TW565577B - Epoxy resin composition - Google Patents

Abstract

This invention discloses an epoxy resin composition, which comprises (A) a phenolic epoxy resin represented by formula (I), in which each R1 can be, the same or different, independently selected from groups composed of free hydrogen, C1-C6 alkyl group, C6-C10 aromatic group, C6-C10 aromatic group substituted with C1-C6 alkyl group, each R2 can be, the same or different, independently selected from groups composed of free hydrogen, C1-C6 alkyl group, C6-C10 aromatic group, C6-C10 aromatic group substituted with C1-C6 alkyl group, R3 can be, the same or different, independently selected from groups composed of free hydrogen, C1-C6 alkyl group, C6-C10 aromatic, C6-C10 aromatic group substituted with C1-C6 alkyl group and each R4 can be, the same or different, independently selected from groups composed of free hydrogen, C1-C6 alkyl group, C6-C10 aromatic, C6-C10 aromatic group substituted with C1-C6 alkyl group, and n is 0 or 1; (B) an epoxy resin different from the compound (I); and (C) hardener. The invented epoxy resin composition can be used as sealing materials, adhesives, printed circuit board materials, and for powder coating. When a composition contains the invented phenolic epoxy resin, moisture absorption and thermal expansion coefficient of a board material can be reduced, and fluidity and glass transition temperature during molding can be increased. Therefore, hest resistance, dimensional stability, reliability, moldability and crack reduction can be improved.

Description

565577 A7 137 V. Description of the invention (i) The present invention relates to an epoxy resin composition, in particular, the epoxy resin composition includes a special phenolic epoxy resin. This can effectively reduce the hygroscopicity and thermal expansion coefficient of the material, improve the fluidity and glass transition temperature during molding, and therefore improve the product's heat resistance, dimensional stability, reliability, moldability and reduce cracking. . When electronic components are becoming thinner, larger, or modularized, it is easy to cause cracks or warpage of the 1C chip due to the presence of a small amount of water or internal stress, which will reduce the reliability of the product. Therefore, it is necessary to There are better packaging materials to improve it. In order to solve the problems of cracking or warping during 1C packaging, many related patents have been published. The main method adopted is to improve heat resistance or increase the content of fillers to reduce hygroscopicity. For example, Shin-Etsu Chemical Company in U.S. Patent No. 5,358,980 uses naphthalene-containing epoxy resin to improve the heat resistance (or glass transition temperature) of the packaging material. However, it caused a significant decrease in liquidity. Printed by Sumitomo Chemical Co., Ltd. in European Patent No. 700947 by the Central Standards Bureau of the Ministry of Economic Affairs of Japan, and by Sumitomo-Bakelite in Japanese Patent Application No. 8-20631. Low viscosity epoxy resin to increase the content of filler in the packaging material, thereby reducing water absorption. However, it can also cause a significant decrease in liquidity. Therefore, an object of the present invention is to provide a novel epoxy resin composition in order to solve the above-mentioned problems. When the epoxy resin composition is used as a packaging material for a semiconductor device, it can reduce moisture absorption while maintaining Or improve its heat resistance and fluidity, or reduce the coefficient of thermal expansion to increase production ______5__ This paper size applies the Chinese National Standard (CNS) Λ4 specification (210 × 297 ^ ϋ 565577 A7 ^ _ __ B7 V. Description of the invention (2) Dimensional stability and crack resistance. In order to achieve the above object, the epoxy resin composition of the present invention includes: (A) a phenolic epoxy resin represented by the chemical formula 化学:

Among them: each R1 may be the same or different, independently selected from the group consisting of free hydrogen, Cle6 hydrocarbon group, C6-1G aromatic group, and Cv1G aromatic group substituted with Cw nicotinyl group, each R2 may be the same or different, Independently select free hydrogen, C1-6 hydrocarbon group, CV1 () aromatic group, C6-1G aromatic group substituted by Cw hydrocarbon group, printed by the Consumer Cooperative of the Central Standards Bureau of the Ministry of Economic Affairs

This paper size applies Chinese National Standard (CNS) Λ4 specification (210X29? Public) 565577 A7 V. Description of invention (R4

