TW570940B - Epoxy resin composition, prepreg and metal-clad laminate - Google Patents

Abstract

An epoxy resin composition of the invention comprises: an epoxy resin; a hardening agent; and a phenol-modified polyphenylene oxide having a number average molecular weight of 1000 to 4000, which is prepared by carried out a redistribution reaction between a polyphenylene oxide and a phenol compound in the presence of a reaction initiator which can be decomposed to generate an alcohol, a prepreg and a metal-clad laminate of the invention contain the epoxy resin composition.

Description

570940 V. Description of the invention 0) Field of the invention The present invention relates to a cyclic stalk composition containing an epoxy resin and a phenol-modified polyphenylene ether. The phenol-modified polyphenylene ether is passed through a reaction initiator. Redistribution reaction between polyphenylene ether and phenolic compounds in the presence of modifiers and additives = preparation, and more specifically, the present invention relates to the use of The epoxy composition of the material of the board should not be used with the prepregs and metal-clad laminates of this composition. Man Fu _ background

The oxygen-expanding resin composition is widely used as a material for preparing an insulating board such as a printed wiring board. As the degree of integration of electronic parts such as semiconductors increases, it is known to be proposed by, for example, Japanese Laid-Open Patent "· 29 1 1 48/1 9 97

The epoxy resin composition containing epoxy resin and phenol-modified polyphenylene ether is a material for an insulating plate having excellent high-frequency properties, such as excellent dielectric constant and high glass transition temperature. The polyphenylene ether is prepared by redistribution reaction between polyphenylene ether and a phenol compound in the presence of a reaction initiator and a hardener, and has a number average molecular weight ranging from 0 0 0 to 3 0 0 . The modified polyphenylene ether is prepared by redistribution of a polymer polyphenylene ether having a number average molecular weight of 100,000 to 3,000, so that the number average molecular weight is reduced to 1,000 to 3,000. This redistribution reaction sometimes results in a less reactive modified polybenzene test by reaction with a reaction initiator. The presence of such less reactive modified polybenzene scales can cause fluctuations in the quality of the products made from them. Therefore, it is desired to improve the reactivity of the epoxy resin composition. In addition, with the recent increase in demand for miniaturization, there will be

C: \ 2D-OODE \ 90-10 \ 90118292.ptd Page 5 570940 V. Description of the invention (2) The printed wiring board with the oxygen-oxygen resin composition 1 When forming a printed wiring board, it is necessary to have: :the trend of. Materials that have a lower coefficient of expansion, or materials that have a lower coefficient of expansion, are related to each other in the related applications. Gg ',,,' 工 ',,, and processing. This application is based on the application 2000-224994A filed on July 26, 2000 ^ ^ Japanese Patent Application Invention No. 94, which is incorporated herein by reference. The present invention has been developed in view of the foregoing situation, and includes a highly reactive epoxy resin, an impregnated product, and a metal coating. The present invention provides an epoxy resin composition which can provide an excellent metal coating laminate. Xiao Zhuan private / Dian Shun Ben Ting provides an epoxy resin composition that can provide a metal clad back layer 5 with a lower expansion coefficient. w Furthermore, the present invention provides an epoxy resin composition that can provide a metal-clad laminate that can achieve a lower dielectric constant and a lower dielectric loss tangent. As a result of intensive research to achieve the purpose of the invention, the present inventors have discovered that the composition of the epoxy resin can be improved by using a specific reaction initiator such as a compound represented by the chemical formula (1), (2), or (3) Reaction of metals and metal-clad laminates prepared from an epoxy resin composition containing an age-modified polyphenylene ether prepared by using this reaction initiator as a component, which has excellent glass The transition temperature, and the lower the coefficient of expansion and the lower dielectric properties, the present invention has been completed based on this finding. this

