epoxy resin B : 3, 4-epoxycyclohexyl fluorenyl-3' , 4'-Epoxycyclohexyl carboxylate (hereinafter referred to as alicyclic epoxy resin) • Trade name: Da i ce 1 Chemical Industry Co., Ltd., "Ce 11 ox i de 2021P" The epoxy equivalent (WPE) and viscosity measured by the above method are as follows. • Epoxy equivalent (WPE): 131 g/eq • Viscosity (25°C): 227 mPa · s (2) Alkoxy calcined compound (2-1) Alkoxylated compound Η: 3-glycidol Methoxypropyltrimethoxydecane (hereinafter referred to as GPTMS) • Trade name: Shin-Etsu Chemical Co., Ltd., "ΚΒΜ-403" (2-2) alkoxydecane compound I: phenyltrimethoxy矽 ( (hereinafter referred to as PTMS) • Trade name: Shin-Etsu Chemical Co., Ltd., "ΚΒΜ-103" (2-3) Alkoxydecane compound J: Dimercaptodimethoxy decane (hereinafter referred to as DMDMS) • Product name: Shin-Etsu Chemical Co., Ltd., "ΚΒΜ-22" (2-4) Alkoxydecane compound Κ: Tetraethoxy decane (hereinafter referred to as TEOS) 23] 321346 201004993 • Trade name: "KBE-04", manufactured by Shin-Etsu Chemical Co., Ltd. (3) Solvent: Tetrahydromethane: manufactured by Wako Pure Chemical Industries Co., Ltd., without stabilizer (hereinafter referred to as THF) (4) Hydrolyzed condensation catalyst : (4-1) Dibutyltin dilaurate (manufactured by Wako Pure Chemical Industries, Ltd., hereinafter referred to as DBTDL) (4-2) Dibutyltin dioxide (Sigma-Al) Drich company

Hereinafter, referred to as DBTDM) (5) Hardener: "4-methylhexahydrophthalic anhydride / hexahydrophthalic anhydride = 70/30"

• Product name: "RIKACID MH-700G" manufactured by Nippon Chemical and Chemical Co., Ltd. (6) Hardening accelerator: Amine compound • Trade name: San-apro Co., Ltd., "U-CAT 18X" (7 Polyoxyl resin 00: Toray · Dow Corning, "EG630 liquid / B liquid" L Synthesis Example 22 (1) = A resin composition was produced by the following procedure. Set the circulating constant temperature water tank to 'return to cool down;

33⁄4--jlK (2) According to , put 8 (TC oil bath) on the magnetic stirrer. The composition ratio shown in the above table is in the environment of 25.

The a1S~A1 epoxy resin, the alkoxy decane compound, and the THI water-like flask were mixed and stirred, and then 7J, -, and a catalyst were added, and the mixture was stirred and mixed. 232 321346 201004993 (3) Next, 'Install the cooling tube in the flask' quickly immersed in an oil bath of 8 ° C and start mixing, and react for 20 hours while refluxing (reflow step). (4) After the reaction was completed, 'cooled to 25 ° C, and then the cooling tube was removed from the flask. (5) After the refluxing, the solution was distilled off at 4 °Pa, 50 °C for 1 hour using an evaporator, and further, dehydration condensation reaction (dehydration condensation) was carried out while 8 (TC was distilled off for 1 hour). (6) After the completion of the dehydration condensation reaction, the mixture was cooled to 25 ° C to obtain a resin group product. (7) The mixing index α71 to ε 71 of the resin composition is shown in Table 27 below. Further, the epoxy equivalent (WPE), the initial viscosity, and the storage viscosity of the resin composition obtained in the above (6) were measured by the above method. Further, the storage stability index 0 Ή ' was obtained. As shown in Table 27, the resin composition of the above Synthesis Example 22 had an epoxy enthalpy (WPE) = 230 g/eq, which showed an appropriate value. Further, 'starting viscosity = 33·7 Pa·s &lt; 1000 Pa· s, and the preservation viscosity = 47· 0 Pa· s &lt; 1000 Pa · s 'both are liquids with fluidity. Also 'preservation stability index 61 71 = 1. 39S4, judged to have preservation stability Resin composition ° [Synthesis Example 23] Except that the time of the reflux step was set to 25 hours, and Synthesis Example 22 The resin composition was produced according to the methods of Tables 25 and 26. The evaluation was carried out in the same manner as in Synthesis Example 22. The evaluation results, the mixed indexes α 72 to e 72 , and the storage stability index 0 72 were expressed in the table. 27 ° 321346 233 201004993 As shown in Table 27, the epoxy equivalent (WPE) of the resin composition of Synthesis Example 23 was 238 g/eq, which showed an appropriate value. Further, the initial viscosity = 15 2 Pa · s &lt; 1000 Pa · s 'And, the storage viscosity = 20 · 3 Pa · s &lt; 1000 Pa · s 'both are liquids with fluidity. Also, the storage stability index 0 72 = 1.3354, which is judged to have a resin composition for preservation stability [Synthesis Example 24] A resin composition was produced in the same manner as in Synthesis Example 22 in accordance with Tables 25 and 26. The evaluation was carried out in the same manner as in Synthesis Example 22, and the evaluation of the 诘® fruit and the mixed index α 73 to ε 73 was carried out. The storage stability index Θ 73 is shown in Table 27. As shown in Table 27, the epoxy equivalent (WPE) of the resin composition of Synthesis Example 24 was 228 g/eq, which showed an appropriate value. =38. 2 Pa · s &lt; 1000 Pa · s ' and, preservation viscosity = 61. 1 Pa · s &lt; 1000 Pa · s 'There are liquids with fluidity. Moreover, the storage stability index θ 73=1. 60S4 is judged to have a resin composition for preserving stability. Q [Synthesis Example 25] The time of the reflux step is set to 7 The resin composition was produced in the same manner as in Synthesis Example 22 except for the above, in accordance with Tables 25 and 26. The evaluation was carried out in the same manner as in Synthesis Example 22. The evaluation results, the mixing indexes α 74 to ε 74 , and the storage stability index Θ 74 are shown in Table 27. As shown in Table 27, the epoxy equivalent (WPE) of the resin composition of Synthesis Example 25 = 214 g/eq, which showed an appropriate value. Further, the initial viscosity = 4. 9 Pa · s &lt; 1000 Pa·s, and the 'preservation viscosity = 9.4 Pa. s &lt; 10 〇〇 Pa. s ' Both are liquids having fluidity. Further, the storage stability index 0 74 = 1. 