0 0 0

0

Among the ethnic groups formed by the Shellfish Consumer Cooperative of the Central Standards Bureau of the Ministry of Economics, among them, select free hydrogen, Cl.6 nicotine, C61. Aromatic groups, in the group consisting of C6_1G aromatic groups substituted with Ci6 hydrocarbon groups, each R4 can be the same or different, independently selected from free hydrogen, Ci 6 hydrocarbon groups, c6.10 aromatic groups' C㈣ aromatic groups substituted with Cl_6 hydrocarbon groups In the group formed, η is 0 or 1; (B) an epoxy resin different from the compound (I); and (C) a hardener, in which the phenolic epoxy resin (A) accounts for one of all epoxy resins. To 99% by weight,% oxygen resin (B) accounts for 99 to 99% by weight of the total epoxy resin, and hardener accounts for 1 to 90% by weight of the epoxy resin composition. Each R1 in the compound (I) may be the same or different, and is preferably independently hydrogen 'c1-6 alkynyl' c1-6 cycloalkynyl 'c2_6 dilute group, c2_6 alkynyl, phenyl, naphthyl, or Ci · 6 courtyard group, c1-0 ring alkyl group, C: 2 · 6 dilute group, or c26 alkynyl substituted phenyl or naphthyl group. Specific examples of R1 such as hydrogen, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, tertiary butyl, n-pentyl, please read the note on the back · Note-then fill in On this page, t if this paper size is applicable to Zhongguanjia County (CNS) Λ4 specification (21GX 297 male i 565577 A7 ------B7) 5. Description of the invention (4) ~ isoamyl, neopentyl, hexyl, Phenyl, tolyl, ethylphenyl, or naphthyl, etc. Preferred examples are hydrogen, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, third butyl, Pentyl, hexyl, or phenyl, etc. More preferred examples are hydrogen, fluorenyl, third butyl, or phenyl. R2 in compound (I) may be the same or different, and most 妤 is independently hydrogen, cv6 Alkyl, Cw cycloalkyl, (: 2 · 6 alkenyl, c26 alkynyl, phenyl, naphthyl, or phenyl substituted with Cw alkyl, Cl · 6 cycloalkyl, c26 alkenyl, c26 alkynyl Or tea based,

Printed by Shellfish Consumer Cooperative of the Central Bureau of Standards of the Ministry of Economic Affairs (please read the notes on the back before filling out this page) R2 specific examples such as hydrogen, methyl, ethyl, n-propyl, isopropyl, n-butyl, Isobutyl, third butyl, n-pentyl, isopentyl, neopentyl, hexyl, phenyl, tolyl, ethylphenyl, or naphthyl. Preferred examples are hydrogen, methyl, ethyl , N-propyl, isopropyl, n-butyl, isobutyl, page _8 This paper size applies to China National Standards (CNS) A4 specifications (210 X 297 public expense) ~~~ '' --- 565577 A7 ______ 5. Description of the invention (5 ^ dibutyl, pentyl, hexyl, or phenyl. More preferred are hydrogen, methyl, ethyl, n-propyl, or isopropyl. When R2 in compound (I) is

R3 is preferably hydrogen, Cw alkyl, Cl-6 cycloalkyl, c2-6 alkenyl, c26 alkynyl, phenyl, naphthyl, or Cw alkyl, Cw cycloalkyl, alkenyl, or C2_6 alkynyl Substituted phenyl or naphthyl. Specific examples of R3 are hydrogen, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, third butyl, n-pentyl, isopentyl, neopentyl, hexyl, phenyl , Pyrene, ethylphenyl, or naphthyl. Preferred are hydrogen, fluorenyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, third butyl, pentyl, hexyl, or benzyl. When R2 in compound (I) is (Please read the precautions on the back before filling this page)

, 1T Printed by the Consumer Standards Cooperative of the Central Bureau of Standards, Ministry of Economic Affairs, R4