C: \ 2D-CODE \ 90-10 \ 90118292.ptd Page 6 570940 V. Explanation of the invention (3) In addition, as a result of further research, the inventor found that by using a special reaction initiator, such as by the chemical formula (1 ), Produced by redistribution in the presence of a compound represented by), (2) or (3), and a phenol-modified polyphenylene ether having a number average molecular weight of less than 4,000 does not cause it The performance of the prepared printed wiring board was deteriorated, and therefore the present invention was completed based on this finding. In addition, the number average molecular weight of the phenol-modified polyphenylene ether used herein refers to a molecular weight measured by measuring a molecular weight distribution using gel permeation chromatography. The present invention includes the following results. (1) An epoxy resin composition, including: a soil oxygen resin; a hardener; and a phenol-modified polybenzene scale having a number average molecular weight of 1,000 to 4000, which is initiated by a reaction that decomposes to produce alcohol Presence of the agent is prepared by redistribution reaction between polyphenylene ether and phenolic compound. Λ (2) The epoxy resin composition as described in the item (1), wherein the alcohol is an aliphatic alcohol. 'Where (3) The epoxy resin composition as described in item (1) or (2) The alcohol has a boiling point of 150 ° C or below. The compound shown is the epoxy resin composition as described in any one of items (1) to (3), in which the Haihai reaction initiator is represented by chemical formula (1) Table R-0-0-R '("where R and R 'are the same or different, and each represents an alkyl group

C: \ 2D-C0DE \ 90 · 10 \ 90118292.ptd Page 7 570940 V. Description of the invention (4) (5) The composition of the epoxy resin as described in any one of item (JU), (3) The reaction initiators are compounds represented by the chemical formula (2). 0 (2) where "" is the same or different, and each of them represents an alkyl group. 乂 6 As described in the ring of item (5) An oxygen resin composition, wherein the reaction initiator represented by the chemical formula (2) is propyl peroxide monobutyl carbonate. (7) As described in any one of the items (1) to (3) Item of the epoxy resin composition, wherein the reaction initiator is a compound represented by the chemical formula (3):

Where R1 represents alkyl and R2 represents CH3 or 11. (8) The epoxy resin composition as described in any one of items (1) to (7), wherein the redistribution reaction is performed in the presence of a catalyst and a reaction initiator. (9) The epoxy resin composition as described in the item (8), wherein the catalyst is cyclic burning acid. (1 0) The epoxy resin composition as described in the item (8), wherein the catalyst

W312 \ 2d-code \ 90-10 \ 90118292.ptd Page 8 570940 V. Description of the invention (5) ----- ί 3 :) Mother 10 ° seriously injured! The polyphenylene ether contains ° · ° 01 to ° · 01 parts by weight of a pre-impregnated product, which is based on the following steps: The substrate is described in any one of (1) to (10) Forming the product; and semi-hardening the epoxy resin composition. , <S know, and (ιί; 2 items, including metal falling and metal coating laminates described in item t? (12), Gongming t? (12), where: Preί: Xiί% ^ The resin composition is hardened by ☆ heat-pressing the prepreg product and the metal after it has been re-embedded. King system ^ 丄: Polyphenylene ether of Gabe is coated by using the aforementioned reaction initiator, so it has less residue. The unreacted material. Therefore, the metal coating layer has an excellent glass transition temperature and exhibits a lower coefficient of expansion: a lower dielectric constant and a lower dielectric loss tangent. Detailed description of the invention 昍 ^ ^ The first specific example of the epoxy resin composition of the present invention is illustrated. The resin composition includes epoxy resin and age-modified polyphenylene ether having a number average molecular weight of 1,000 to 4,000 ( Polyphenylene scale modified with phenolic compounds) 'This age-modified polyphenylene ether was prepared by conducting a redistribution reaction between polyphenylene ether and ageing compounds in the presence of a reaction initiator and a hardener. The phenol-modified polyphenylene ether used in the epoxy resin composition can be made to have 10,000 30,000 number average molecular weight of the high molecular weight polyphenylene ether redistribution reaction to carry out 'thus the number average molecular weight reduced to 4〇〇〇 and 1〇〇〇