91 234 321346 201004993 S 4 was determined to have a resin composition for preserving stability. [Comparative Synthesis Example 4] A resin composition was produced in the same manner as in Synthesis Example 22 according to Tables 25 and 26. The evaluation was carried out in the same manner as in Synthesis Example 22. The evaluation results, the mixing index α 75 to ε 75 , and the storage stability index θ 75 are shown in Table 27. As shown in Table 27, the epoxy equivalent (WPE) of the resin composition of Comparative Synthesis Example 4 was 295 g/eQ, which showed an appropriate value. Further, the initial viscosity = 33 qi s &lt; 1000 Pa. s ' and the 'preservation viscosity = 48.2 Pa·s < 1000 Pa. s, both of which are fluid liquids. also. The storage stability index 0 75 = 1 44 S 4 was determined, and it was judged that there was a resin composition for preserving stability. [Comparative Synthesis Example 5] A resin composition was produced in the same manner as in Synthesis Example 22 according to Tables 25 and 26. The evaluation was carried out in the same manner as in Synthesis Example 22. The evaluation results, the mixing index α 76 to ε 76, and the storage stability index θ 76 are shown in Table 27. As shown in Table 27, the epoxy equivalent (WPE) = 295 g / eq' of the resin composition of Comparative Synthesis Example 5 showed an appropriate value. Further, the initial viscosity = 29. OPa · s &lt; 1 OOOPa · s ' is a fluid liquid. However, the preservation viscosity > lOOOPa · s ' is no-flow, and when the stability index 0 76 &gt; 35 is preserved, the stability of the lens is poor. Therefore, the sample for optical lens evaluation cannot be produced. [Example 60] The resin composition 321346 235 201004993 of the above Synthesis Example 22 after the storage for 2 weeks at 25 C was subjected to a light resistance test by the following procedure. The results are shown in Table 27. (1) In a 25 C environment, the resin composition, the hardener, and the hardening accelerator were mixed and scrambled according to the composition ratio of Table 26, and after degassing under vacuum, it was used as a solution for the hardened material. (2) A π-shaped 矽 rubber having a thickness of 3 mm was placed between two stainless steel sheets coated with a release agent to prepare a molding jig. (3) Injecting the above-mentioned hardened solution into the forming jig, and hardening it at i2〇°C for 1 hour and further at 15 (rc&amp; i hours). (4) Temperature drop in the oven After the temperature is less than 3 ° C, the cured product is taken out, and the sample for light resistance test is prepared by the above method. (5) The knot of the light resistance test by the above method using the above sample is not shown in Table 27. The index of the light resistance test of the object γι = 1〇·1^13 'The light resistance was judged to be acceptable. Ο It was confirmed that the resin composition of Synthesis Example 22 was used to produce an optical lens by the following procedure and subjected to thermal shock resistance. Test, surface adhesion test, void test. The results are shown in Table 27. (6) Mixing raw materials in accordance with the blending method of Table 26, after defoaming in a vacuum, set in an injection molding machine (Sodick Co., Ltd.) (7) Also, at 140. (: Hardening for 15 minutes, leaving it to room temperature and then releasing it to obtain an optical lens having a diameter of about 1 cm. The result of the thermal shock test by the above method, the thermal shock test Test - the number of people is 4 times $ 200 times, to determine the cold tolerance The impact resistance was acceptable. 236 321346 201004993 As a result of the surface adhesion test, the adhesion was not confirmed, and it was judged to be acceptable. As a result of the hole test by the above method, no void was confirmed, and it was judged as pass. From the above results, the optical lens of Example 60 was tested for light resistance, thermal shock test, surface adhesion test, and void test, and was judged to be acceptable. [Example 61] The resin of Synthesis Example 23 was used. The composition was replaced with the resin composition of Synthesis Example 22, and a cured product and an optical lens were produced in the same manner as in Example 60, and subjected to a light resistance test, a thermal shock test, a surface adhesion test, and a void test. The results are shown in Table 27. The light resistance test index YI=8.11^13, and it is judged that the light resistance is acceptable. The result of the thermal shock test by the above method, the number of thermal shock tests is 300 times 2,200 times, and it is judged that the thermal shock resistance is qualified. As a result of the surface adhesion test by the above method, the adhesion was not confirmed, and it was judged to be acceptable. As a result of the voiding test, the void was not confirmed, and it was judged to be acceptable. From the above results, it was found that the optical lens of Example 61 was subjected to the light resistance test, the thermal shock test, the surface adhesion test, and the void test. After passing the test, the resin composition of Synthesis Example 24 was replaced with the resin composition of Synthesis Example 24, and the cured product and the optical lens were produced in the same manner as in Example 60, except that the resin group of Synthesis Example 22 was replaced with the resin group 237 321346 201004993. The light resistance test, the thermal shock test, the surface adhesion test, and the void test were carried out. The results are shown in Table 27. The light resistance test index YI=8. 9S13, and the light resistance was judged to be acceptable. As a result of the above-described thermal shock resistance test, the number of thermal shock tests was 500 or more and 2,200 times, and it was judged that the thermal shock resistance was acceptable. As a result of the surface adhesion test by the above method, the adhesion was not confirmed, and it was judged to be acceptable. ® As a result of the void test by the above method, no void was confirmed, so it was judged to be acceptable. From the above results, it was found that the optical lens of Example 62 was qualified for the light resistance test, the thermal shock test, the surface adhesion test, and the void test, and was comprehensively judged to be acceptable. [Example 63] A resin composition of Synthesis Example 25 was used instead of the resin group of Synthesis Example 22, and a cured product and an optical lens were produced in the same manner as in Example 60, and a light resistance test and a thermal shock test were carried out. Surface adhesion test, cavity test. The results are shown in Table 27. The light resistance test index YI=8. 3^13, and it was judged that the light resistance was acceptable. As a result of the thermal shock test by the above method, the number of thermal shock tests was 300 times ^ 200 times, and it was judged that the thermal shock resistance was acceptable. As a result of the surface adhesion test by the above method, the adhesion was not confirmed, and it was judged to be acceptable. As a result of the void test by the above method, it was not confirmed that the empty 238 321346 2〇l〇〇4993 'the same' was judged to be combined. As a result of the test and the above, it was found that the optical lens of Example 63 had a light resistance test, a surface adhesion test, and a void test, all of which were judged to be acceptable. [Comparative Example 31] Composition Comparison The resin composition of Synthesis Example 4 was substituted for the resin of Synthesis Example 22.