0 〇 0

〇

It is preferred that each R4 is independently hydrogen, Cw alkyl, Cw cycloalkyl, C26 alkenyl, C2 · 6 alkynyl, phenyl, naphthyl, or Cu alkyl, (: 1-6 cycloalkyl , C 6 alkenyl, or C2 · 6 alkynyl substituted phenyl or naphthyl. Specific examples of R4 include hydrogen, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, and 565577 ^ " -l- > / V. Description of the invention (土) -n-pentyl #pentyl, neopentyl, hexyl, phenyl, tolyl, ethylphenyl, or naphthalene Preferred examples are hydrogen, methyl, ethyl, n-propyl, 2propyl JL butyl'isobutyl 'tert-butylpentylhexyl or phenyl earth. More preferred is hydrogen, or phenyl J Dology, the various types of epoxy resins shown can be para-position and para-position, (P, 〆 ·) is optional. Specific examples of phenolic epoxy resins can be used (please read the back first! / Note Things • Items to fill out this page}

Printed by Shellfish Consumer Cooperative, Central Bureau of Standards, Ministry of Economic Affairs

This paper size applies to Chinese National Standard (CNS) A4 specification (210 × 297 public power) 565577 A7 Β7 V. Description of the invention (7)

Formed by the ethnic group. The% Oxygen Resin composition of the present invention printed by the Central Bureau of Standards, Shellfish Consumer Cooperative of the Ministry of Economic Affairs may use one or more phenolic% oxygen resins (A) and one or more phenolic epoxy resins (A) Different% oxygen resin (B). The phenolic epoxy resin (A) has been defined in detail as above. Epoxy resin (B) can be commonly used epoxy resins, such as phenolic epoxy resin, bisphenol A ring gas resin, varnish type (〇rth〇_cres〇i novolak) epoxy Resin, polyfunctional epoxy resin, etc. The phenol-based epoxy resin (A) needs to account for 99 to 99% of the total epoxy resin, preferably 1 to 95 wt. /. '' More preferably, the epoxy resin needs to contain 4 to 90 wt% / phenol phenolic epoxy resin (A) in all epoxy resins. The epoxy resin (B) accounts for 1 to 99 wt% of the total epoxy resin. The hardener (c) in the epoxy resin composition of the present invention may include various hardeners used in general% oxygen resins, such as amines, anhydrides, or phenols (phenoHc). hardener. The content of the hardener (c) is 1 to 90 wt% of the entire epoxy resin composition. The preferred amount of amine hardener used in the present invention is 0.5 ~ 3.0 active 11 per epoxy group (please read the precautions on the back before filling this page) «Clothing · Order __ This paper Standards General National Standards (CNS) A4 Specification (21〇 < 297g ^ 565577 Printed by the Consumer Cooperatives of the Central Standards Bureau, Ministry of Economic Affairs, printed A7 Β7 V. Description of the invention (8) Activity of wind hardener The equivalent ratio of hydrogen to the epoxy group of the epoxy resin is 0.5 to 3.0. The preferred amount of the acid anhydride (acid anhydrous) hardener used in the present invention is the acid anhydride of the acid anhydride hardener and the epoxy group of the epoxy resin. The equivalent ratio is 0.5 to 3.0. The preferred amount of the phenol-based hardener used in the present invention is that the equivalent ratio of the hydroxyl group of the various hardener to the epoxy group of the epoxy resin is 0.5 to 2.0, and most preferably 0. 6 to 1.3. Examples of the phenol-based hardener include novolac, cresol novolac, resorcinol novolac, and bisphenol A novolac. The epoxy resin composition of the present invention may further include a hardening accelerator. This hardening accelerator can use a common catalyst, and its type is not particularly limited The content of the hardening accelerator may be from 0.1 to 20 wt%, based on the total amount of the epoxy resins (A), (B) and the hardener being 100 wt%. Specific examples of the hardening accelerator include, for example, : Phosphorus compounds such as triphenylphosphine, tris (2,6 · dimethoxyphenyl) phosphine, tris (para-β-tolyl) phosphine, triphenylphosphite, etc .; 2-fluorenimidazole, 2-benzene Imidazoles, 2-undecylimidazole, 2-heptadecylimidazole, 2-ethyl-4 · fluorenimidazole, and the like; 2-dimethylaminomethylphenol, benzyldiamine Tertiary amines such as methylamine; 2,5-azobicyclo [4,3,0] _5_nonene, 1,4-azobicyclo [2,2,2] octane, 1,8_ Organic salts of azobicyclo [5,4,0] -7-undecene etc. The epoxy resin composition of the present invention may contain various additives as needed. Examples of the additives include fillers and surface treatment of fillers. Agents, flame retardants, release agents, colorants, stress relieving agents, etc. The type of filler is not particularly limited, and examples thereof include crystallinity; epsilon powder, fusible silica powder, quartz glass powder, talc powder , Aluminum silicate powder, cistern powder, aluminum powder, calcium carbonate powder Among them, silica-based fillers are especially preferred. 