Resin composition

Abstract

To provide a resin composition which contains an epoxy resin and a resin containing a radically-polymerizable unsaturated group and an alkylene oxide structure in combination, and enables production of a cured product excellent in chemical resistance.SOLUTION: A resin composition contains (A) an epoxy resin, (B) a resin containing a radically-polymerizable unsaturated group and an alkylene oxide structure, (C) a curing agent, and (D) two or more kinds of silane coupling agents, wherein the amount of the component (A) is larger than 100 wt.% of the total of the component (B) and the component (C) by 100 mass%.SELECTED DRAWING: Figure 1

Description

[Technical Field]

[0001] The present invention relates to a resin composition. More specifically, the present invention relates to a resin composition, and a cured product, a resin sheet, a circuit board, and a semiconductor device obtained using the resin composition. [Background technology]

[0002] A cured layer may be formed on a circuit board such as a semiconductor chip package by curing a resin composition. These cured layers can be used as sealing layers or insulating layers. Patent Document 1 proposes a resin composition for forming such a cured layer, which comprises an epoxy resin, a resin containing a combination of a radically polymerizable unsaturated group and an alkylene oxide structure, and a silane coupling agent. [Prior art documents] [Patent documents]

[0003] [Patent Document 1] Patent Publication No. 2021-195540 Summary of the Invention [Problem to be solved by the invention]

[0004] To improve the properties of a cured product layer, two or more types of silane coupling agents may be used. However, the inventors have found that when a resin composition containing an epoxy resin, a resin containing a combination of a radically polymerizable unsaturated group and an alkylene oxide structure, and two or more types of silane coupling agents is used, the resulting cured product tends to have poor chemical resistance. Specifically, the cured product of the resin composition tends to have poor resistance to alkaline solutions.

[0005] The present invention has been made in view of the above-mentioned problems, and aims to provide a resin composition which contains an epoxy resin, a resin containing a combination of a radically polymerizable unsaturated group and an alkylene oxide structure, and two or more types of silane coupling agents, and which is capable of giving a cured product having excellent chemical resistance; a resin sheet containing the resin composition; a cured product of the resin composition; a circuit board including the cured product and a method for producing the same; and a semiconductor device including the circuit board. [Means for solving the problem]

[0006] The present inventors have conducted extensive research to solve the above-mentioned problems, and as a result, have found that the above-mentioned problems can be solved by a resin composition comprising (A) an epoxy resin, (B) a resin containing a radically polymerizable unsaturated group and an alkylene oxide structure, (C) a curing agent, and two or more (D) silane coupling agents, in which the amount of component (A) is greater than the total amount of components (B) and (C), and have thus completed the present invention. That is, the present invention includes the following:

[0007] <1> A resin composition comprising (A) an epoxy resin, (B) a resin containing a radically polymerizable unsaturated group and an alkylene oxide structure, (C) a curing agent, and two or more types of (D) silane coupling agents, A resin composition in which the amount of component (A) is more than 100% by mass, relative to 100% by mass of the total of components (B) and (C). <2> the ratio of the number of active groups in component (C) to the number of epoxy groups in component (A) is 0.35 or less; <1> The resin composition according to claim 1. <3> (E) containing an inorganic filler; <1> or <2> The resin composition according to claim 1. <4> The amount of component (E) is 50% by mass or more relative to 100% by mass of the nonvolatile components of the resin composition. <3> The resin composition according to claim 1. <5> The amount of the (D) component is 2% by mass or more relative to 100% by mass of the (B) component. <1> ~ <4> The resin composition according to any one of claims 1 to 10. <6> The amount of the (D) component is 1% by mass or more relative to 100% by mass of the (C) component. <1> ~ <5> The resin composition according to any one of claims 1 to 10. <7> For forming an insulating layer or a sealing layer, <1> ~ <6> The resin composition according to any one of claims 1 to 10. <8> For forming a cured layer by compression molding, <1> ~ <7> The resin composition according to any one of claims 1 to 10. <9> A support and a resin composition layer provided on the support, The resin composition layer is <1> ~ <8> A resin sheet comprising the resin composition according to any one of claims 1 to 4. <10> <1> ~ <8> A cured product of the resin composition according to any one of claims 1 to 4. <11> <1> ~ <8> A circuit board comprising a cured product of the resin composition according to any one of claims 1 to 4. <12> <11> A semiconductor device comprising the circuit board according to claim 1. <13> <1> ~ <8> Step (I) of forming a resin composition layer containing the resin composition according to any one of the above; a step (II) of curing the resin composition layer; A method for manufacturing a circuit board, comprising: <14> The step (I) includes forming a resin composition layer by a compression molding method. <13> A method for manufacturing the circuit board according to claim 1. [Effects of the Invention]

[0008] According to the present invention, there can be provided a resin composition comprising an epoxy resin, a resin containing a combination of a radically polymerizable unsaturated group and an alkylene oxide structure, and two or more types of silane coupling agents, and capable of giving a cured product having excellent chemical resistance; a resin sheet comprising the resin composition; a cured product of the resin composition; a circuit board comprising the cured product and a method for producing the same; and a semiconductor device comprising the circuit board. [Brief explanation of the drawings]

[0009] [Figure 1] FIG. 1 is a cross-sectional view schematically showing a semiconductor chip package as a circuit board according to an embodiment of the present invention. DETAILED DESCRIPTION OF THE INVENTION

[0010] The present invention will be described in detail below with reference to embodiments and examples. However, the present invention is not limited to the following embodiments and examples, and can be implemented with any modifications within the scope of the claims and their equivalents.

[0011] As used herein, the term "optionally substituted" in reference to a compound or group means both a case where the hydrogen atoms of the compound or group are not substituted with substituents, and a case where some or all of the hydrogen atoms of the compound or group are substituted with substituents.

[0012] <Outline of Resin Composition> A resin composition according to one embodiment of the present invention comprises (A) an epoxy resin, (B) a resin containing a radically polymerizable unsaturated group and an alkylene oxide structure, (C) a curing agent, and two or more types of (D) silane coupling agents. In the following description, the "(B) resin containing a radically polymerizable unsaturated group and an alkylene oxide structure" may be referred to as the "(B) polymerizable alkylene oxide resin." In the resin composition according to this embodiment, the amount of the (A) epoxy resin is greater than 100% by mass, relative to the total of the (B) polymerizable alkylene oxide resin and the (C) curing agent (100% by mass).

[0013] This resin composition can provide a cured product with excellent chemical resistance, and typically can suppress the formation of flow marks.

[0014] <(A) Epoxy resin> The resin composition according to this embodiment contains an epoxy resin (A) as component (A). The epoxy resin (A) may be a curable resin having an epoxy group. The epoxy resin (A) may be used singly or in combination of two or more types. The resin composition according to this embodiment contains the epoxy resin (A) in an amount within a specific range.

[0015] Specifically, the amount of (A) epoxy resin is typically greater than 100% by mass, preferably at least 105% by mass, more preferably at least 110% by mass, and preferably at most 500% by mass, more preferably at most 400% by mass, and even more preferably at most 300% by mass, relative to 100% by mass of the total of (B) polymerizable alkylene oxide resin and (C) curing agent. When the amount of (A) epoxy resin is within this range, a cured product with excellent chemical resistance can be obtained, and the formation of flow marks can usually be suppressed.