A shovel was used to produce a cured product and an optical device in the same manner as in Example 60. The light resistance test, the thermal shock test, the surface adhesion test, and the hole test were carried out. The results are shown in Table 27. The indicator of the optical test YI=8. 42 13, it is judged that the light resistance is acceptable. 1 The results of the thermal shock test by the above method were carried out, and the number of thermal shocks was 100 times &lt; 200 times, and it was judged that the thermal shock resistance was unacceptable. As a result of the surface adhesion test by the above method, the adhesion was not confirmed, and it was judged to be acceptable. The result of the void test by the above method was judged to be unqualified. As a result of the above, it is understood that the optical lens of Comparative Example 31 has passed the photo-resistance test, the surface adhesion test, and the void test, but the thermal shock test is not satisfactory, and the overall judgment is unacceptable. [Comparative Example 32] A resin composition of Comparative Synthesis Example 5 was used instead of the resin composition of Synthesis Example 22, and a cured product and an optical lens were produced in the same manner as in Example 60, although a light resistance test and a thermal shock test were attempted. , surface adhesion reduction test, void test, but the storage stability of the resin composition is poor, 239 321346 201004993 It is impossible to manufacture hardened materials and optical lenses, therefore, the overall judgment is unqualified. [Comparative Example 33] A cured product and an optical lens were produced in the same manner as in Example 60 except that the resin composition of Synthesis Example 22 was replaced with a Bis-A epoxy resin, and the light resistance test, surface adhesion test, and void test were performed. . The results are shown in Table 27. The index of the light resistance test YI = 17. 2 &lt; 13, the determination of light resistance is not the same

As a result of the thermal shock test by the above method, the number of thermal shock tests was 500 or more and 2,200 times, and it was judged that the cold and thermal shock resistance was acceptable. As a result of the surface adhesion test by the above method, the adhesion was not confirmed, and it was judged to be acceptable. As a result of the void test by the above method, no void was confirmed, and it was judged as pass. From the above results, the optical lens of Comparative Example 35 was qualified for the thermal shock test, the surface adhesion test, and the void test. However, since the light resistance test was unacceptable, the overall judgment was unacceptable. [Comparative Example 34] The resin composition of Synthesis Example 22 was replaced with the above-mentioned polyoxyxylene resin in which a mash and a mash were mixed at a mass ratio of 1:1, and a cured product and an optical product were produced in the same manner as in Example 60. The lens was subjected to a light resistance test, a surface adhesion test, and a void test. The results table is not in Table 27. 240 321346 201004993 Index of light resistance test YI=2. OS 13, it is judged that the light resistance is acceptable. As a result of the thermal shock resistance test by the above method, the number of thermal shock tests was 100 times &lt; 200 times, and it was judged that the thermal shock resistance was unacceptable. As a result of the surface adhesion test by the above method, the adhesion was not confirmed, and it was judged to be acceptable. As a result of the void test by the above method, no void was confirmed, and it was judged as pass. As a result of the above, although the optical lens of Comparative Example 34 was qualified, the surface adhesion test, the surface adhesion test, and the void test were satisfactory, but the thermal shock test failed, and the overall judgment was unacceptable. [Comparative Example 35] A composition obtained by mixing Bis-A epoxy resin, GPTMS, and PTMS was replaced with a resin composition of Synthesis Example 2 2 in the same manner as in Example 60, and was produced in the same manner as in Example 60. The cured product and the optical lens were subjected to a light resistance test, a surface adhesion test, and a void test. The results are shown in Table 27. In the light resistance test, the test sample produced a plurality of voids, and the light resistance was not measured. As a result of the thermal shock test by the above method, the number of thermal shock tests was 200 times 200 times, and it was judged that the thermal shock resistance was acceptable. As a result of the surface adhesion test by the above method, the adhesion was confirmed and it was judged to be unacceptable. As a result of the void test by the above method, voids were confirmed in 8 of the 10 samples, and it was judged to be unacceptable. 241 321346 201004993 It is understood from the above results that the optical lens of Comparative Example 35 was qualified in the thermal shock test, but the light resistance test, the surface adhesion test, and the void test were unacceptable, so that the overall judgment was unacceptable. ❹❹ ί 1 1 1 1 1 1 1 ο 8 1 I 1 SB 1 ο 1 1 1 1 1 \ 1 1 CO 〇1 mo IT) ο* ΟΟ C? σ&gt; o 1 1 1 〇♦Η CD 〇· CO C5 C3 03 C0 ixi ^—4 1 1 1 s' Bu C3 (Νϊ f I OO Csl 1 1 1 1 S % t 1 ο ο Ο c £ CS3 Ο C=^ ο ο ◦ c&gt; 1 1 1 Read ο ο ο ixi 卜 Cs3 σ&gt; ο ^4 CT) CO* 1 1 ο oi 1 CD ΟΟ rH CO ID od r·^ ΟΟ «&gt;Μ4 ί Ή Ο ΟΟ C&gt;3 CO CD 1 1 ο CO Cs3 CNI CO CO Oo ΟΟ CO D0 Oi oi CO 1 1 ο id Race 3 tmr «r 1 1 1 Ο CO 1 1 1 1 1 °°赛05 CSJ od 卜 CO C5 CD &lt;M 1 ο ο ο g 称 · JO 5 Ο CM CO CNI :Army»-&lt; CO CD CO Nw/ /-N 哒CO ΙΛ CO &lt;ΝΙ Q So f •us Nu Cang «ί φ Fen! I £ I £ f Μ 242 321346 201004993 Table 26 Unit: mass % Composition ratio resin composition Bis-A epoxy resin polyoxyl resin hardener hardening accelerator Example 60 (Synthesis Example 22) 58. 3 - a 41. 6 0. 2 Example 61 (Synthesis Example 23) 58.4 - ~ 41. 4 0. 2 Example 62 (Synthesis Example 24) 59. 5 - 40. 3 0. 2 Example 63 (Synthesis Example 2 5 ) 59 8 — — 40 0. 2 Comparative Example 31 (Comparative Synthesis Example 4) 64. 1 — — 35. 7 0. 2 Comparative Example 32 (Comparative Synthesis Example 5) — — — — — Comparative Example 33 — 53. 2 — 46. 6 0. 2 Comparative Example 34 — — 100. 0 — 0. 2 Comparative Example 35 63. 7 — — 36. 1 0. 2

243 321346 201004993

-嵴.. X δΑ^ν II 〇〇〇〇XXXXX Optical speed sharp S % 〇〇〇〇〇〇t 〇X The number of holes generated is 0/10/10悃0/10/10 t 0/10 0 of /10 of 0 悃/_t 1 0悃/10 of 0/丨0 of 8 smoke/丨0 f Surface adhesion determination 〇〇〇〇〇1 〇Ο X. Resistance to thermal shock Sex 1 0 〇〇〇. X 1 〇X 〇Number of times write g CO 2500 〇g 1 ^500 g 1 Light resistance judgment 〇〇〇〇〇1 X 〇X 〇in· QO 〇〇od tc*a | Determination of tree wax composition 1 _____ Guaranteed thief determination 〇〇〇〇〇X 1 1 1 Index 0 ?? s 八 I 1 1 ? « £ II 47.0 20.3 -Ό* σΐ 48.2 &gt;1000 i 1 1 Initial viscosity 33.7 15.2 38.2 03 33.4 29.0 1 1 ! WPE (g/eq) c&gt;a 00 CO 〇〇«ec〇m Oi CO Unable to measure 1 1 1 [ Washing index 1 10 g 0.98 5 2 g LT3 2 ε i 1 1 K3 0.0017 0.0014 0.0018 0.0018 0.0019 0.0018 1 1 0.68 i 0.69 0,69 0.68 ! 