12 This paper size applies Chinese National Standard (CNS) Λ4 specification (210 × 297 公 #) (Please read the precautions on the back before filling this page), 11 565577 5 _ ^ _ The A7 B7 printed by the Consumer Cooperatives of the Central Bureau of Standards of the Ministry of Economic Affairs, and the description of the invention (9) The content of the filler is 1 to 97% by weight of the total epoxy resin composition, especially 60 to 90% by weight. Examples include silane coupling agents. Examples of flame retardants include antimony trioxide, phosphate, and bromide. Examples of release agents include various waxes. Examples of colorants include carbon black. The stress relieving agent may include, for example, silicone resin or rubber. The epoxy resin composition of the present invention can generally be prepared by mixing the aforementioned various components with an appropriate kneading device, and if necessary, mixing with other additive components, and the mixing order of these components is not particularly specified. The present invention will be further explained by the following examples, but the present invention is not limited to these examples. All ingredients of all compositions are by weight. Preparation Example 1: Preparation of 2,2'-bis (glycidoxy) biphenyl (epoxy resin 0) 2,2'-bis (glycidyloxy) biphenyl In a 500 ml two-necked round-bottomed bottle was equipped with a machine Stirrer and condensing tube, 48.4 g (0 · 20 mole) of 3,3 ', 5,5 · -tetramethyl-4,4 ·· biphenol, 0.68 g (0. 01 mole) of imidazole And 185.2 g (2.0 mol) of epigas, heated to 115 ° C and refluxed for two hours (the starting material 3,3 ', 5,5f-tetramethyl-4,4'-linked was determined by chromatography Complete reaction of phenol). After returning to room temperature, it was concentrated by a rotary concentrator to remove excess surface gas. The obtained product was further added with 200 ml of toluene and 50 ml of a 1N aqueous sodium hydroxide solution, heated to 90 ° C and vigorously stirred, and the reaction was refluxed for two hours. After returning to room temperature, the organic layer and the water layer are extracted and separated. The water layer is extracted with toluene. 13 Paper size is applicable to Chinese National Standard (CNS) Λ4 specification (210X 297 male f) (Please read the precautions on the back before filling in this Page) # 衣. -Rr Fill in Taiding 565577 Printed by A7, Shellfish Consumer Cooperative of the Central Standards Bureau of the Ministry of Economic Affairs 5. Description of the Invention (ιοί) (160 ml x 2 times); Combine the organic layers, dry over anhydrous sodium sulfate, filter, and spin Concentrator concentrated to give the crude product. The crude product was purified by silica gel chromatography to give a colorless liquid product with a yield of 920 / 〇oil, 1H NMR (CDC135 200 MHz) δ 2.54 (2H, dd, J = 5.1, 2.5 Hz), 2.70 (2H, dd, J = 5.1, 4.0 Hz), 3.16 (2H, dddd, J = 5.5, 4.0, 2.9, 2.5 Hz), 3.93 (2H, dd, J = 1L2, 5.5 Hz), 4. · 17 (2H, dd, J = 11.2, 2.9 Hz), 6.95 (2H, dd, J = 8.1, < 1.0 Hz), 7.03 (2H, dd, J = 7.3, 1.0 Hz), 7.24 (4H, m) 13C NMR (CDC13, 100 MHz) δ 44.3 (t), 50.2 (d), 68.9 ⑴, 112 · 6 (d), 121.0 (d), 128.3 (s), 128.5 (d), 131.4 (d) , 155.9 (s). '' Preparation Example 2: Preparation of 2,2'-bis (glycidoxy) _3,3 ', 5,5'-tetratert-butylbiphenyl (epoxy resin D) 9 2,2'_bis (glycidyloxy) -3,3,5,5, -tetra-tert-butylbiphenyl was prepared in the same manner as in Example 1, except that during the purification process, a white solid product was obtained by crystallization from ethanol with a yield of 85%. Melting point is 186 ° C. NMR (CDC13, 200 MHz) δ 1.33 (18Η5 s) 5 1.43 (ΐ8Η s), 2.19 (2Η, dd, J = 4.9, 2.7 Ηζ), 2.63 (2Η, dd, J = (9, 4 4 Ηζ), 3.00 (2Η, dddd, J = 5.5, 4.4, 3.3, 2.7 Ηζ), 3.57 (2Η, dd J = 11.0, 5.6 Ηζ), 3.68 (2Η, dd, 11.0, 3.3 Ηζ), 7 · 14 (2Η d J = 2.4 Hz), 7.38 (2H, d, J = 2.4 Hz) '14 This paper size is applicable to the Chinese National Standard (CNS) Λ4 size (210X 297 cm) (Please read the first note on the back ^ Fill in this page again]