C: \ 2D-C0DE \ 90-10 \ 90118292.ptd $ 9 pages 570940 V. Description of invention (6) Manufactured. If the number-average molecular weight of the phenol-modified polyphenylene ether is less than 1,000, a metal-clad laminate having deteriorated heat resistance properties will be produced, and if it is more than 400,000, a manifestation will occur. Pre-impregnated products with a relatively high melt viscosity, so that it may be difficult to make metal-clad laminates by adhesion defects of pre-impregnated products. The phenol-modified polyphenylene ether has a better number average molecular weight of 100 to 300. The redistribution reaction (decomposition and recombination reaction) of the invention refers to the reaction of a lower molecular weight polyphenylene ether with a higher molecular weight via a terminal reaction of a higher molecular weight polyphenylene with a desired compound under the reaction. Contrary to the phenol compounds used in redistribution reactions, and the aging compounds are better, and they include bisphenol or sulfonic acid. 々77 beno lacquer (novolak) In the case of using bisphenol A as a phenol compound, take # to heat until melted, and then add a reaction initiator to cause ♦ Hachimoto scales and double-age A fruit to obtain a phenol modified polymer Phenyl ether. Regarding the bisphenol A, the knife reaction, the weight of the polyphenylene ether contains i to 10 parts by weight. The proper amount :::: The reaction initiator used in the redistribution reaction per 100 is the stomach. Decomposes to produce alcohol compounds. This alcohol is at 200. The redistribution reaction evaporates, so it hardly remains in the final product or below at a temperature of 150 t: or less, more preferably ⑽ to less than the boiling point of the aliphatic alcohol. · Hands, for example, when using decomposable in redistribution reaction, but not containing hair agent (for example, over-gasified benzyl alcohol), the reaction bow in the reaction

570940

V. Description of the invention (7) It has a south boiling point, and it is not easy to evaporate when the epoxy resin composition is heated in the post-treatment. For example, the decomposition products of phenylhydrazone (ie, benzoic acid, acid) have a boiling point of about 249 ° C. Therefore, in the hardening reaction of the epoxy resin composition, the decomposition product reacts with the epoxy group of the epoxy resin. As a result, the crosslinking properties and reactivity of the oxygen-generating resin are deteriorated, and the crosslinking density is reduced. In contrast, when a reaction initiator capable of decomposing and generating $ in a redistribution reaction is used as in the present invention, this alcohol can be easily evaporated when the epoxy resin composition is heated in a post-treatment. As a result, the crosslinking properties of the epoxy resin are not deteriorated, the reactivity of the epoxy resin is improved, and the crosslinking density is increased. Regarding the reaction initiator, a compound represented by the chemical formula (1), a compound represented by the chemical formula ⑺, and a compound represented by the chemical formula (3) are taken as examples, which are more preferable than the carbon atoms. In the following chemical formulas (1) to (3) obtained by using a lower amount of peroxy isopropanol as the resin, the alkyl group of R, R ', Ri &amp; R3 is an alkyl group having 1 to 12 atoms. More preferably, from 3 to 6 carbon atoms. The cloth reaction is in the presence of a reaction initiator and a catalyst. A specific example of the reaction initiator represented by formula (2) is a third butyl peroxide monobutyl carbonate represented by X in formula (j). In the case of the second butyl monocarbonate, a second butyl shovel is produced. However, due to this morphology: matter: phase, eruption, it will not remain in the final product, and therefore unreacted material. The use of phenol-modified polyphenylene ether can improve the reactivity of the product and increase the glass transition temperature of the coating laminate made of the resin composition and the coating layer composition.