[0016] Examples of (A) epoxy resins include bixylenol-type epoxy resins, bisphenol A-type epoxy resins, bisphenol F-type epoxy resins, bisphenol S-type epoxy resins, bisphenol AF-type epoxy resins, dicyclopentadiene-type epoxy resins, trisphenol-type epoxy resins, naphthol novolac-type epoxy resins, phenol novolac-type epoxy resins, tert-butyl-catechol-type epoxy resins, naphthalene-type epoxy resins, naphthol-type epoxy resins, anthracene-type epoxy resins, glycidylamine-type epoxy resins, glycidyl ester-type epoxy resins, cresol novolac-type epoxy resins, phenol aralkyl-type epoxy resins, biphenyl-type epoxy resins, linear aliphatic epoxy resins, epoxy resins having a butadiene structure, alicyclic epoxy resins, heterocyclic epoxy resins, spiro ring-containing epoxy resins, cyclohexane-type epoxy resins, cyclohexane dimethanol-type epoxy resins, naphthylene ether-type epoxy resins, trimethylol-type epoxy resins, tetraphenylethane-type epoxy resins, isocyanurate-type epoxy resins, and phenolphthalimidine-type epoxy resins.

[0017] From the viewpoint of obtaining a cured product having excellent heat resistance, the (A) epoxy resin preferably contains an epoxy resin having an aromatic structure. The aromatic structure is a chemical structure generally defined as aromatic, and also includes polycyclic aromatic rings and aromatic heterocycles. Examples of epoxy resins containing an aromatic structure include bisphenol A type epoxy resins, bisphenol F type epoxy resins, bisphenol S type epoxy resins, bisphenol AF type epoxy resins, dicyclopentadiene type epoxy resins, trisphenol type epoxy resins, naphthol novolac type epoxy resins, phenol novolac type epoxy resins, tert-butyl-catechol type epoxy resins, naphthalene type epoxy resins, naphthol type epoxy resins, anthracene type epoxy resins, bisxyleneol type epoxy resins, glycidylamine type epoxy resins having an aromatic structure, glycidyl ester type epoxy resins having an aromatic structure, cresol novolac type epoxy resins, biphenyl type epoxy resins, linear aliphatic epoxy resins having an aromatic structure, epoxy resins having a butadiene structure having an aromatic structure, alicyclic epoxy resins having an aromatic structure, heterocyclic epoxy resins, spiro ring-containing epoxy resins having an aromatic structure, cyclohexanedimethanol type epoxy resins having an aromatic structure, naphthylene ether type epoxy resins, trimethylol type epoxy resins having an aromatic structure, and tetraphenylethane type epoxy resins having an aromatic structure.

[0018] Among these, bisphenol A-type epoxy resins, naphthalene-type epoxy resins, and glycidylamine-type epoxy resins are preferred, and naphthalene-type epoxy resins and glycidylamine-type epoxy resins are more preferred. When these epoxy resins are used, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0019] The (A) epoxy resin preferably contains an epoxy resin having two or more epoxy groups per molecule, and the proportion of the epoxy resin having two or more epoxy groups per molecule relative to 100% by mass of the non-volatile components of the (A) epoxy resin is preferably 50% by mass or more, more preferably 60% by mass or more, and even more preferably 70% by mass or more.

[0020] (A) Epoxy resins include epoxy resins that are liquid at a temperature of 20°C (hereinafter sometimes referred to as "liquid epoxy resins") and epoxy resins that are solid at a temperature of 20°C (hereinafter sometimes referred to as "solid epoxy resins"). (A) Epoxy resins may contain only liquid epoxy resins, only solid epoxy resins, or a combination of liquid epoxy resins and solid epoxy resins. Of these, from the viewpoint of obtaining a resin composition that has excellent fluidity during compression molding, it is preferable that (A) epoxy resin contains a liquid epoxy resin.

[0021] The liquid epoxy resin is preferably a liquid epoxy resin having two or more epoxy groups in one molecule, and examples of the liquid epoxy resin include bisphenol A epoxy resin, bisphenol F epoxy resin, bisphenol AF epoxy resin, naphthalene epoxy resin, glycidyl ester epoxy resin, glycidyl amine epoxy resin, phenol novolac epoxy resin, alicyclic epoxy resin having an ester skeleton, cyclohexane epoxy resin, cyclohexanedimethanol epoxy resin, and epoxy resin having a butadiene structure; more preferably bisphenol A epoxy resin, naphthalene epoxy resin, and glycidyl amine epoxy resin.

[0022] Specific examples of liquid epoxy resins include "HP-4032", "HP-4032-D", and "HP-4032-SS" (naphthalene type epoxy resins) manufactured by DIC Corporation; "EXA-850CRP" (bisphenol A type epoxy resin) manufactured by DIC Corporation; "828US", "828EL", "jER828EL", "825", and "Epikote 828EL" (bisphenol A type epoxy resins) manufactured by Mitsubishi Chemical Corporation; "jER807" and "1750" (bisphenol F type epoxy resins) manufactured by Mitsubishi Chemical Corporation; "jER152" (phenol novolac type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "630", "630LSD", and "604" (glycidylamine type epoxy resins) manufactured by Mitsubishi Chemical Corporation; "ED-523T" (glycirol type epoxy resin) manufactured by ADEKA Corporation; Examples of epoxy resins include EP-3950L and EP-3980S (glycidylamine type epoxy resins); ADEKA's EP-4088S (dicyclopentadiene type epoxy resin); Nippon Steel Chemical & Material's ZX1059 (a mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin); Nagase ChemteX's EX-721 (glycidyl ester type epoxy resin); Daicel's CELLOXIDE 2021P (alicyclic epoxy resin with an ester skeleton); Daicel's PB-3600, Nippon Soda's JP-100 and JP-200 (epoxy resins with a butadiene structure); and Nippon Steel Chemical & Material's ZX1658 and ZX1658GS (liquid 1,4-glycidylcyclohexane type epoxy resin).

[0023] The amount of the liquid epoxy resin is preferably 20% by mass or more, more preferably 30% by mass or more, and even more preferably 40% by mass or more, and preferably 90% by mass or less, more preferably 85% by mass or less, and even more preferably 80% by mass or less, based on 100% by mass of the resin components in the resin composition. Unless otherwise specified, the resin components in the resin composition refer to the non-volatile components in the resin composition excluding the inorganic filler (E) described below. When the inorganic filler (E) is surface-treated with a surface treatment agent, the surface treatment agent is classified as a resin component. Therefore, the resin components in the resin composition generally refer to the non-volatile components in the resin composition excluding the inorganic material particles contained in the inorganic filler (E) described below. Furthermore, unless otherwise specified, the non-volatile components in the resin composition refer to the components in the resin composition excluding the solvent. When the amount of the liquid epoxy resin is within the above range, the chemical resistance of the cured resin composition can be particularly improved, and the formation of flow marks can usually be effectively suppressed.