Printed by the Central Bureau of Standards, Shellfish Consumer Cooperative, 565577 kl B7 ---------- V. Description of Invention (11) MS (m / e): 522 (M +), 466 (base), 451 337, 225, 57, 41, 29 〇 Preparation Example 3: 1, lf-bis [(4-glycidoxy-3-phenyl) phenyl] -2-methylpropane (epoxy resin B ) Preparation of 1, l'-bis [(4-glycidyloxy_3-phenyl) phenyl] _2-methylpr〇pane The preparation steps were the same as in Example 1, except that during the purification process, a mixed solution of f-ethyl ethyl ketone and toluene ( 3: 1) to extract and crystallize from toluene to obtain a white solid product with a yield of 85-90%. Melting point is 131-134 ° C. lU NMR (CDC135 200 MHz) δ 0.83 (6Η? d9 J = 6.5 Ηζ) 5 2 · 37 (1Η, dsept, J = 11.0, 6.5 Ηζ), 2.57 (2Η, dd, J = 4.9, 2 · 7

Hz), 2.71 (2H, dd, J = 4.9, 4.4 Hz), 3.15 (2H, dddd,] = 5.0, 4.4, 3.0, 2 · 7 Hz), 3.31 (1H , D, J = 11. 0 Hz), 3.86 (2H, dd, J = 11.l, 5.0 Hz), 4.07 (2H, dd, J = 1M, 3.0 Hz), 6.81 (2H , D, J = 8.2 Hz), 7 · 12 (2H, dd, J = 8.2, 2.0 Hz), 7.20 (2H, d, J = 2.0 Hz), 7.30 (6H, m), 7. · 45 (4H, dd, J = 6.9, 1.7 Hz). Examples 1 to 3 and Comparative Example 1 Each component in the epoxy resin composition was mixed with a double-roller kneader at 80-130 ° C, and then it was pulverized to prepare the epoxy resin composition in b. The chemical formula and equivalent weight of the epoxy resin are shown in Table 1 *, and the amounts of the epoxy resin and hardener in the examples and comparative examples are shown in Table 2. Among them, the epoxy resin Y is a conventional epoxy resin, and the epoxy resin B is , D, 〇 are special epoxy resins used in the present invention. The hardener is phen〇i_formaldehyde nov〇iakresin 'softening point is 7051. When the paper size is applicable to China ----- (Please read the notes on the back before filling this page)

-、 1T Yinzhong, Co-operative Consumer Cooperative, Central Standards Bureau, Ministry of Economic Affairs 565577 A7 __ 一 __ 5. Description of the invention (l2) The amount is 103 g / eq. In addition, each composition in Table 2 contains 82% by weight of fusible silica powder, 0.85% by weight of hardening accelerator and various additives (such as surface treatment agents, flame retardants, release agents, colorants ... ....) A total of 1.75wt ° / 〇. Test method: • Water absorption according to the SEMI G66-96 test specification. The sample is compression molded in a hot press to prepare a test piece with a thickness of 3mm and a diameter of 50mm. It is postcure at 175 ° C and placed in 85GC. In a constant temperature and humidity machine at / 85% RH for 72 hours, measure the weight of the test piece before and after placing it in the constant temperature and humidity machine to calculate the water absorption of the sample. • Gel time: Take a small amount of sample powder and place it on a cure plate at 175 ° C. Stir the duck tongue until the sample loses fluidity. The gelation time is measured. • Spiral flow length According to SEMI G11-88 test specifications, the important conditions are as follows:

1. Hardening time in mold 90 seconds 2. Mold temperature 175 ° C 3. Transfer pressure 6.895 ± 0.177MPa (1000 ± 25psi) 4. Transfer speed at least 25.4mm / sec (r7sec) • Glass transfer Temperature and coefficient of thermal expansion are based on SEMI G13-88 test specifications. Sample preparation is a cylinder with a diameter of 5mm obtained by hot pressing. It is hardened (Post Cure) for more than 6 hours in an oven at 175 ° C, and then cut into a 5mm thickness. The sample is placed on a thermomechanical analyzer. 16 This paper is suitable for China. Standard (CNS) A4 Standard Orange (210X 297 ^ #) (Please read the precautions on the back before filling out this page), 1T 565577 Printed by A7 B7 of the Central Bureau of Quasi-Ministry of Economic Affairs, Consumer Cooperation, I ...... .... — .-, I _ 1 1 One, five, description of the invention (13) (TMA) test, heating rate 5 ° c / min. From the experimental results in Table 2, it can be seen that the inclusion of epoxy resin B or D in the formulation can reduce the water absorption and thermal expansion coefficient of the material, and increase the glass transition temperature, while epoxy resin D or 〇 can significantly improve fluidity. Implement your 4 ~ 6 and Comparative Examples 2, 3 The sample preparation method and the types and amounts of hardeners and additives used in the formula are the same as those in Examples 1 ~ 3, and the amount of hardening accelerator is 0.7wt%, each The composition and properties of the components are summarized in Table III. The epoxy resin M is a multifunctional epoxy resin produced by Japan's Nippon Kayaku company, the equivalent weight is 160 ~ 170, the trade name is EPPN-501; the epoxy resin N is the O-cresol novolac epoxy resin produced by Sumitomo Chemical Co., Ltd. , Equivalent weight 190 ~ 205, trade name is ESCN-195XF. From the experimental results in Table 3, it can be seen that epoxy resin O or B can reduce the water absorption of the material and improve its fluidity at the same time. From the results of the above examples, it can be known that the epoxy resin composition of the present invention has low hygroscopicity, low thermal expansion coefficient, high fluidity, and heat resistance, so it is particularly suitable for use as semiconductor sealing or encapsulants, and can also be used as Products or devices such as molding materials, powder coatings, adhesives, printed circuit board materials, etc. --1 --- ： ---- clothing-(Please read the note on the back V before filling in this tribute) The size of the paper is applicable to the Chinese National Standard (CNS) Λ4 specification (210X 297 male) 565577 A7 B7 V. Description of the invention (14) Table 1 Chemical formula equivalent (g / eq) (Please read the precautions on the back before filling this page)

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Yuka Shell Co. YX-4000H (Epoxy Y) 2,2,-bis (glycidylox y) biphenyl (Epoxy 0) 2,2,-bis (glycidylox y) _3,3,5,5,5f-tetra-tert-butyl biphenyl (Epoxy D)