570940 V. Description of the invention (8)

〒H3 9? H3 H3C——c—ο—0—-c—〇—CH ⑷ ch3 CH3 reaction initiator in redistribution reaction is produced per 100 parts by weight ~ contains 1 to 10 parts by weight Amount mixing is better. + 笨 _ Regarding the catalyst used in the redistribution reaction, organic metal salts of alkanoic acid, stearic acid, and acetic acid can be taken as examples. Preferred metals are such as rings Co, Mn, and Zn. Preferred examples of the catalyst include manganese stearate, and vinegar includes cobalt naphthenate. The catalyst is more preferably cobalt naphthenate. This catalyst contains 0.001 to 0.001 parts per 100 parts by weight of polyphenylene ether in the catalyst and the reaction mixture, and is preferably mixed in the opposite amount. 77 In addition, polyphenylene ether modified with novolac as a phenol compound. It is prepared by heating the polyphenylene ether and various varnishes to melt, and then applying a reaction initiator therein to cause a redistribution reaction. Regarding the ^ re ^ $ in the reaction, the acid varnish is appropriately mixed in an amount of 5 to 10 parts by weight per 100 parts by weight of polyphenylene oxide. As for the reaction initiator, the same ones as described above can be used. The reaction initiator is preferably used in the same amount as described above. The redistribution reaction for producing the modified polyphenylene ether is performed, for example, under the following conditions. That is, an organic solvent such as benzene, benzene, or dibenzobenzene is used, and a polyphenylene compound, a phenol compound such as bisphenol A and novolac, and a reaction initiator are added to the solvent, and stirred at 80 to 100 艽. Heat 10 to f〇〇

570940

minute. The epoxy resin used in the epoxy resin composition is used for preparing the metal-clad laminate epoxy resin. Example = epoxy resin, let-varnish ring, "” m self-type epoxy resin, internal urea type epoxy resin, aliphatic epoxy? Funnel benzene epoxy resin, multifunctional epoxy Resins, and epoxy resins obtained by bromination of isocyclic emulsion resins. The epoxy resin composition contains 40 to 7 per 100 parts by weight of the total amount of modified polyphenylene ether and epoxy resin. 0 parts by weight of the epoxy resin is preferred. Regarding the hardener used in the epoxy resin composition, it includes amine-type hardeners such as diaminodiphenylmethane, m-phenylenediamine, and triethylene glycol. Amine, ammonia, triethylamine, and diethylamine. Epoxy resin composition is modified at a weight of 1,000 parts by weight? The sum of epoxy resin and epoxy resin contains 1 to 5 parts by weight of hardening in a preferred amount In order to accelerate the hardening reaction, a hardening accelerator may be practically added to the epoxy resin composition. As for the hardening accelerator, it includes, for example, Weijun, such as 2-methylimidazole, 2-ethyl-4-methyl Imidazole and 2-phenylimidazole, and a tertiary amine such as 1,8-diazine bicyclic [5.4.0. 7-undecene, triethylene glycol And benzyldiamine. The epoxy resin composition contains a hardening accelerator in an amount of 0.1 to 1 part by weight per 100 parts by weight of the modified polyphenylene ether and epoxy resin. Next, the second specific example of the epoxy resin composition of the present invention will be described below.

\\ 312 \ 2d-code \ 90-10 \ 90118292.ptd Page 13 570940 V. Description of the invention (ίο) Only the differences of the aforementioned epoxy resin composition will be described. The epoxy resin composition includes a phenol having a number-average molecular weight of 100 to 4,000, which is prepared by redistribution reaction between polyphenylene ether and an age compound in the presence of a reaction initiator. The modified polyphenylene ether and the reaction initiator used in the redistribution reaction are compounds represented by the above chemical formula (3).