0.64 0.00 1 1 1 &lt;〇. 0.00 0.26 i 0.14 i 0.26 0.62 0.26 ii ί ϋ 1.0023 0.5716 0.5996 0.5894 23.71 0.5916 1 1 1 Index compilation 1 e a72 Θ 72 α73 Θ 73 α 74 074 074 CL· i a7G ～ ε76 ij 1 4C Example / Comparative Example /-N g S /-s »-· CO CO CO NwX Example 62 (Synthesis Example 2 妁r-*s 2 Ω ^ ψ than the case of example 31 (t匕 is compared with synthesis example 4) ratio 32 (tbfe synthesis example 5) taste example 33 comparison example 34 than the case example 35 244 321346 201004993 Next, related to this implementation The conductive resin composition obtained by adding a conductive metal powder to the modified resin composition of the form is specifically described by way of examples and comparative examples. The physical properties of Examples 64 to 67 and Comparative Examples 36 to 38 are as follows. The following methods are performed. The epoxy equivalent (WPE), viscosity, and mixing index α to 7? were obtained in the same manner as above. &lt;Measurement of average particle diameter of conductive metal powder&gt; ^ The average particle diameter was measured in a dry mode using a laser diffraction type particle size distribution measuring apparatus ("HELOS system" manufactured by SYMPATEC Co., Ltd.). &lt;Measurement of Viscosity of Conductive Resin Composition&gt; The container in which the composition immediately after the production was placed was sealed, and the temperature was adjusted at 25 ° C for 1 hour, and then the viscosity at 25 ° C was measured. When the viscosity is 100 Pa·s or less, it is judged to have fluidity. &lt;Measurement of softening point of phenolic phenol resin&gt; Q Measured according to item 5.8 of "JISK6910: 2007 (phenol resin test method)". &lt;Measurement of hydroxyl equivalent of phenolic phenol resin&gt; The hydroxyl value is measured in accordance with "JIS K0070: 1002 (Test method for acid value, saponification value, ester value, iodine value, hydroxyl value, and unsaponifiable matter of chemical products)" It is a hydroxyl equivalent. &lt;Measurement of Volume Resistivity of Conductive Resin Composition&gt; The conductive resin composition was applied to a thickness of 40/m on a slide glass by a bar coater, and heated at 200 ° C for 60 minutes. A coating film is formed. 245 321346 201004993 This coating film was measured by a resistivity meter ("Loresta" manufactured by Dia Instruments Co., Ltd.), and when the volume resistivity was 9 χ 10 -4 Ω · cm or less, the conductivity was judged to be good. &lt;Measurement of adhesion strength and adhesion evaluation of conductive resin composition&gt; The adhesion strength before and after the moisture absorption treatment was measured by the following procedure. (1) A conductive resin composition is applied to a die pad portion (9 Å x 9 雠) of a copper lead frame. (2) Next, the Shixi wafer (8 mm x 16 mm) was mounted on the die pad portion and heated in an oven at 200 ° C for 1 hour (the sample before moisture absorption treatment). (3) The sample prepared in (2) was absorbed by a constant temperature and humidity machine set to a temperature of 85 ° C and a humidity of 85% for 72 hours (sample after moisture absorption treatment). (4) The above [pre-hygroscopic treatment sample] and [moisture-absorbing sample] are placed on the lower side of the hot plate at 250 °C for 20 seconds, and the lead wire of the lead frame is pulled up. The tensile strength (manufactured by IMADA Co., Ltd.) was measured for the adhesion strength when the tantalum wafer and the die pad were peeled off. 〇 (5) When the residual strength residual ratio expressed by the following formula is 8〇% or more, it is determined that the adhesion is + good. Then, the residual rate of strength (%) = (the strength after the moisture absorption treatment) / (the strength after the moisture absorption treatment) x l 〇〇 &<; void evaluation of the conductive resin composition> above, in the crystal of the copper lead frame The grain pad portion was coated with a conductive resin composition 'mounting glass wafer (8 mm x 8 mm)' at 2 Torr (TC x 1 hour in an oven. The sample was visually confirmed under a magnifying glass to see if there was a void.) Examples and Comparative Examples Resin composition system fluidity, conductivity and 321346 246 201004993 one right two: and when it is not confirmed that voids are formed, the overall judgment is qualified. (1) to (Immediately use the raw materials used in the examples and comparative examples) is expressed in the following ( 1) Epoxy resin _ _ 1) Each _ oxy resin A. Cone 1 Λ Α A type of epoxy resin (hereinafter referred to as "Bis-A epoxy resin"). Name: Asahi Kasei epoxy (share) Company system, [AER] 〇 In addition, the epoxy equivalent (WPE) and viscosity measured by the above method are as follows: • Epoxy equivalent (WPE): 187 g/eq • Viscosity (25t): 14. 3 Pa · s ( 2) Epoxy resin F: bisphenol f-type epoxy resin (hereinafter, referred to as "Bis-F epoxy tree" "): The product name: j本 Epoxy resin company, "jER807" The epoxy equivalent (WPE) and viscosity measured by the above method are as follows. • Epoxy equivalent (WPE): 169 g/eq Ο • Viscosity (25°C): 3. 2 Pa · s (2) Alkoxydecane compound Η : 3-glycidoxypropyltrimethoxy decane (hereinafter referred to as GPTMS) • Trade name: Shin-Etsu Chemical Industrial Co., Ltd.'s "ΚΒΜ-403" (3) Alkoxydecane Compound I: Phenyltrimethoxydecane (hereinafter referred to as PTMS) • Trade Name: Shin-Etsu Chemical Co., Ltd., "ΚΒΜ- 103 (4) Alkoxydecane compound J: Dimercaptodimethoxy decane (hereinafter referred to as DMDMS) 247 321346 201004993 • Trade name: Shin-Etsu Chemical Co., Ltd., "ΚΒΜ-22" (5) Alkoxydecane compound Κ : Tetraethoxy decane (hereinafter referred to as TEOS) • Trade name: Shin-Etsu Chemical Co., Ltd., “ΚΒΕ-04” (6) Solvent (6-1) Tetrahydrofuran: Wako Pure Chemicals Industrial (stock) company, does not contain stabilizer (hereinafter referred to as THF) (7) Hydrolysis condensation catalyst: dilauric acid Butyltin (manufactured by Wako Pure Chemical Industries, Ltd., hereinafter referred to as DBTDL) ® (8) Hardener (8-1) Hardener Α: Phenolic phenol resin (trade name "PHEN0LITE", manufactured by DIC Corporation); Hydroxyl equivalent 104 g/eq, softening point 100 ° C) (hereinafter, abbreviated as "NP resin") (8-2) Hardener B : 1,8-diazabicyclo [5. 4.0] undecene-7 ( San-apro Co., Ltd., trade name "DBU" (hereinafter referred to as "DBU") Q (9) Thinner: o-nonylphenol glycidyl ether (product of Sakamoto Pharmaceutical Co., Ltd., trade name) "SY-0CG"; epoxy equivalent 181g/eq, viscosity 8mPa · s) (10) Silver powder (10-1) scaly silver powder (average particle size 6. 3# m) (10-2) spherical silver powder (average Particle size (Synthesis Example 26) Resin composition J: Resin composition J was produced by the following procedure and evaluated. 248 321346 201004993 (1) Preparation: Set the circulating constant temperature water tank to 5 °C to return to the cooling tube. Further, an 8 〇t oil bath was placed on a magnetic stirrer. (2) According to the composition ratio of Table 28, in an environment of 25 C, an epoxy resin, an alkoxy compound, and THF are added to a flask to which a stir-mixer has been added, and after mixing and stirring, water is added thereto. Hydrolyze the condensation catalyst and mix and stir. (3) Secondly, install the cooling tube in the burning furnace, quickly dipped in 8 (rc oil bath and start stirring, and react for 1 hour while refluxing. (4) After the reaction is finished, 'cool down to 25t' ^ and then remove from the flask. Lower the cooling tube, and take the sample solution after the end of the refluxing step. Distillate for 5 hours at 80 ° C using an evaporator at 400 Pa, 50 side, (5) After the refluxing step, the C column is removed for 1 hour. Further, the dehydration condensation reaction is carried out on one side. (6) After completion of the reaction, it is cooled to 25 ° C, (7) the mixing index of the resin composition is ❹. 'Transferred to the resin composition j. α 77 to ε In Table 30, according to the above method, the epoxy equivalent (WPE) of the resin composition j obtained in the above (6).