o o s0

o o

R propane (Epoxy B) R = i-Pr (isopropyl) The paper size is applicable to the Chinese National Standard (CNS) A4 specification (210 × 297 mm) 192 177 261 253 565577 A7 B7 V. Description of the invention (15) Table 2 Printed by the Consumers' Cooperative of the Central Bureau of Standards, Ministry of Economic Affairs 11 Example 1 Example 2 Example 3 Comparative Example 1 Group of epoxy resin Y 8.66 9.65 10.20 10.62 into epoxy resin B 2.16 _-—— epoxy resin D _ 1.07 __________ wt Epoxy resin 〇_ ______ 0.42% Hardener 4.58 4.68 4.78 4.78 Gelation time (sec ·) 27 29 28 28 Spiral flow length 40 49 59 40 Property (in) Water absorption (wt%) @ 85 ° C / 85% R 0.192 0.193 0.211 0.199 H / 72h Glass transition temperature 150 159 138 148 (° C) Coefficient of mass thermal expansion < Tg 11 10 13 13 (ppm / C) > Tg 37 37 47 45 Please read one of the first notes-item Refill this page 19 This paper size applies the Chinese National Standards (CNS) Λ4 Regulations (210 × 297) 565577 A7 B7 Printed by the Consumer Cooperatives of the Central Standards Bureau of the Ministry of Economic Affairs 5. Description of the invention (β Table 3 Example 4 Example 5 Comparative Example 2 Example 6 Comparative Example 3 Group of epoxy resin 0 2.06 _ 5.24 into epoxy resin M 8.24 3.55 10.3 — epoxy resin N — — — 5.24 10.48 wt epoxy resin B — 10.62 — —% hardener 5.25 5.38 5.25 5.07 5.07 Filler 82 78 82 82 82 Hardening accelerator 0.7 0.7 0.7 0.7 0.7 Additive 1.75 1.75 1.75 1.75 1.75 Gelation time (sec.) 20 30 17 22 15 Spiral flow length 29 46 21 31 12 Property (in) Water absorption Rate (Wt ° / o) 0.291 0.259 0.306 0.232 0.234 @ 85 ° C / 85 ° / 〇quality RH / 72h Glass transition temperature 161 150 — 147 — (° C) Coefficient of thermal expansion (ppm / ° C) < Tg 12 15 -13 — > Tg 45 57 — 42 — (Please read the notes on the back before filling out this page) Order ο 2 This paper size applies to the Chinese National Standard (CNS) Λ4 specification (210X 297 mm)

Claims (1)