[0024] The solid epoxy resin is preferably a solid epoxy resin having three or more epoxy groups per molecule, and more preferably an aromatic solid epoxy resin having three or more epoxy groups per molecule.The solid epoxy resin is preferably a bixylenol type epoxy resin, a naphthalene type epoxy resin, a naphthalene type tetrafunctional epoxy resin, a naphthol novolac type epoxy resin, a cresol novolac type epoxy resin, a dicyclopentadiene type epoxy resin, a trisphenol type epoxy resin, a naphthol type epoxy resin, a biphenyl type epoxy resin, a naphthylene ether type epoxy resin, an anthracene type epoxy resin, a bisphenol A type epoxy resin, a bisphenol AF type epoxy resin, a phenol aralkyl type epoxy resin, a tetraphenylethane type epoxy resin, or a phenolphthalimidine type epoxy resin.

[0025] Specific examples of solid epoxy resins include DIC Corporation's "HP4032H" (naphthalene-type epoxy resin); DIC Corporation's "HP-4700" and "HP-4710" (naphthalene-type tetrafunctional epoxy resins); DIC Corporation's "N-690" (cresol novolac-type epoxy resin); DIC Corporation's "N-695" (cresol novolac-type epoxy resin); DIC Corporation's "HP-7200," "HP-7200HH," "HP-7200H," and "HP-7200L" (dicyclopentadiene-type epoxy resins); and DIC Corporation's "EXA-7311." "EXA-7311-G3", "EXA-7311-G4", "EXA-7311-G4S", "HP6000" (naphthylene ether type epoxy resin); "EPPN-502H" (trisphenol type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.; "NC7000L" (naphthol novolac type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.; "NC3000H", "NC3000", "NC3000L", "NC3000FH", "NC3100" (biphenyl type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.; "ESN475V", "ESN4" manufactured by Nippon Steel Chemical & Material Co., Ltd. 100V" (naphthalene-type epoxy resin); "ESN485" (naphthol-type epoxy resin) manufactured by Nippon Steel Chemical & Material Co., Ltd.; "ESN375" (dihydroxynaphthalene-type epoxy resin) manufactured by Nippon Steel Chemical & Material Co., Ltd.; "YX4000H", "YX4000", "YX4000HK", and "YL7890" (bixylenol-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "YL6121" (biphenyl-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "YX8800" (anthracene-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "Y" manufactured by Mitsubishi Chemical Corporation Examples include "X7700" (phenol aralkyl type epoxy resin); "PG-100" and "CG-500" manufactured by Osaka Gas Chemicals Co., Ltd.; "YX7760" (bisphenol AF type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "YL7800" (fluorene type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "jER1010" (bisphenol A type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "jER1031S" (tetraphenylethane type epoxy resin) manufactured by Mitsubishi Chemical Corporation; and "WHR991S" (phenolphthalimidine type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.

[0026] When the (A) epoxy resin contains a combination of a liquid epoxy resin and a solid epoxy resin, the mass ratio thereof (liquid epoxy resin:solid epoxy resin) is preferably 20:1 to 1:20, more preferably 10:1 to 1:10, and particularly preferably 7:1 to 1:7.

[0027] The epoxy equivalent of the (A) epoxy resin is preferably in the range of 50 g / eq to 5,000 g / eq, more preferably 60 g / eq to 3,000 g / eq, even more preferably 80 g / eq to 2,000 g / eq, and particularly preferably 110 g / eq to 1,000 g / eq. The epoxy equivalent represents the mass of the resin per equivalent of epoxy groups. This epoxy equivalent can be measured according to JIS K7236.

[0028] The weight average molecular weight (Mw) of the (A) epoxy resin is preferably in the range of 100 to 5,000, more preferably 250 to 3,000, and even more preferably 400 to 1,500. The weight average molecular weight can be measured by gel permeation chromatography (GPC) as a polystyrene-equivalent value.

[0029] The amount of (A) epoxy resin is preferably 3% by mass or more, more preferably 5% by mass or more, and even more preferably 8% by mass or more, relative to 100% by mass of the nonvolatile components in the resin composition, and is preferably 40% by mass or less, more preferably 30% by mass or less, and even more preferably 20% by mass or less. When the amount of (A) epoxy resin is within this range, the chemical resistance of the cured product of the resin composition can be particularly improved, and usually the formation of flow marks can be effectively suppressed.

[0030] The amount of (A) epoxy resin is preferably 20% by mass or more, more preferably 30% by mass or more, and even more preferably 40% by mass or more, relative to 100% by mass of the resin components in the resin composition, and is preferably 90% by mass or less, more preferably 85% by mass or less, and even more preferably 80% by mass or less. When the amount of (A) epoxy resin is within this range, the chemical resistance of the cured product of the resin composition can be particularly good, and further, the formation of flow marks can usually be effectively suppressed.

[0031] The range of the total amount of (A) epoxy resin, (B) polymerizable alkylene oxide resin, and (C) curing agent is, relative to 100% by mass of the resin components in the resin composition, preferably 70% by mass or more, more preferably 80% by mass or more, even more preferably 90% by mass or more, and preferably 99% by mass or less, more preferably 97% by mass or less, and even more preferably 95% by mass or less. When the total amount of (A) epoxy resin, (B) polymerizable alkylene oxide resin, and (C) curing agent is within the above range, the chemical resistance of the cured product of the resin composition can be particularly good, and further, the formation of flow marks can usually be effectively suppressed.

[0032] The total amount of (A) epoxy resin, (B) polymerizable alkylene oxide resin, (C) curing agent, and (D) silane coupling agent is preferably 70% by mass or more, more preferably 80% by mass or more, and even more preferably 90% by mass or more, and is preferably 99% by mass or less, more preferably 98% by mass or less, and even more preferably 97% by mass or less, based on 100% by mass of the resin components in the resin composition. When the total amount of (A) epoxy resin, (B) polymerizable alkylene oxide resin, (C) curing agent, and (D) silane coupling agent is within the above range, the chemical resistance of the cured product of the resin composition can be particularly good, and the formation of flow marks can usually be effectively suppressed.

[0033] <(B) Polymerizable alkylene oxide resin> The resin composition according to the present embodiment includes a (B) polymerizable alkylene oxide resin as component (B). The (B) polymerizable alkylene oxide resin contains a radically polymerizable unsaturated group and an alkylene oxide structure. The (B) polymerizable alkylene oxide resin can form bonds through a radical polymerization reaction, thereby curing the resin composition. A resin composition containing the (B) polymerizable alkylene oxide resin in combination with an (A) epoxy resin and a (C) curing agent typically suppresses warpage of a circuit board having a cured product of the resin composition, since the flexible alkylene oxide structure can relieve stress. However, conventionally, cured products of resin compositions containing a combination of components (A) to (C) tend to have poor chemical resistance and are prone to the formation of flow marks. In contrast, the resin composition according to the present embodiment can improve chemical resistance and typically suppress the formation of flow marks.