(Synthesis Example 27) (8) Further, the composition ratio thereof was evaluated in conjunction with Synthesis Example 2 6 7 Κ '. Mixing index Resin composition Κ : According to the same procedure, the synthetic resin composition α 78 to ε 78 is shown in Table 30. 321346 249 201004993 The above resin composition is an epoxy equivalent (WPE) = 228 g/eq, which shows an appropriate value. Further, the viscosity is 13. 8 Pa . s, which is a liquid having fluidity. (Synthesis Example 28) Resin Composition L: The resin composition L was synthesized and evaluated in the same manner as in Synthesis Example 26 in accordance with the composition ratio of Table 28. Mixed fingers α79 to ε79 are shown in Table 30. The above resin composition is an epoxy equivalent (WPE) = 2 〇 6 g / e (}, which indicates a suitable value. Further, the viscosity is 18.2 Pa · s, which is a liquid having fluidity. (Synthesis Example 29) ° Resin composition Μ : According to the composition ratio of Table 28, the resin composition 合成 was synthesized and evaluated in the same manner as in the synthesis example. _ to “0 is shown in Table 30. The above resin composition is epoxy. Equivalent (WPE) = 2 〇 8 When the value is 10.2 Pa.s, it is a liquid with fluidity. &quot;Ill (Example 64) Conductive resin composition 制造 is manufactured according to the following steps, will be evaluated The results and the mixing index α 77 to £ 77 are shown in the table.... Using the resin composition j of the above Synthesis Example 26, according to Table 29: blending the raw material 'with three roll mills (manufactured by Inoue Manufacturing Co., Ltd.): f Further, the step of 'using a vacuum chamber' will be defoamed at 400 ° 3 for 3 minutes. Γ Electrical resin composition μ conductive resin composition k sticky sound field · s ' is a liquid with excellent fluidity. · 5 On the slide of the slide, the conductive resin composition i is applied to the thickness and is fine. C plus (four) minutes 321346 250 201004993 When the volume resistivity of the coating film was measured, the volume resistivity of the coating film was 2 χ 10-4 Ω · cm, and it was judged that the conductivity was good. The bonding strength of the conductive resin composition 1 was measured. The residual ratio was obtained by the following procedure: (1) Four conductive resin compositions 1 were applied to the die pad portion (9 mm x 9 mm) of the copper lead frame. 8mmxl6mm) Mounted in the die pad section 'heated in the oven at 200 ® °C x l hours. (3) In the sample made in (2), two are considered as "pre-hygroscopic sample" (4 The two remaining samples of the sample prepared in (2) were absorbed for 72 hours in a temperature-dependent humidifier set to a temperature of 85 ° C and a humidity of 85%, and then regarded as "a sample after moisture absorption treatment". (5) Using the above "pre-moisture-preventing sample" and "moisture-absorbing sample", the crucible wafer is placed underneath on a hot plate at 250 °C for 20 seconds to pull up the lead wire of the lead frame. The adhesion strength at the time of peeling the stone wafer and the die pad was measured using a push-pull meter (manufactured by IMADA Co., Ltd.), and each measurement was performed with n=2. (6) Substituting the average value of the subsequent strengths of the "pre-hygroscopic treatment sample" and the "moisture-absorbing sample" obtained above into the following equation, the residual strength residual ratio is obtained, and the evaluation is performed. Then, the residual rate of strength (%) = (the strength after the moisture absorption treatment (the strength after the moisture absorption treatment) xl0 (Kl48inN) / (151mr 〇 X100 = 98% 2 80% 'the conductive resin composition i The subsequent determination is good. 25] 321346 201004993 Next, a conductive resin composition 1 '' mounted glass wafer (8 mm x 8 mm)' was applied to the die pad portion of the copper lead frame to be heated in an oven at 200 ° C for 1 hour. The sample was visually confirmed under a magnifying glass and no void was produced. As a result of the above, it has been found that the conductive resin composition is excellent in fluidity, electrical conductivity, and adhesion, and voids are not formed. (Example 65) 导电 The conductive resin composition 2 was produced in the same manner as in Example 64 using the composition of Table 29, and the evaluation results and the mixing index α 78 to ε 78 were evaluated. Shown in Table 30. The viscosity of the conductive resin composition 2 is 23·7 Pa·s, which is a liquid excellent in fluidity. The volume resistivity of the conductive resin composition 2 was 3×1 (Γ4 Ω·cm, and it was judged that the conductivity was good. The sample before the moisture absorption treatment of the conductive resin composition 2 and the sample after the moisture absorption treatment were used. Then, the average value of the intensity is substituted into the following equation to obtain the residual strength residual ratio, and the adhesion is evaluated. Then, the residual strength of the strength (the subsequent strength before the moisture absorption treatment after the moisture absorption treatment) xl 〇〇 = (138 mN) / ( 145mN)xl00=95% $80% 'The conductivity of the conductive tree wax composition 2 is judged to be good. Next, 'the conductive resin composition 2' is coated on the die pad portion of the copper lead frame. ^Glass wafer (8niinx8mffl The sample was heated in an oven at 200 ° C for 1 hour. The sample was visually confirmed under a magnifying glass, and voids were not formed. From the above results, it was found that the conductive resin composition 2 was flowed 252 321 346 201004993, conductivity, (Embodiment 66) No voids were formed. Therefore, it was determined in accordance with Table 9, and the above-mentioned resin composition was used to produce conductivity in the same manner as in Example 64. Resin composition 3, and The evaluation results and the mixed pure α79 to ε79 are shown in Table 3. The viscosity of the conductive resin composition 3 is 28.2 Pa · s, which is a liquid with excellent fluidity. ® The volume resistivity of the conductive resin composition 3 The rate is 3 χ 10 _ 4 Ω · cm, and it is judged that the conductivity is good. The average value of the subsequent strengths of the sample before the moisture absorption treatment and the sample after the absorbing treatment of the conductive resin composition 3 is obtained by the following formula. The strength residual rate of the receiver is evaluated, and the adhesion is evaluated. Then, the residual rate of strength (%) = (the strength after the moisture absorption treatment) / (the strength after the moisture absorption treatment) x l00 = (124 mN) / (136 mN) x l00 = 91 %

G8 〇%, and the adhesion property of the conductive resin composition 3 was judged to be good. Further, since the conductive resin composition of Example 65 of the same composition was produced in the same composition except that the ratio of the NP resin to the DBU was changed, the present embodiment (10) showed a better adhesion, so it was estimated that the combination was used 2 A kind of hardener, which will be followed by 'coating a conductive tree on the die pad of the copper lead frame, and the material 3 'go-breaking wafer (8mmx8mm)' is heated at 200 °C x l hours. The sample was visually confirmed under a magnifying glass and no void was produced. * As a result of the above, it was found that the conductive resin composition 3 was excellent in the properties of the joints 321346 253 201004993, conductivity, and adhesion, and no voids were formed. (Example 67) The conductive resin composition 4 was produced and evaluated in the same manner as in Example 64, using the resin composition μ described above. The evaluation results and the mixed indexes α80 to ε8〇 are shown in Table 3〇. The viscosity of the conductive resin composition 4 is 19. i ρ & · s, which is a fluid _ excellent liquid.