565577 5 ^ " 11 -----.. Two: /. .J person ▲ * " * " * · ·· " " PRIVATE * " 乂 一秘 1 · 1 · Scope of patent application, Continued | Announcement, Scope of Patent Application 1. An epoxy resin composition comprising: (A) a phenolic epoxy resin represented by the chemical formula (I): Wherein: each R1 may be the same or different, and independently selected from the group consisting of free hydrogen, Cm hydrocarbon group, C6-H) aromatic group, C㈣ aromatic group substituted with Cm hydrocarbon group, each R2 may be the same or different, Independently selected free hydrogen, Cm hydrocarbon, Gh) aromatic group, C6-1G aromatic group substituted with Cl-6 nicotyl group ' Continuation page (if the patent application page is insufficient, please note and use the continuation page) 565577 Patent application scope, continuation page; In the group of members, in which R3 is a free hydrogen, α6 hydrocarbon group, c6, an aromatic group, and a group consisting of a C㈣ aromatic group substituted with a Cl-e hydrocarbon group, each R4 may be the same or different and independently Select free hydrogen, hydrocarbyl, c㈣ aromatic group, substituted by Ci-efe group On. In the group consisting of aromatic groups, η is 0 or 1; (B) a phenolic epoxy resin different from the compound (I), a bisphenoi a epoxy resin, ortho-cresol novolak ) Epoxy resin, or polyfunctional epoxy resin; (C) a hardener, selected from the group consisting of amines, anhydrides, and phenols; wherein the phenolic epoxy resin (A) occupies all the rings The epoxy resin is 1 to 99 wt%, the epoxy resin (B) accounts for 1 to 99 wt% of the total epoxy resin, and the hardener accounts for 1 to 90% of the epoxy resin composition. 2. The epoxy resin composition as described in item 1 of the scope of the patent application, wherein each R1 is independently a nitrogen 'Cl-6' group, a Cl-G group is a C2 · 6 group. C2 · 6 fast base 'benji' naki 'or Ci 6 Hyunji, Cm ring Hyunji' 2 _ Continued page (when the patent application page is insufficient, please note and use the continuation page) 565577 Patent application scope Continued fluorenyl, or benzyl or naphthyl substituted by fastyl. 3. The epoxy resin composition as described in claim 1 of the scope of patent application, wherein each γ is independently hydrogen, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, Third butyl, n-pentyl 'isopentyl, neopentyl, hexyl, benzyl, methylbenzyl, ethylbenzyl, or naphthyl. 4. The epoxy resin composition according to item 1 of the scope of patent application, wherein each Ri is independently hydrogen, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, Tributyl, pentyl, hexyl, or phenyl. 5. The epoxy resin composition according to item 4 of the scope of patent application, wherein each Ri is independently hydrogen, methyl, third butyl, or phenyl. 6. The epoxy resin composition as described in item 1 of the scope of the patent application, wherein each R2 is independently a hydrogen 'Cl-6 alkyl group', a Cl-6 cycloalkyl group, a G.6 dilute group, and a C2-6 alkyne , Phenyl, naphthyl, or phenyl or naphthyl substituted with Ci-6, C1-6 ring, C2-6 alkenyl, C2-6 alkynyl, _Continued pages (please note and use continuation pages when the patent application page is insufficient) .565577 Patent Application Continued 7. The epoxy resin as described in item 1 of the patent application; F sealing composition, wherein each R2 is independently hydrogen, methyl, ethyl, n-propyl, isopropyl, n Butyl, isobutyl, third butyl, n-pentyl, isopentyl, neopentyl, hexyl, phenyl, methylbenzyl, ethylphenyl, or naphthyl. 8. The cyclofluorene resin composition according to item 1 in the scope of the patent application, wherein each R2 is independently hydrogen, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, Tributyl, pentyl, hexyl, or phenyl. 9. The epoxy resin composition according to item 8 of the scope of the patent application, wherein each R2 is independently hydrogen, methyl, ethyl, n-propyl, or isopropyl. 10. The epoxy resin composition according to item 1 of the scope of the patent application, wherein R3 can be hydrogen, Cm alkyl, Cm cycloalkyl, Cm alkenyl, Cm alkynyl, phenyl, naphthyl, or Cm Alkyl, Cm cycloalkyl, Cm alkenyl, or C2-6 alkynyl substituted phenyl or naphthyl. 11. The epoxy resin composition as described in item 丨 of the patent application, wherein R3 may be hydrogen, methyl'ethyl, n-propyl, isopropyl, n-butyl, isobutyl, or tert-butyl Group, n-pentyl, isopentyl, neopentyl, hexyl, benzyl, methylbenzyl, ethylphenyl, or naphthyl. 12. The epoxy resin composition as described in item i of the patent application scope, in which R3 can be hydrogen, * · * * \. · Continued pages (If the patent application page is insufficient, please note and use the continuation page ) 565577 Patent Application Continued on page Methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, third butyl, pentyl, hexyl, or benzyl. 13. The epoxy resin composition according to item 1 of the scope of patent application, wherein each R4 is independently hydrogen, Cm alkyl, Cm cycloalkyl, G-6 alkenyl, C2-6 alkynyl, phenyl , Naphthyl, or phenyl or naphthyl substituted with (^ 6 alkyl, G-0 cycloalkyl, C2-6 alkenyl, or Cm alkynyl. 14. Rings as described in item 1 of the scope of patent application Oxygen resin composition in which each p is independently hydrogen, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, third butyl, n-pentyl, isopentyl, neo Amyl, hexyl, benzyl, methylbenzyl, ethylphenyl, or naphthyl 15. 15. The epoxy resin composition according to item 1 of the scope of patent application, wherein each R4 is independently hydrogen, methyl , Ethyl, n-propyl, isopropyl, n-butyl, isobutyl, third butyl, pentyl'hexyl, or phenyl. 16. The epoxy resin composition according to item 15 of the scope of patent application Each of R4 is independently hydrogen, or a phenyl group. Π · The epoxy resin composition as described in item 1 of the scope of patent application, wherein the various epoxy resins (A) may be para-position, para-position , (P, p,-) or adjacent, (〇, 〇, —). 18. The epoxy resin composition as described in item 1 of the scope of patent application, wherein the hope epoxy resin (A) is selected from the following page (scope of patent application) When the page is insufficient, please note and use the continuation page) Formed by the ethnic group. 19. The epoxy resin composition according to item 1 of the scope of application for a patent, wherein the phenolic epoxy handle * monthly (A) accounts for 1 to 30% of the total epoxy resin. 20. The epoxy resin composition according to item 19 of the scope of application for a patent, wherein the phenolic epoxy resin (A) accounts for * to 90 wt% of all epoxy resins. □ Continued pages (If the patent application page is insufficient, please note and use the continuation page) 6 _ Continuation pages (If the patent application page is insufficient, please note and use the continuation page)