The specific reaction initiator represented by the chemical formula (3) is represented by the following chemical formula (5): 1, bis (third hexyl peroxide) —3, 3, 5—trimethylcyclohexane. When this 1,: 1-bis (third hexyl peroxide) -3,3,5-trimethylcyclohexane is used ', 2-methyl-2-pentanol is produced. Since this 2-fluorenyl-2-pentanol is an alcohol having a boiling point of 121 ° C and evaporated at a relatively low temperature, it does not remain in the final product, so a small amount of Unreacted component 0

H CH3 ch3 I ^ H3C-H2C-H2C-C-〇-〇 · (5) ch3 ch3 h3c-h2c-h2c-co-σ ch3 Use of the reaction initiator represented by the above formula (3) can improve the epoxy resin The reactivity of the composition is as follows: the glass transition temperature of the metal-clad laminate using this soil-rolling resin composition with M, ^ ^, and k. As explained in the foregoing, the present day # 明 之 j 泪 虫 resin composition contains in the presence of the name: &amp; special reaction initiator (with the above and ^, take the initial dagger 3 ^ © in the special compound is better) (2) or (3) The phenol-modified polymer produced by the re-knife reaction

C: \ 2D-CODE \ 90-10 \ 90li8292.ptd Page 14 570940 _-_ V. Description of the invention (11) Benzene, which means that the% oxygen resin composition shows high reactivity. "The pre-impregnated product of Γ is prepared by immersing the substrate in the epoxy tree tincture of the present invention, and scooping the cup and semi-hardening the epoxy resin composition. About the base, n ^ ^ # 破 璃 基Materials, such as broken glass fiber cloth and glass non-woven cloth. Pre-impregnation: _ By, for example, immersing the substrate in the warp ::

The diluted epoxy resin is thin and thin, and it is made so that it is impregnated, and then it is heated at 80 ° C to 180 ° C. (: It is prepared by adding semi-hardened composition at the temperature. There is no particular limitation on the amount of the tree used for impregnating the substrate, but it contains the pre-impregnated sigma σ, For the earth material, it is better that the resin content after drying is 30 to 70% by weight based on the replacement of the pre-two coat. From the viewpoint of stability and better properties of the laminate, it will come to an end * 3 / Again When the epoxy resin composition is maintained at 25.0 to 50, the metal coating laminate of the present invention includes a metal product, wherein the epoxy resin composition is hardened. 2: In the pre -... , Pre-impregnated. Medium s $ X month metal package impregnated products and all genus ;: Resin composition is made by pre-pressing / pre-coating. Mouth and thermally pressurized after the mooring ^ a predetermined number of The prepared prepreg and materials such as the material to be pressurized, and then the material is hot metal overlapped, which is a coating laminate. Specific examples of metal foil include two, and gold polyphenylene ether is prepared. , The cross-linking of epoxy resin and hardener, and aluminum alloy. The modification can be carried out considering the type of hardener, It depends on the reaction temperature of the hardening agent and the temperature hardener of the W. The pressure is mainly dependent on the conditions of the 2 conditions, so that the positive pressure does not remain in the prepared metal coating laminate and does not remain Gas, bubble. Heat plus 1 C: \ 2D- ®DE \ 90-10 \ 90118292.ptd Page 15 570940 V. Description of the invention (12) The conditions can be placed in the right column / 'to 6 liver a and time: 10 minutes ^ Vy (temperature: 50 to 300 t, the house is Λ to 20 minutes due to the metal coating). 1 The prepared warp contains a specific inverse "low expansion coefficient, car;!;! Better The glass transition temperature, obtained, will now pass through Quan Zhaoxin: the number of electric hangs and the lower dielectric loss tangent. The solution is more detailed than any other way to illustrate the present invention, 'However, Ding Ba explained In order to limit the present invention. No, (experiment using reaction-induced experiments) Knife cloth reaction and quantity of flat molecules are carried out in the preparation of phenol-modified polyphenylene ethers. The average number of products: the average molecular weight of the polyphenylene oxide of the hair seed type: 2_.) Γ part under the cone ^ "part") "inverse to Table 1) The initiator and 70 parts of γ-benzene as a solvent, the predetermined amount = downward ^ redistribution reaction for 90 minutes. Use chemical and 90 oxidation of the second butyl monocarbonate, chemical _, not the third peroxide Hexyl) -3,3,5-trimethylcyclohexane, not bis (expressed by (6), ι — bis (peroxidation of chemical formula represented by formula (7)) The third butyl peroxyformate is reacted by diisopropyl peroxide represented by the chemical formula (8), the following is expressed by di-third butyl oxide, and the basic iso-emulsified lice by isopropyl isopropyl Initiator. Measured by reaction using gel permeation [HLC-8120; manufactured by TOSOH Corporation] 9: ^ C: \ 2D-C0DE \ 90-10 \ 90118292.ptd Page 16 570940 V. Description of the invention (13) Number average molecular weight. In Table 1, the term "unreacted substance" means a compound having a number average molecular weight of 10,000 or more. The half-life decomposition temperature (1 hour half-life decomposition temperature) refers to the reaction temperature at which the reaction initiator is reduced to half under one hour of reaction. ❿