[0034] The radically polymerizable unsaturated group contained in the (B) polymerizable alkylene oxide resin is typically a group containing a radically polymerizable carbon-carbon unsaturated bond, such as a group containing an ethylenic carbon-carbon double bond. Specific examples of the radically polymerizable unsaturated group include vinyl, allyl, 1-butenyl, 2-butenyl, acryloyl, methacryloyl, fumaroyl, maleoyl, vinylphenyl, styryl, and cinnamoyl groups. Among these, the radically polymerizable unsaturated group is preferably an α,β-unsaturated carbonyl group, more preferably an acryloyl or methacryloyl group. The number of radically polymerizable unsaturated groups contained in the (B) polymerizable alkylene oxide resin may be one or two or more. The type of radically polymerizable unsaturated group contained in the (B) polymerizable alkylene oxide resin may be one or two or more. The polymerizable alkylene oxide resin (B) may have a radically polymerizable unsaturated group at its molecular terminal.

[0035] The alkylene oxide structure contained in the polymerizable alkylene oxide resin (B) is represented by the following formula (1).

[0036] [ka]

[0037] (In formula (1), R 1 represents an alkylene group which may have a substituent; * represents a bonding site.

[0038] In formula (1), R 1 represents an alkylene group which may have a substituent. The number of carbon atoms in this alkylene group is usually 1 or more, preferably 2 or more, and preferably 6 or less, more preferably 5 or less, even more preferably 4 or less, and even more preferably 3 or less. R 1 The number of carbon atoms in the alkylene group may be 2. Specific examples of the alkylene group include a methylene group, an ethylene group, a propylene group, a 1-methylmethylene group, a 1,1-dimethylmethylene group, a 1-methylethylene group, a 1,1-dimethylethylene group, a 1,2-dimethylethylene group, a butylene group, a 1-methylpropylene group, a 2-methylpropylene group, a pentylene group, and a hexylene group.

[0039] R 1 Examples of the substituent that the alkylene group may have include a halogen atom, a hydroxy group, an alkoxy group having 1 to 5 carbon atoms, an aryl group having 6 to 10 carbon atoms, an amino group (-NH2), a cyano group (-CN), a carboxy group (-COOH), an epoxy group, a nitro group (-NO 2) , formyl group (-CHO), -N(C 1-5 alkyl group)2, -C(O)OC 1-5 alkyl groups, etc. 1-5The term "alkyl group" refers to an alkyl group having 1 to 5 carbon atoms. Among these, epoxy group, hydroxy group, amino group, and carboxy group are preferred. These substituents may be reactive with (A) epoxy resin or (C) curing agent. In (B) polymerizable alkylene oxide resin having such reactive substituents, the substituents can react to form a crosslinked structure, so that a cured product having a high elastic modulus and excellent handleability can be obtained. In this specification, even if a resin has an epoxy group, a resin containing a radically polymerizable unsaturated group and an alkylene oxide structure is classified as (B) polymerizable alkylene oxide resin. The substituents may be used singly or in combination of two or more. However, when R 1 is particularly preferably an alkylene group having no substituent.

[0040] Specific examples of the alkylene oxide structure include an ethylene oxide structure (-C2H4O-), a propylene oxide structure (-C3H6O-), a butylene oxide structure (-C4H8O-), a pentylene oxide structure (-C5H 10 O-), hexylene oxide structure (-CH 12 Among these, the ethylene oxide structure and the propylene oxide structure are preferred, and the ethylene oxide structure is more preferred.

[0041] The number of alkylene oxide structures contained in the (B) polymerizable alkylene oxide resin may be one or two or more. It is particularly preferred that the (B) polymerizable alkylene oxide resin contains two or more alkylene oxide structures. When the (B) polymerizable alkylene oxide resin contains two or more alkylene oxide structures, the alkylene oxide structures may be the same or different. The number of alkylene oxide structures contained per molecule in the (B) polymerizable alkylene oxide resin is usually one or more, preferably two or more, and may be four or more, nine or more, ten or more, or eleven or more. The upper limit is preferably 101 or less, more preferably 90 or less, even more preferably 68 or less, and even more preferably 65 or less.

[0042] The polymerizable alkylene oxide resin (B) may contain a polyalkylene oxide structure in which two or more alkylene oxide structures are bonded in succession, as represented by the following formula (2).

[0043] [ka]

[0044] In formula (2), n represents an integer of 2 or more. The range of n may be the same as the range of the number of alkylene oxide structures per molecule contained in the polymerizable alkylene oxide resin (B) described above. 1 are each independently R in formula (1). 1 represents the same thing.

[0045] Specific examples of the polyalkylene oxide structure include polyethylene oxide structures (-(C2H4O) n -), polypropylene oxide structure (-(C3H6O) n -), polybutylene oxide structure (-(C4H8O) n -), poly(ethylene oxide-co-propylene oxide) structure, poly(ethylene oxide-ran-propylene oxide) structure, poly(ethylene oxide-alt-propylene oxide) structure, and poly(ethylene oxide-block-propylene oxide) structure. Among these, polyethylene oxide structure, polypropylene oxide structure, poly(ethylene oxide-co-propylene oxide) structure, poly(ethylene oxide-ran-propylene oxide) structure, poly(ethylene oxide-alt-propylene oxide) structure, and poly(ethylene oxide-block-propylene oxide) structure are preferred, polyethylene oxide structure and polypropylene oxide structure are more preferred, and polyethylene oxide structure is even more preferred.

[0046] Examples of the (B) polymerizable alkylene oxide resin include resins represented by the following formulas (B-1) to (B-3).

[0047] [ka]

[0048] In formula (B-1), R 1 are each independently R in formula (1). 1 In formula (B-1), R 2 each independently represents a hydrogen atom or an alkyl group having 1 to 6 carbon atoms, preferably a hydrogen atom or a methyl group. In formula (B-1), n1 represents an integer of 1 or greater. The range of n1 may be the same as the range of the number of alkylene oxide structures per molecule contained in the polymerizable alkylene oxide resin (B) described above.

[0049] In formula (B-1), R 3 represents a monovalent hydrocarbon group. 3 R may be an aliphatic hydrocarbon group or an aromatic hydrocarbon group. The aliphatic hydrocarbon group may be a saturated aliphatic hydrocarbon group or an unsaturated aliphatic hydrocarbon group. The aliphatic hydrocarbon group may be linear, branched, or cyclic. 3 Examples of the alkyl group include an alkyl group, an alkenyl group, an alkynyl group, and an aryl group.

[0050] R 3 The number of carbon atoms in the alkyl group is usually 1 or more, preferably 10 or less, more preferably 6 or less, and even more preferably 3 or less. Specific examples of this alkyl group include a methyl group, an ethyl group, a propyl group, an isopropyl group, a butyl group, a sec-butyl group, an isobutyl group, a tert-butyl group, a pentyl group, a hexyl group, a heptyl group, an octyl group, a nonyl group, a decyl group, and a cyclohexyl group.

[0051] R 3The number of carbon atoms in the alkenyl group in the formula (I) is usually 2 or more, preferably 12 or less, more preferably 6 or less, and even more preferably 3 or less. Specific examples of the alkenyl group include a vinyl group, an allyl group, a propenyl group, an isopropenyl group, a 1-propenyl group, a 1-butenyl group, a 2-butenyl group, a 3-butenyl group, a 1-hexenyl group, a 2-hexenyl group, a 3-hexenyl group, a 4-hexenyl group, a 5-hexenyl group, a 1-octenyl group, a 2-octenyl group, a cyclopentenyl group, a cyclohexenyl group, a cyclooctenyl group, a 1,3-butadienyl group, a 1,4-butadienyl group, a hexa-1,3-dienyl group, a hexa-2,5-dienyl group, and a hexa-1,3,5-trienyl group.