体积 The volumetric electricity (4) of the conductive tree rib forming material 4 is 3xlG_4Q · CD1, and it is judged that the conductivity is good. The average value of the subsequent strengths of the "pre-hygroscopic treatment sample" and the "post-moisture-treated sample" of the conductive resin composition 4 was substituted into the following equation to determine the subsequent strength residual ratio, and the adhesion was evaluated. Then, the residual rate of strength (%) = (the strength after the moisture absorption treatment) / (the strength after the moisture absorption treatment) xloo = (108 mN) / (128 mN) x l 〇〇 = 84% © , conductive resin composition 4 The adhesion determination is good. Next, the conductive resin composition 4 was applied to the die lining of the copper lead frame, and the glass piece (8 mm x 8 mra) was mounted at 2 Torr (TC x 1 hour in an oven. The sample was visually confirmed under a magnifying glass. The results of the above-mentioned results show that the conductive resin composition 4 is excellent in fluidity, conductivity, and adhesion, and no voids are formed, which is acceptable. The mouth is 疋 (Comparative Example 36) According to Table 29 In the same manner as in Example 64, a conductive resin composition 5 was produced and evaluated using a Bls_A epoxy resin and a Bis_F epoxy tree 321346 254 201004993 fat-substituted resin composition J. The evaluation results are shown in Table 3 The viscosity of the conductive resin composition 5 is 26.4 Pa·s, which is a liquid having excellent fluidity. The volume resistivity of the conductive resin composition 5 is 3χΐ〇-4ω·cm, and it is judged that the conductivity is good. The average value of the bonding strength between the "pre-hygroscopic treatment sample" and the "moisture-absorbing sample" of the resin composition 5 is substituted into the following equation, and the ratio of the residual strength of the subsequent strength is evaluated. (%)=( Subsequent strength after wet treatment) / (external strength before moisture absorption treatment) &gt;&lt;1〇〇=(8111^)/(13211^众1〇〇=61%&lt;80%, conductive resin composition The adhesion determination of 5 is defective. Next, the conductive resin composition 5 is applied to the die pad portion of the copper lead frame, and a glass wafer (8 mm x 8 mm) is mounted, and heated at 20 TC x 1 hour in an oven. The sample was visually confirmed to have no voids. ❹ From the above results, the conductive resin composition 5 was excellent in fluidity and conductivity, and voids were not formed. However, the adhesion was poor, and the overall judgment was unacceptable. (Comparative Example 37) The conductive resin composition 6 was produced and evaluated in the same manner as in Example 1 except that the resin composition J was replaced with Bis-A epoxy resin, PTMS, or TMS according to the composition of Table 29. The results are shown in Table 3. The viscosity of the conductive resin composition 6 was 18.2 Pa·s, which was a liquid excellent in fluidity. 321346 255 201004993 The volume resistivity of the conductive resin composition 6 was 42 χ 10_4 Ω · cm, and the conductivity was determined to be Poor. Conductive resin composition 6 The average value of the subsequent strengths of the "sample before moisture absorption treatment" and the "sample after moisture absorption treatment" was substituted into the following equation to determine the residual strength of the adhesive strength, and the adhesion was evaluated. Then, the residual ratio of strength (%) = (hygroscopicity) The strength after the treatment) / (the strength before the moisture absorption treatment) x l 〇〇 = (12 〇 mN) / (134 mN) x 100 = 89% 2 80% 'The adhesion property of the conductive resin composition 6 was judged to be good. Next, the conductive resin composition 6 was applied to the die pad portion of the copper lead frame, and a glass wafer (8 mm x 8 mm) was mounted and heated at 20 TC for 1 hour in an oven. Visually confirm that this sample has voids under a magnifying glass. As a result of the above, it was found that the conductive resin composition 6 was excellent in fluidity and adhesion, but it was confirmed that voids were formed due to poor conductivity. (Comparative Example 38) A conductive resin composition 7 was produced in the same manner as in Example 62 except that the composition of Table 29 was replaced with a Bis-A epoxy resin, a Bis-F epoxy resin and TEOS in place of the resin composition J. 'And evaluate. The results are shown in Table 30. The viscosity of the conductive resin composition 7 is 16.3 Pa · s, which is a liquid excellent in fluidity. The volume resistivity of the conductive resin composition 7 was 3 x 10 · cm '. It was judged that the conductivity was good. The average value of the joint strengths of the "pre-hygroscopic treatment sample" and the "moisture-absorbing sample" of the conductive resin composition 7 was substituted into the following equation to obtain 323346 256 201004993, and the strength residual ratio was then evaluated. Then, the residual rate of strength (%) = (the strength after the moisture absorption treatment) / (the strength before the moisture absorption treatment) x l 〇〇 = (13 lmN) / (14 〇 mN) x l 〇〇; r 94% 2 80% ' The adhesion of the conductive resin composition 7 was judged to be good. Next, the electroless resin composition 7 was applied to the crystal pad portion of the copper lead frame, and a glass wafer (8 mm x 8 mm) was mounted and heated in the supply at 200 ° C x l. Visually confirm that the sample produced empty meat under a magnifying glass. As a result of the above, the conductive resin composition 7 was excellent in fluidity, conductivity, and adhesion. However, it was confirmed that voids were formed, and it was judged that it was unacceptable. As shown in Table 28 to Table 30, a resin composition obtained by mixing an epoxy resin with a specific alkoxylated compound at a specific ratio in the present embodiment and performing cohydrolysis condensation, and a conductive metal The conductive resin composition of the powder or the curing agent is excellent in fluidity. Further, the conductive resin composition of the present embodiment is excellent in conductivity and adhesion, and voids are not generated. Table 28 Unit: mass % Composition ratio Bis-A epoxy resin Bi sF epoxy resin ^ .1. Alkoxydecane compound THF Hydrolysis condensation catalyst GPTMS PTMS DMDMS TE0S DBTDL Synthesis Example 26 37· 5 31. 6 3 1 0.9 8. 5 0. 40 Synthesis Example 27 43. 5 - ]〇. 2 14. 3 3. 5 — 20.4 7. 8 0. 36 Synthesis Example 28 48. 0 6. 9 11.8 5. 9 2. 5 0.3 9 5. 4 0. 32 Synthesis Example 29 72. 4 — 1.8 6 4. 6 — ]〇. 8 , 4. I 0. 24 321346 257 201004993

6Z&lt; bag 铋: rock 蚌〇ΙΛ OO 卜 · L〇 Bu · m 〇CO scaly silver powder 〇iri CO 63.0 62.0 62.0 65.0 o 05 in 65.0 thinner m iri ΙΛ ΙΛ in ιή m ΙΛ ΙΛ tri LT> ΙΛ 1 1 1 I 1 1 1 ◦ 1 1 1 1 1 1 o ^J3 1 1 I 1 1 1 o 1 1 CO o C&lt;l ο C&lt;l ο CO CNJ 〇1 NF resin oo CD ο oo cd 05 CO oo CD Oo CO oo cd Bis-F 环娜意1 I 1 1 CO c&lt;i 1 Bis-A ring-frequency grease 1 I 1 1 15.3 17.5 12.3 Resin composition in Bu · 16.5 18.0 18.0 1 1 1 Composition ratio resin composition j Resin Composition K Resin Composition L Resin Composition M Comparative Example 36 Comparative Example 37 Comparative Example 38 Example 64 Example 65 Example 66 Example 67 258 321346 201004993