C: \ 2D-CODE \ 90-10 \ 90118292.ptd Page 17 570940 V. Description of the invention (14) 3C Η Η

⑹

H3C one I 〇 i 丨 〇 H3h3

H3C

⑼ H 〇3-03 H 1 H c—c—c C: \ 2D-C0DE \ 90-10 \ 90118292.ptd Page 18 570940 V. Description of the invention (15) ❿ Table 1 Types of reaction initiators Periodic decomposition temperature (1 hour) Amount (parts) of molecular weight reaction initiator The ratio of the number-average molecular weight unreacted substance is given by chemical formula (4) 118.4. . 176.2 1.1 1300 9 Use 0.01 parts of cobalt naphthenate as catalyst Chemical formula (5) 1 0 6.4 ° C 3 5 8.6 2.5 1320 12 Chemical formula (6) 1 0 2.4 ° C 274.4 1.9 1320 13 Chemical formula (7) 1 2 4.7 ° C 194.2 1.2 1320 40 Chemical formula (8) 1 3 5.7 ° C 270.4 1.7 1 0000 Almost unreacted chemical formula (9) 1 4 4.1 ° C 146.2 0.9 20000 Almost unreacted chemical formula (10) 1 8 8.2 ° C 152.2 1.. 1 1 8000 almost unreacted C: \ 2D-CODE \ 90-10 \ 90118292.ptd Page 19 570940 V. Description of the invention (22)

Example 1 Example 2 Example 3 Comparative Example 1 Comparative Example 2 Comparative Example 3 Reaction initiator Chemical formula (4) Chemical formula (4) Chemical formula (5) BPO Chemical formula (4) Chemical formula (4) Number average molecular weight 1900 3260 2900 3000 890 8600 Reactivity (%) 98 97 98 96 93 72 Tg (° C) 172 175 170 160 160-a (ppm) 58 62 60 62 67-Specific permittivity (1 MHz) 3.75 3.73 3.95 3.85 Dielectric loss Tangent (1 MHz) 0.0057 0.0050 0.0090 0.0065 Heat resistance AAAB at 250 ° C Heat resistance ABAB at 260 ° C Table 2 Chemical formula (4): Third butyl peroxide monopropyl carbonate Chemical formula (5): 1-bis (Third hexyl peroxide) -3, 3, 5 -trimethylcyclohexane

C: \ 2D-C0DE \ 9 (M0 \ 90118292.ptd page 26 570940 V. Description of the invention (23) The result is not good. The glass obtained in the examples in the examples has a low conversion to coating layer laminate In the presence of the present invention, a high-reflection glass transition temperature laminate is achieved. 2 ^ / π: The reactivity to mid-range is higher than that in the comparative example, which is a high coat. 1 @ θ # The metal-clad laminates appear to be better than Comparing the actual results, the better thermal expansion coefficient (α) of the laminate and the better appearance than df; the dielectric properties of gold obtained in Examples 1 and 2. b is better than that of yoke examples 1 and 2. Metal clad