[0052] R 3 The number of carbon atoms in the alkynyl group is usually 2 or more, preferably 12 or less, more preferably 6 or less, and even more preferably 3 or less. Specific examples of this alkynyl group include an ethynyl group, a propargyl group, a 1-butynyl group, a 2-butynyl group, a 3-butynyl group, a 3-pentynyl group, a 4-pentynyl group, and a 1,3-butadiynyl group.

[0053] R 3 The aryl group in the above formula represents a monovalent hydrocarbon group obtained by removing one hydrogen atom from an aromatic hydrocarbon. This aryl group includes not only monovalent hydrocarbon groups obtained by removing one hydrogen atom from a monocyclic compound (e.g., a hydrocarbon compound formed by one aromatic ring, such as benzene), but also monovalent hydrocarbon groups obtained by removing one hydrogen atom from a fused ring compound (e.g., a hydrocarbon compound in which two or more aromatic rings are fused, such as naphthalene), and monovalent hydrocarbon groups obtained by removing one hydrogen atom from a ring assembly compound (e.g., a hydrocarbon compound in which two or more aromatic rings are bonded by a single bond, such as biphenyl). The number of carbon atoms in the aryl group is preferably 6 or more, and preferably 20 or less, more preferably 14 or less, and even more preferably 12 or less. Specific examples of the aryl group include a phenyl group, a naphthyl group, an anthracenyl group, and a biphenyl group (a group obtained by removing one hydrogen atom from biphenyl).

[0054] Among the above, R3 is preferably an alkyl group or an aryl group, more preferably a methyl group, a phenyl group or a biphenyl group.

[0055] [ka]

[0056] In formula (B-2), R 1 are each independently R in formula (1). 1 In formula (B-2), R 2 are each independently R in formula (B-1). 2 In formula (B-2), n2 represents an integer of 1 or 2 or more, and preferably an integer of 2 or more. The range of n2 may be the same as the range of the number of alkylene oxide structures per molecule contained in the polymerizable alkylene oxide resin (B) described above.

[0057] [ka]

[0058] In formula (B-3), R 1 are each independently R in formula (1). 1 In formula (B-3), R 2 are each independently R in formula (B-1). 2 In formula (B-3), m1 and m2 each independently represent 0 or 1, preferably 1. In formula (B-3), n3 and n4 each independently represent 1 or an integer of 2 or more, preferably an integer of 2 or more. The total range of n3 and n4 may be the same as the range of the number of alkylene oxide structures per molecule contained in the polymerizable alkylene oxide resin (B) described above.

[0059] In formula (B-3), R 4 represents a divalent hydrocarbon group. 4R may be an aliphatic hydrocarbon group or an aromatic hydrocarbon group. The aliphatic hydrocarbon group may be a saturated aliphatic hydrocarbon group or an unsaturated aliphatic hydrocarbon group. The aliphatic hydrocarbon group may be linear, branched, or cyclic. The number of carbon atoms in the divalent hydrocarbon group is usually 1 or more and 20 or less. 4 Examples of the alkylene group include an alkylene group having usually 1 to 20, preferably 1 to 10, and more preferably 1 to 6 carbon atoms; a cycloalkylene group having 3 to 20 carbon atoms; an alkenylene group having 2 to 10 carbon atoms; an arylene group having 6 to 10 carbon atoms; an aralkylene group having 7 to 10 carbon atoms; and groups formed by combining these groups.

[0060] R 4 Specific examples of include alkylene groups such as methylene, ethylene, propylene, trimethylene, tetramethylene, pentamethylene, hexamethylene, heptamethylene, and octamethylene; cycloalkylene groups such as cyclohexylene; alkenylene groups such as vinylene and propenylene; arylene groups such as phenylene, tolylene, xylylene, and naphthylene; aralkylene groups such as benzylene, phenylethylene, and phenylpropylene; and groups represented by the following formulas (b1) to (b6). In formulas (b1) to (b6), * represents a bonding site.

[0061] [ka]

[0062] Preferred examples of the (B) polymerizable alkylene oxide resin include resins represented by the following formulas (b-1) to (b-5).

[0063] [ka]

[0064] (In the above formula, n5, n6, and n7 each independently represent an integer of 1 or 2 or more, and may be the same as n1 in formula (B-1). n8 and n9 each independently represent an integer of 1 or 2 or more, and the total range of n8 and n9 may be the same as the range of the number of alkylene oxide structures per molecule contained in the polymerizable alkylene oxide resin (B) described above. n 10 and n 11 each independently represents an integer of 1 or 2 or more, and n 10 and n 11 The range of the total may be the same as the range of the number of alkylene oxide structures per molecule contained in the polymerizable alkylene oxide resin (B) described above.

[0065] As the (B) polymerizable alkylene oxide resin, a commercially available product may be used. Examples of commercially available products of the (B) polymerizable alkylene oxide resin include monofunctional acrylates "AM-90G", "AM-130G", and "AMP-20GY" manufactured by Shin-Nakamura Chemical Co., Ltd.; bifunctional acrylates "A-1000", "A-B1206PE", "A-BPE-20", "A-BPE-30", and "A-3000PER" manufactured by Shin-Nakamura Chemical Co., Ltd. (resins represented by formula (b-4) in which n8:n9 is approximately 6:13); and monofunctional methacrylate "M-20G" manufactured by Shin-Nakamura Chemical Co., Ltd. (resin represented by formula (b-1) ) where n5 = 2), "M-40G" (resin represented by formula (b-1) where n5 = 4), "M-90G", "M-130G" (resin represented by formula (b-1) where n5 ≒ 13), "M-230G", "PHE-1G" (resin represented by formula (b-2) where n6 = 1), "A-LEN-10" (resin represented by formula (b-3) where n7 = 1); bifunctional methacrylates "23G", "BPE-900", and "BPE-1300N" (resin represented by formula (b-5) 10 +n 11≒30 resin), "1206PE"; "Light Ester BC", "Light Ester 041MA", "Light Acrylate EC-A", and "Light Acrylate EHDG-AT" manufactured by Kyoeisha Chemical Co., Ltd.; "FA-023M" manufactured by Resonac Corporation; and "Blenmer (registered trademark) PME-4000", "Blenmer (registered trademark) 50POEO-800B", "Blenmer (registered trademark) PLE-200", "Blenmer (registered trademark) PLE-1300", "Blenmer (registered trademark) PSE-1300", "Blenmer (registered trademark) 43PAPE-600B", and "Blenmer (registered trademark) ANP-300" manufactured by NOF Corporation.

[0066] The (B) polymerizable alkylene oxide resin may be used alone or in combination of two or more.