Oe&lt;0G .· X ^ $ .· OA^CV Comprehensive judgment 〇〇〇〇 XXX Conductive composition void determination 〇〇〇〇〇 XX Residual strength residual rate (%) 〇〇〇〇X 〇〇 Residual rate § 55 5 〇〇Volume resistivity (χΙΟ'Ώ · an) 1 〇. 〇〇〇〇X 〇 电阻 电阻 CM CM CO CO CO CQ CS3 CO Viscosity (Pa · s) % 〇〇〇〇〇〇〇 Viscosity 21.5 1 23.7 [CO 05 18.2 16.3 Resin composition mixed index 1.02 1.07 1.05 1.20 1 1 1 0.0014 0.0014 0.0017 0.002 1 1 I Bu 1.05 1.56 1 Bu CO cnS 5.82 1 1 1 0.05 0.25 0.25 1.00 1 1 1 0.1177 1.666G 0.5914 4.0000 1 1 1 対 4 pale result index number α 77 ～ 077 α78 ～ £78 X i 〇 1 § 1 1 1 Example / Comparative Example Example 64 Example 65 Example 66 Real 67 Comparative Example 3G Comparative Example 37 丨 1 Comparison Example 38 259 321346 201004993 This application is based on a Japanese special request for a Japanese company on July 3, 2008 (Japan’s special wish), on December 1st, 2008, against Japan. Japanese patent application for the franchise Japanese Patent No. 2_-314273) is used for this purpose with reference to its contents. [Industrial Applicability] According to the present invention, a heart-country has a good-looking scented resin composition, which can be formed in a good transparency, has excellent resistance to touch, discoloration, resistance, and cold resistance. _, hetero-hardened. ^ ^ Further, by using the modified resin composition of the present invention, it is possible to provide an excellent adhesion to the element or the sealing material, and a fineness in which the cracking brightness is reduced over a long period of time.咖 ' ' ' 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 发光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光 光b&gt; a photosensitive material excellent in adhesion of polymerization due to oxygen; a coating agent containing the composition; and a fluorescent resin composition excellent in dispersion stability of the coating grade &lt; And a light-storing material composed of the fluorescent resin composition; and <d> excellent in mobility, conductivity, and adhesion without causing a void resin composition; electric &lt;e&gt; mobility, insulation, and It is excellent in the following, and does not produce a void resin composition or the like. , 邑 260 321346 201004993 [Simple description of the diagram] Figure 1 shows a cross-sectional view of the shell-type LED. Fig. 2 is a cross-sectional view showing an SMD type LED. [Main component symbol description] ❹ 10, 20 Light-emitting diode (LED) 10A, 20A LED chip 10A, 20A Anode 10C, 20C Cathode 12, 22 Sealing material 14, 24 Bonding wire 16 Outer resin 18 Lead frame 26 Package substrate 28 Reflector 261 321346

Claims (1)

201004993 VII. Patent application scope: L A modified resin composition obtained by reacting an alkoxy decane compound represented by an epoxy resin (彡 彡 with the following formula ,), (R丨)η—Si one ( OR)4-n (1) (wherein η represents an integer of 3 or more and 整数 or more; and R1 each independently represents a hydrogen atom, and at least one organic group selected from the group consisting of "to c" below) The group: a) an aliphatic hydrocarbon unit having one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, or cyclic groups, and having a carbon number of 4 An organic group having a cyclic ether group of 24 or less and an oxygen atom number of 1 or more and 5 or less. b) having a structural group selected from a chain, a branch, or a ring selected from unsubstituted or substituted. An aliphatic hydrocarbon unit composed of one or more kinds of structures, and a monovalent aliphatic organic group having a carbon number of 1 or more and 24 or less and an oxygen atom number of 5 or more; 〇c) having an unsubstituted or substituted aromatic group a hydrocarbon unit and, if necessary, having a chain, branch, or ring selected from unsubstituted or substituted An aliphatic hydrocarbon unit composed of one or more types of structures, and a monovalent aromatic organic group having a carbon number of 6 or more and 24 or less and an oxygen atom number of 5 or more; on the other hand, R2 is independently represented by each other; a halogen atom or one or more organic groups selected from the group consisting of d): d) having a structural group selected from a chain, a branch, or a ring selected from unsubstituted or substituted Aliphatic smoke consisting of 321346 262 201004993 unit 'and a monovalent organic group having a carbon number of 1 or more and 8 or less;) The above-mentioned dazzling compound contains the following (β) and (C): (Β) At least one alkoxydecane compound having η = 1 or 2 and having at least one cyclic ether group as Ri, and at least one alkoxy group having (C) or 2 and having at least one aromatic organic group as R1 a decane compound; a mixing index α of the alkoxydecane compound represented by the following general formula (2) is 〇. 〇01 or more and 19 or less: a mixing index a = (ac) / ( 〇: b) (2) (in Here, in the formula (2), ab represents the content of the component (B) in the alkoxydecane compound represented by the general formula (i). Mol%), 〇:c represents the content (mol%) of the above component (c) in the non-alkoxydecane compound of the general formula (1); and the residual alkoxy group in the above modified resin composition The amount of the modified resin composition of the first aspect of the invention, wherein the modified resin composition is 25. (The viscosity is 1 〇〇〇pa·s or less) 3. The modified resin composition of claim 1 or 2, wherein the epoxy equivalent of the composition of the fresh-modified resin is 100 g/eq or more and 700 g/eq or less. 4. The modified resin composition of any one of claims 1 to 3, wherein the alkoxydecane compound has a condensation ratio of 8% or more. 5. The modified resin composition of any one of claims 1 to 4 wherein the viscosity of the aforementioned epoxy resin (A) at 253⁄4 is 500 Pa · 263 321346 201004993 s or less 6. If the scope of application is The modified resin composition according to any one of items 1 to 5, wherein the epoxy resin (1) has an epoxy equivalent of not more than 300 g/eq. 7. For the modified resin composition of any of the claims 1 to 6 of the patent application, the epoxy resin (A) is composed of the glycidyl etherate of the poly-preferable compound. Polyfunctional epoxy resin. 8. For the modified resin composition of any of the first to seventh patent applications, the above-mentioned epoxy resin (A) is a bisphenol A type ring urgency. In the range of the U 8th item, the composition index 'in the above-mentioned general formula (3), the above-mentioned alkoxylate compound has a mixing index point of 0.01 or more and 1.4 or less: 〇 mixed index {( (2) (wherein, in the formula (3), 0η2 represents an alkoxydecane compound of the general formula (1), and an alkoxydecane compound of η=2 Content mol%) 'Red Q represents the content of the alkoxylated compound of the alkoxy group-n and oxime represented by the general formula (1), and the stone μ represents the salt of the alkoxy compound represented by the formula (1). , η = ι of the alkoxy compound containing 篁 (m〇l%), and the system satisfies the value of the following formula: ^ 〇SKySn〇) / (stone n0+) Snl + stone n2)} 芸〇 1) . (1) The resin composition (manufactured by the following general formula (4) and the oxime alkoxy decane compound shown in the following general formula (4) The mixing index is 〇〇2 to 15: Mixed index 7 = ( 7 a) / ( 7 s) (4) 321346 264 201004993 (here, in the formula (4), ra represents the mass of the epoxy resin (A) ( g), 7 s represents the mass (g) of the alkoxy oxime compound having n = 〇 to 2 in the alkoxy oxalate compound represented by the general formula (1). A method for producing a modified resin composition, which comprises an alkoxydecane compound containing at least (B) and (C) represented by the following general formula (1) in the presence of an epoxy resin (4) A method of producing a modified resin composition according to any one of claims 10 to 10, which comprises the following steps (a) and (b): (a) step: in an epoxy resin ( In the presence of A), a step of producing an intermediate by subjecting at least an alkoxydecane compound represented by the general formula (1) (B) and (C) to a co-hydrolysis by a reflux step without dehydration; (b) Step: The step of subjecting the intermediate produced in the step (a) to a dehydration condensation reaction; (R)n - Si _ (0R2)4-n (1) ❹ (where η represents 0 or more and 3 or less In addition, R1 each independently represents a hydrogen atom, and at least one organic group selected from the group consisting of the following tenth to c): a) having a chain or sub-group selected from unsubstituted or substituted An aliphatic hydrocarbon unit composed of a structure of more than one of a group of branches and rings, and having a carbon number of 4 or more and 24 And an organic group of a cyclic ether group having an oxygen atom number of 1 or more and 5 or less; b) having a structure group selected from a chain, a branch, and a ring selected from unsubstituted or substituted An aliphatic 265 321 346 201004993 hydrocarbon unit having a structure of more than one, and a monovalent aliphatic organic