Epoxy resin compositions are prepared using M-distribution reactions based on the suitability of specific reaction initiators. In addition, I ^ and phenol-modified polyphenylene ether are prepared. Therefore, i. The lower face ^ milk resin composition provides a metal coating with a better L car low, coefficient and lower dielectric properties. The impregnated product is controlled by the redistribution reaction in the presence of 9. It is composed of an epoxy resin composition containing a special reaction initiator. Γ, the phenyl-modified polyphenylene ether has a better glass transfer. The temperature, ^ 'therefore allows us to make a coating layer. -^ Coefficient of Coefficient and Gold with Lower Dielectric Properties The redistribution reaction in the presence of the metal-clad hair-forming agent of the present invention consists of an epoxy resin containing one component by a specific reaction: prepared by jf Phenol modified polyphenylene ether

Therefore, it has a better glass transition temperature prepreg because of its properties. &amp; Low specific expansion coefficient and lower dielectrics know specific examples of it, but the spirit and scope of which &gt; Although the present invention has been described in detail and it will be understood by those skilled in the art that various changes can be made without departing from it and modify.

C: \ 2D-CODE \ 90_10 \ 901i8292.ptd 苐 Page 27 570940

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Claims (1)

570940 I 々i Patent Application Circle A · ^ JL Month Amendment 92. I. 30 Replacement 1. An epoxy resin composition comprising: a bisphenol A epoxy resin or a resin containing brominated epoxy resin Epoxy-monoamine-type hardener; and a phenol-modified polyphenylene ether having a number average molecular weight of 1000 to 4000, in the presence of a reaction initiator capable of decomposing to produce an alcohol It is prepared by redistribution reaction between polyphenylene ether and phenolic compound. The epoxy resin composition contains 40 to 70 per 100 parts by weight of the total amount of modified polyphenylene ether and epoxy resin. Parts by weight of epoxy resin and 1 to 5 parts by weight of hardener. 2. The epoxy resin composition according to item 1 of the application, wherein the alcohol is an aliphatic alcohol. 3. The epoxy resin composition according to item 1 of the patent application scope, wherein the alcohol has a boiling point of 150 ° C or below. 4. For example, the epoxy resin composition of the scope of patent application, wherein the reaction initiator is a compound represented by the chemical formula (1): R-0-0-R, (1) where R and R 'are the same Or different, and each of them represents an alkyl group having 1 to 12 carbon atoms. 5. The epoxy resin composition according to item 1 of the patent application range, wherein the reaction initiator is a compound represented by the chemical formula (2): 〇 ⑺ R3-0-0-C-0-R4 c: \ General file of patent cases \ 9〇 \ 9〇118292 \ 9〇1! 8292 (replace w.ptc, page 29, 570940, case number 90118292, amended), the scope of patent application where R3 and R4 are the same or different, And each of them represents an alkyl group having 1 to 12 carbon atoms. 6. The epoxy resin composition according to item 5 of the patent application scope, wherein the reaction initiator represented by the chemical formula (2) is a peroxide group. The purpose of tributyl propylene carbonate S. 7. The epoxy resin composition according to item 1 of the patent application scope, wherein the reaction initiator is a compound represented by the chemical formula (3): —〇〇〇R1—〇〇〇 HR2 (3) wherein R1 represents an alkyl group having 1 to 12 carbon atoms, and R2 represents CH3 or 11. 8. The epoxy resin composition according to item 1 of the application, wherein the redistribution reaction is performed in the presence of a catalyst and a reaction initiator. 9. For example, the bad emulsion resin composition 5 in the scope of the patent application, 5 of which the catalyst is cobalt naphthenate. 1 〇. The epoxy resin composition according to item 8 of the scope of the patent application, wherein the catalyst is mixed in an amount of 0.00 1 to 0.01 parts by weight per 100 parts by weight of polyphenylene ether. . 11. A pre-impregnated product, which is prepared by the following steps: impregnating a substrate with an epoxy resin composition as described in claim 1; and C: \ Master File of Patent Cases \ 90 \ 90118292 \ 90118292 (Replacement)-2.ptc Page 30 570940 Case No. 90118292 C: \ Master File of Patent Cases \ 90 \ 90118292 \ 90118292 (Replacement) -2.ptc Page 31