[0067] The radical polymerizable group equivalent weight of the (B) polymerizable alkylene oxide resin is preferably 150 g / eq. or more. Specifically, the radical polymerizable group equivalent weight of a monofunctional (B) polymerizable alkylene oxide resin having one radical polymerizable group per molecule is preferably 150 g / eq. or more, more preferably 250 g / eq. or more, and even more preferably 400 g / eq. or more. The radical polymerizable group equivalent weight of a bifunctional (B) polymerizable alkylene oxide resin having two radical polymerizable groups per molecule is preferably 500 g / eq. or more, more preferably 510 g / eq. or more, and even more preferably 600 g / eq. or more. The upper limit of the radical polymerizable group equivalent weight of the (B) polymerizable alkylene oxide resin is preferably 4500 g / eq. or less, more preferably 3000 g / eq. or less, even more preferably 2000 g / eq. or less, and even more preferably 1500 g / eq. or less. The radical polymerizable group equivalent represents the mass of the resin per equivalent of the radical polymerizable group.

[0068] The molecular weight range of the (B) polymerizable alkylene oxide resin is preferably 150 or more. Specifically, the molecular weight of a monofunctional (B) polymerizable alkylene oxide resin having one radically polymerizable group per molecule is preferably 150 or more, more preferably 250 or more, and even more preferably 400 or more. The molecular weight of a bifunctional (B) polymerizable alkylene oxide resin having two radically polymerizable groups per molecule is preferably 1000 or more, more preferably 1020 or more, and even more preferably 1200 or more. The upper limit of the molecular weight of the (B) polymerizable alkylene oxide resin is preferably 5000 or less, more preferably 3000 or less, even more preferably 2500 or less, even more preferably 2000 or less, and even more preferably 1500 or less. When the (B) polymerizable alkylene oxide resin is a polymer, it is preferable that its weight-average molecular weight or number-average molecular weight be within the above range. The weight average molecular weight and number average molecular weight of the (B) polymerizable alkylene oxide resin can be measured by gel permeation chromatography (GPC) in terms of polystyrene.

[0069] The amount of (B) polymerizable alkylene oxide resin is preferably 0.5% by mass or more, more preferably 1.0% by mass or more, and even more preferably 1.4% by mass or more, relative to 100% by mass of nonvolatile components in the resin composition, and is preferably 20% by mass or less, more preferably 10% by mass or less, and even more preferably 5% by mass or less. When the amount of (B) polymerizable alkylene oxide resin is within this range, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0070] The amount of (B) polymerizable alkylene oxide resin is preferably 1% by mass or more, more preferably 3% by mass or more, and even more preferably 6% by mass or more, relative to 100% by mass of the resin components in the resin composition, and is preferably 40% by mass or less, more preferably 35% by mass or less, and even more preferably 30% by mass or less. When the amount of (B) polymerizable alkylene oxide resin is within the above range, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0071] <(C) Hardener> The resin composition according to this embodiment includes a (C) curing agent as component (C). The (C) curing agent reacts with the (A) epoxy resin to form a bond, thereby curing the resin composition. The (C) curing agent does not include those corresponding to the above-mentioned components (A) and (B). One type of (C) curing agent may be used alone, or two or more types may be used in combination.

[0072] Examples of the (C) curing agent include acid anhydride resins, active ester resins, phenolic resins, carbodiimide resins, benzoxazine resins, cyanate ester resins, amine resins, thiol resins, etc. One type of (C) curing agent may be used alone, or two or more types may be used in combination.

[0073] The (C) curing agent preferably contains an acid anhydride resin, and may contain only an acid anhydride resin. Conventional resin compositions containing an acid anhydride resin tend to have particularly poor chemical resistance and are particularly prone to the formation of flow marks. In contrast, the resin composition according to the present embodiment can improve chemical resistance and suppress flow marks, even when the (C) curing agent contains an acid anhydride resin. Therefore, when the resin composition contains an acid anhydride resin, the advantages of the present invention can be particularly effectively utilized.

[0074] As the acid anhydride resin, a resin having one or more, preferably two or more, acid anhydride groups in one molecule can be used. Specific examples of the acid anhydride resin include phthalic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, methyltetrahydrophthalic anhydride, methylhexahydrophthalic anhydride, methylnadic anhydride, hydrogenated methylnadic anhydride, trialkyltetrahydrophthalic anhydride, dodecenyl succinic anhydride, 5-(2,5-dioxotetrahydro-3-furanyl)-3-methyl-3-cyclohexene-1,2-dicarboxylic anhydride, trimellitic anhydride, pyromellitic anhydride, and benzophenonetetracarboxylic dianhydride. Examples of suitable anhydrides include anhydrides, biphenyltetracarboxylic dianhydride, naphthalenetetracarboxylic dianhydride, oxydiphthalic dianhydride, 3,3'-4,4'-diphenylsulfonetetracarboxylic dianhydride, 1,3,3a,4,5,9b-hexahydro-5-(tetrahydro-2,5-dioxo-3-furanyl)-naphtho[1,2-C]furan-1,3-dione, ethylene glycol bis(anhydrotrimellitate), and polymeric anhydrides such as styrene-maleic acid resins, which are copolymers of styrene and maleic acid.

[0075] Commercially available acid anhydride resins include, for example, "HNA-100," "MH-700," "MTA-15," "DDSA," and "OSA" manufactured by New Japan Chemical Co., Ltd.; "YH-306" and "YH-307" manufactured by Mitsubishi Chemical Corporation; "HN-2200" and "HN-5500" manufactured by Resonac Corporation; and "EF-30," "EF-40," "EF-60," and "EF-80" manufactured by Cray Valley Chemical Industries, Ltd.

[0076] The amount of the acid anhydride resin is preferably 0.5% by mass or more, more preferably 1.0% by mass or more, and even more preferably 2.0% by mass or more, relative to 100% by mass of the nonvolatile components in the resin composition, and is preferably 20% by mass or less, more preferably 10% by mass or less, and even more preferably 6% by mass or less. When the amount of the acid anhydride resin is within this range, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0077] The amount of the acid anhydride resin is preferably 3% by mass or more, more preferably 5% by mass or more, and even more preferably 10% by mass or more, relative to 100% by mass of the resin components in the resin composition, and is preferably 40% by mass or less, more preferably 35% by mass or less, and even more preferably 30% by mass or less. When the amount of the acid anhydride resin is within the above range, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0078] The active ester resin may be a resin having one or more, preferably two or more, active ester groups in one molecule. Among them, preferred active ester resins are those having two or more highly reactive ester groups in one molecule, such as phenol esters, thiophenol esters, N-hydroxyamine esters, and esters of heterocyclic hydroxy compounds.

[0079] The active ester resin is preferably one obtained by a condensation reaction between a carboxylic acid compound and / or a thiocarboxylic acid compound and a hydroxy compound and / or a thiol compound. From the viewpoint of improving heat resistance in particular, an active ester resin obtained from a carboxylic acid compound and a hydroxy compound is preferred, and an active ester resin obtained from a carboxylic acid compound and a phenol compound and / or a naphthol compound is more preferred. Examples of the carboxylic acid compound include benzoic acid, acetic acid, succinic acid, maleic acid, itaconic acid, phthalic acid, isophthalic acid, terephthalic acid, and pyromellitic acid. Examples of phenol compounds or naphthol compounds include hydroquinone, resorcinol, bisphenol A, bisphenol F, bisphenol S, phenolphthalene, methylated bisphenol A, methylated bisphenol F, methylated bisphenol S, phenol, o-cresol, m-cresol, p-cresol, catechol, α-naphthol, β-naphthol, 1,5-dihydroxynaphthalene, 1,6-dihydroxynaphthalene, 2,6-dihydroxynaphthalene, dihydroxybenzophenone, trihydroxybenzophenone, tetrahydroxybenzophenone, phloroglucin, benzenetriol, dicyclopentadiene-type diphenol compounds, and phenol novolak. Here, "dicyclopentadiene-type diphenol compounds" refers to diphenol compounds obtained by condensing one dicyclopentadiene molecule with two phenol molecules.