group having a carbon number of 1 or more and 24 or less and an oxygen atom number of 5 or more; c) having an unsubstituted or substituted aromatic group a hydrocarbon hydrocarbon unit and, if necessary, an aliphatic hydrocarbon unit formed of one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, or cyclic structures, and having a carbon number of 6 or more and 24 or less and a monovalent aromatic organic group having an oxygen atom number of 0 or more and 5 or less; on the other hand, R each independently represents a hydrogen atom, and one or more organic groups selected from the group consisting of d) : d) an aliphatic hydrocarbon unit having one or more structures selected from the group consisting of unsubstituted or substituted chain, branched, or cyclic structures, and having a carbon number of 1 or more and 8 or less} Valence organic group); (B) n=l or 2 and at least one cyclic test group as y One less alkoxydecane compound; (C) n=l or 2 and having at least one aromatic organic group as one of R1 to G less than one alkoxydecane compound; and, the following general formula (2) represents The mixing index α of the alkoxydecane compound is 0· 〇〇1 or more and 19 or less: the mixing index a = ( ac) / ( α b) (2) (here, in the formula (2), ab The content of the above (Β) component (m〇1%), ac represents the content of the component (c). 12. The method for producing a modified resin composition, in the presence of the epoxy resin (a), A modified resin composition containing at least one of the following formula (1) and the alkoxy decane compound of the following formula (1), and the production of the modified resin composition of any one of the claims 1 to 321346 266 201004993 And the method comprises the following steps (c) and (d): (c) a step of: containing at least the alkoxydecane compound of (B) and (C) represented by the general formula (1), a step of producing an intermediate by co-hydrolysis without a reflux step of dehydration; (d) Step: subjecting the intermediate produced in the step (c) to an epoxy tree (A) a step of performing a dehydration condensation reaction in the coexistence; (ROn-Si - (0R2)4-n (1) ^ (wherein η represents an integer of 0 or more and 3 or less, and R1 each independently represents a hydrogen atom And at least one organic group selected from the group consisting of a) to c): a) having a structural group selected from the group consisting of unsubstituted or substituted chain, branched, and cyclic An aliphatic hydrocarbon unit composed of one or more kinds of structures, and an organic group having a cyclic ether group composed of a carbon number of 4 or more and 24 or less and an oxygen atom number of 1 or more and 5 or less; Q b) having a selected from An aliphatic hydrocarbon unit composed of one or more types of unsubstituted or substituted chain, branched, and cyclic structural groups, and having a carbon number of 1 or more and 24 or less and an oxygen atom number of 0 or more a monovalent aliphatic organic group of 5 or less; c) an unsubstituted or substituted aromatic hydrocarbon unit, and having a structure selected from a chain, a branch, or a ring selected from unsubstituted or substituted, if necessary An aliphatic hydrocarbon unit composed of one or more types of structures, and having a carbon number of 6 or more and 24 or less and an oxygen atom number of 0 or more The monovalent aromatic organic group; 267 321346 201004993 On the other hand, R2 each independently represents a hydrogen atom, and one or more organic groups selected from the group consisting of d): d) having an unselected substituent Or an aliphatic hydrocarbon unit composed of one or more types of structures in a chain, a branched, or a cyclic structure, and a monovalent organic group having a carbon number of 1 or more and 8 or less; (B) n=l or 2 and at least one cyclic ether group as at least one oxodecane compound of R1; (C) n=l or 2 and having at least one aromatic organic group as R1 to less 1 The alkoxy decane compound; and the mixing index α of the above-mentioned compound oxime compound represented by the following general formula (2) is 0.001 or more and 19 or less: the mixing index a = (ac) / ( a: b) (2) Here, in the formula (2), <2b represents the content (m〇i%) of the component (B), and <2c represents the content of the component (C) (mo 1%). ).至1. 01至1。 01. The mixing indicator yS of the alkoxy decane compound represented by the following general formula (3) is 0. 01 to 1 4 : Mixed index / 5 = { (; 5n2) / (ygn0 + ySnl) } (3) (In the formula (3), '々n2 represents the alkoxydecane compound represented by the general formula (1) 'π -2 of the content of the calcined base-calcined compound (mo 1 %), the stone π Ο is not in the general formula (1), the content of the alkoxy compound of n = oxime 〇l%), 々nl represents the content (mol%) of the alkoxylated compound of 'n=1' in the oxyxanthene compound represented by the general formula (1) and these systems satisfy the value of the following formula : 268 321346 201004993 0${(々η0)/(/9η0+/5η1+^η2)}$0.1). 14. The method for producing a modified resin composition according to any one of claims 11 to 13, wherein the epoxy resin (Α) represented by the following general formula (4) and the alkoxydecane compound are used. The mixing index 7 is 〇.〇2 to 15: the mixing index γ = (T a) / ( rs) (4) (here, in the formula (4), ra represents the mass of the epoxy resin (A) (g) ' 7 s represents the mass (g) of the alkoxydecane compound of n=0 to 2 ® in the alkoxylated compound of the general formula (1). The method for producing a modified resin composition according to any one of claims 11 to 14, wherein the temperature of the reflux step without dehydration is from 50 to 100 °C. The method for producing a modified resin composition according to any one of claims 11 to 15, wherein the condensation ratio of the intermediate obtained by co-hydrolysis without a reflux step with dehydration is 78% or more . The method for producing a modified resin composition according to any one of claims 11 to 16, wherein an alkoxide-based organotin is used as a catalyst when the co-hydrolysis is carried out. A resin composition obtained by adding an oxetane compound (D) to the modified resin composition of claim 1 of the patent application. A fluorescent resin composition obtained by adding a phosphor (E) to a modified resin composition of claim 1 of the patent application. 2 0. A kind of conductive resin composition' is added to the conductive resin powder (F) in the resin composition of 269 321346 201004993. 21. An insulating resin composition obtained by adding an insulating powder (G) to a modified resin composition of the first aspect of the patent application. 22. A resin composition obtained by adding an epoxy resin (A') to a modified resin composition of claim 1 of the patent application. A curable resin composition obtained by adding a hardener (H) to a resin composition according to any one of claims 1, 18 and 19. ® 24. A curable resin composition obtained by adding a hardening accelerator (I) to the resin composition of claim 23 of the patent application. A photosensitive resin composition obtained by adding a photo-acid generator (J) to a resin composition according to any one of claims 1, 18 and 19. 26. A luminescent component produced by using the resin composition of claim 24 or 25. 〇 27. An optical lens obtained by using the resin composition of claim 24 or 25. 28. A light-storing material obtained by using the resin composition of claim 24 or 25. 29. A semiconductor device comprising the luminescent component of claim 26 and/or the optical lens of claim 27 of the patent application. A curable resin composition obtained by adding a hardening accelerator (I) to a resin composition according to any one of claims 20 to 22. 270 321346 201004993 31. A photosensitive resin composition obtained by adding a photoacid generator (J) to a resin composition according to any one of claims 20 to 22. A coating agent comprising the resin composition of any one of claims 24, 25, 30, and 31. 33. A coating film obtained by using the coating agent of claim 32. 271 321346