[0080] Specifically, the active ester resin is preferably a dicyclopentadiene-type active ester resin, a naphthalene-type active ester resin containing a naphthalene structure, an active ester resin containing an acetylated product of phenol novolac, or an active ester resin containing a benzoylated product of phenol novolac, and among these, a dicyclopentadiene-type active ester resin is more preferred. As the dicyclopentadiene-type active ester resin, an active ester resin containing a dicyclopentadiene-type diphenol structure is preferred.

[0081] Commercially available active ester resins include, for example, "EXB9451", "EXB9460", "EXB9460S", "EXB-8000L", "EXB-8000L-65M", "EXB-8000L-65TM", "HPC-8000L-65TM", "HPC-8000", "HPC-8000-65T", "HPC-8000H", and "HPC-8000H-65TM" (manufactured by DIC Corporation) as active ester resins containing a dicyclopentadiene-type diphenol structure; and "HP-B-8151-62T", "EXB-8100L-65T", "EXB-8150-60T", and "EXB-815 Examples of such active ester resins include "EXB-9416-70BK", "HPC-8150-60T", "HPC-8150-62T", and "EXB-8" (manufactured by DIC Corporation); an active ester resin containing phosphorus, such as "EXB9401" (manufactured by DIC Corporation); an active ester resin which is an acetylated product of phenol novolac, such as "DC808" (manufactured by Mitsubishi Chemical Corporation); active ester resins which are benzoylated products of phenol novolac, such as "YLH1026", "YLH1030", and "YLH1048" (manufactured by Mitsubishi Chemical Corporation); and an active ester resin containing a styryl group and a naphthalene structure, such as "PC1300-02-65MA" (manufactured by Air Water Inc.).

[0082] As the phenolic resin, a resin having one or more, preferably two or more, hydroxyl groups (phenolic hydroxyl groups) bonded to an aromatic ring such as a benzene ring or a naphthalene ring per molecule can be used. From the viewpoint of heat resistance and water resistance, a phenolic resin having a novolac structure is preferred. From the viewpoint of adhesion, a nitrogen-containing phenolic resin may be used, for example, a phenolic resin containing a triazine skeleton. As a specific example, from the viewpoint of highly satisfying heat resistance, water resistance, and adhesion, a phenolic novolac resin containing a triazine skeleton may be used.

[0083] Specific examples of phenolic resins include "MEH-7700", "MEH-7810", "MEH-7851", and "MEH-8000H" manufactured by Meiwa Kasei Co., Ltd.; "NHN", "CBN", and "GPH" manufactured by Nippon Kayaku Co., Ltd.; "SN-170", "SN-180", "SN-190", "SN-475", "SN-485", "SN-495", "SN-495V", and "SN-375" manufactured by Nippon Steel Chemical & Material Co., Ltd. Examples include "SN-395"; "TD-2090", "TD-2090-60M", "LA-7052", "LA-7054", "LA-1356", "LA-3018", "LA-3018-50P", "LA-1356", "TD2090", "TD-2090-60M", and "KA-1160" manufactured by DIC Corporation; and "GDP-6115L", "GDP-6115H", and "ELPC75" manufactured by Gun-ei Chemical Co., Ltd.

[0084] As the carbodiimide resin, a resin having one or more, preferably two or more, carbodiimide structures in one molecule can be used. Specific examples of the carbodiimide resin include aliphatic biscarbodiimides such as tetramethylene-bis(t-butylcarbodiimide) and cyclohexanebis(methylene-t-butylcarbodiimide); aromatic biscarbodiimides such as phenylene-bis(xylylcarbodiimide); aliphatic polycarbodiimides such as polyhexamethylenecarbodiimide, polytrimethylhexamethylenecarbodiimide, polycyclohexylenecarbodiimide, poly(methylenebiscyclohexylenecarbodiimide), and poly(isophoronecarbodiimide); poly(phenylenecarbodiimide), poly(naphthalenecarbodiimide); Examples of polycarbodiimides include aromatic polycarbodiimides such as poly(methylenediphenylenecarbodiimide), poly(tolylenecarbodiimide), poly(methyldiisopropylphenylenecarbodiimide), poly(triethylphenylenecarbodiimide), poly(diethylphenylenecarbodiimide), poly(triisopropylphenylenecarbodiimide), poly(diisopropylphenylenecarbodiimide), poly(xylylenecarbodiimide), poly(tetramethylxylylenecarbodiimide), poly(methylenediphenylenecarbodiimide), and poly[methylenebis(methylphenylene)carbodiimide]. Commercially available carbodiimide resins include, for example, "Carbodilite V-02B," "Carbodilite V-03," "Carbodilite V-04K," "Carbodilite V-05," "Carbodilite V-07," and "Carbodilite V-09" manufactured by Nisshinbo Chemical Inc.; and "Stavaxol P," "Stavaxol P400," and "Hykasil 510" manufactured by Lanxess AG.

[0085] The benzoxazine resin may be a resin having one or more, preferably two or more, benzoxazine rings in one molecule. Specific examples of the benzoxazine resin include "JBZ-OP100D" and "ODA-BOZ" manufactured by JFE Chemical Corporation, "HFB2006M" manufactured by Showa Polymer Co., Ltd., and "Pd" and "Fa" manufactured by Shikoku Chemical Industry Co., Ltd.

[0086] As the cyanate ester resin, a resin having one or more, preferably two or more, cyanate groups in one molecule can be used. Examples of cyanate ester resins include bifunctional cyanate ester resins such as bisphenol A dicyanate, polyphenol cyanate, oligo(3-methylene-1,5-phenylene cyanate), 4,4'-methylenebis(2,6-dimethylphenyl cyanate), 4,4'-ethylidene diphenyl dicyanate, hexafluorobisphenol A dicyanate, 2,2-bis(4-cyanate)phenylpropane, 1,1-bis(4-cyanatephenylmethane), bis(4-cyanate-3,5-dimethylphenyl)methane, 1,3-bis(4-cyanatephenyl-1-(methylethylidene))benzene, bis(4-cyanatephenyl)thioether, and bis(4-cyanatephenyl)ether; multifunctional cyanate ester resins derived from phenol novolac, cresol novolac, and the like; and prepolymers in which these cyanate ester resins are partially triazine converted. Specific examples of cyanate ester resins include "PT30" and "PT60" (phenol novolac type multifunctional cyanate ester resins) manufactured by Lonza, "BA230" and "BA230S75" (prepolymers in which part or all of bisphenol A dicyanate has been triazine converted to a trimer).

[0087] The amine resin may be a resin having one or more, preferably two or more, amino groups in one molecule. Examples of the amine resin include aliphatic amines, polyether amines, alicyclic amines, and aromatic amines, with aromatic amines being preferred. The amine resin is preferably a primary amine or secondary amine, with primary amines being more preferred. Specific examples of the amine resin include 4,4'-methylenebis(2,6-dimethylaniline), 4,4'-diaminodiphenylmethane, 4,4'-diaminodiphenyl sulfone, 3,3'-diaminodiphenyl sulfone, m-phenylenediamine, m-xylylenediamine, diethyltoluenediamine, 4,4'-diaminodiphenyl ether, 3,3'-dimethyl-4,4'-diaminobiphenyl, 2,2'-dimethyl-4,4'-diaminobiphenyl, 3,3'-dihydroxybenzidine, and 2,2-bis(3-amino-4-hydroxyphenyl)propanol. Examples of suitable bis(4-aminophenoxy)benzene include bis(4-aminophenyl)propane, 3,3-dimethyl-5,5-diethyl-4,4-diphenylmethanediamine, 2,2-bis(4-aminophenyl)propane, 2,2-bis(4-(4-aminophenoxy)phenyl)propane, 1,3-bis(3-aminophenoxy)benzene, 1,3-bis(4-aminophenoxy)benzene, 1,4-bis(4-aminophenoxy)benzene, 4,4'-bis(4-aminophenoxy)biphenyl, bis(4-(4-aminophenoxy)phenyl)sulfone, and bis(4-(3-aminophenoxy)phenyl)sulfone. Commercially available amine-based resins include, for example, "SEIKACURE-S" manufactured by Seika Corporation; "KAYABOND C-200S," "KAYABOND C-100," "KAYAHARD AA," "KAYAHARD AB," and "KAYAHARD AS" manufactured by Nippon Kayaku Co., Ltd.; "Epicure W" manufactured by Mitsubishi Chemical Corporation; and "DTDA" manufactured by Sumitomo Seika Chemicals Co., Ltd.

[0088] Examples of thiol-based resins include trimethylolpropane tris(3-mercaptopropionate), pentaerythritol tetrakis(3-mercaptobutyrate), and tris(3-mercaptopropyl)isocyanurate.

[0089] The active group equivalent of the (C) curing agent is preferably 50 g / eq to 3000 g / eq, more preferably 100 g / eq to 1000 g / eq, even more preferably 100 g / eq to 500 g / eq, and particularly preferably 100 g / eq to 300 g / eq. The active group equivalent represents the mass of the resin per equivalent of the active group. Thus, for example, the active group equivalent of an acid anhydride resin represents the acid anhydride group equivalent, which represents the mass of the resin per equivalent of the acid anhydride group.

[0090] In one example, the weight average molecular weight (Mw) range of the (C) curing agent may be the same as the weight average molecular weight (Mw) range of the (A) epoxy resin.

[0091] The ratio of the number of active groups in the (C) curing agent to the number of epoxy groups in the (A) epoxy resin (number of active groups / number of epoxy groups) is preferably within a specific range. Specifically, the range of the ratio (number of active groups / number of epoxy groups) is preferably 0.50 or less, more preferably 0.40 or less, and even more preferably 0.35 or less. The lower limit is preferably 0.05 or more, more preferably 0.10 or more, and even more preferably 0.15 or more. The number of epoxy groups in the (A) epoxy resin refers to the sum of all values obtained by dividing the mass of the non-volatile components of the (A) epoxy resin present in the resin composition by its epoxy equivalent. Furthermore, the number of active groups in the (C) curing agent refers to the sum of all values obtained by dividing the mass of the non-volatile components of the (C) curing agent present in the resin composition by its active group equivalent. When the ratio (number of active groups / number of epoxy groups) is within the above range, the chemical resistance of the cured product of the resin composition can be particularly good, and the formation of flow marks can usually be effectively suppressed.

[0092] The amount of (C) curing agent is preferably 0.5% by mass or more, more preferably 1.0% by mass or more, and even more preferably 2.0% by mass or more, relative to 100% by mass of nonvolatile components in the resin composition, and is preferably 20% by mass or less, more preferably 10% by mass or less, and even more preferably 6% by mass or less. When the amount of (C) curing agent is within this range, the chemical resistance of the cured product of the resin composition can be particularly improved, and usually the formation of flow marks can be effectively suppressed.

[0093] The amount of (C) curing agent is preferably 3% by mass or more, more preferably 5% by mass or more, and even more preferably 10% by mass or more, relative to 100% by mass of the resin components in the resin composition, and is preferably 40% by mass or less, more preferably 35% by mass or less, and even more preferably 30% by mass or less. When the amount of (C) curing agent is within this range, the chemical resistance of the cured product of the resin composition can be particularly good, and further, the formation of flow marks can usually be effectively suppressed.

[0094] The amount of (C) curing agent is preferably 5% by mass or more, more preferably 10% by mass or more, and even more preferably 15% by mass or more, relative to 100% by mass of the total of (A) epoxy resin and (B) polymerizable alkylene oxide resin, and is preferably 70% by mass or less, more preferably 60% by mass or less, and even more preferably 50% by mass or less. When the amount of (C) curing agent is within this range, the chemical resistance of the cured product of the resin composition can be particularly good, and usually the formation of flow marks can be effectively suppressed.

[0095] <(D) Silane coupling agent> The resin composition according to the present embodiment includes a silane coupling agent (D) as the component (D). The silane coupling agent (D) as the component (D) generally contains an organic reactive moiety and an inorganic reactive moiety, and therefore can increase the adhesive strength between the cured product of the resin composition and the conductor layer in contact with the cured product. Furthermore, the resin composition according to the present embodiment includes two or more types of silane coupling agents (D).

[0096] As described below, the (D) silane coupling agent may be used as a surface treatment agent for the (E) inorganic filler. Therefore, the (D) silane coupling agent may be adsorbed onto particles of the inorganic material contained in the (E) inorganic filler. Alternatively, the (D) silane coupling agent may be contained in the resin composition in a free state in the resin component without being adsorbed onto particles of the inorganic material. For example, a portion of the (D) silane coupling agent may be adsorbed onto particles of the inorganic material, and another portion may be free in the resin component.

[0097] Examples of silane coupling agents include γ-aminopropyldimethoxysilane, N-(β-aminoethyl)-γ-aminopropylmethyldimethoxysilane, γ-glycidoxypropylmethyldimethoxysilane, γ-mercaptopropylmethyldimethoxysilane, 3-methacryloxypropyldimethoxymethylsilane, 3-methacryloxypropyltrimethoxysilane, 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropyltriethoxysilane, dimethoxymethyl-3-piperidinopropylsilane, diethoxy-3-glycidoxypropylmethylsilane, N-(3-diethoxymethylsilylpropyl)succinimide, N-[3-(triethoxysilyl)propyl]phthalamic acid, benzophenone-3,3'-bis(N-[3-triethoxysilyl]propylamide)-4,4'-dicarboxylic acid, benzene-1,4-bis(N-3-triethoxysilyl]propylamide)-2,5-Dicarboxylic acid, 3-(triethoxysilyl)propyl succinic anhydride, N-phenylaminopropyltrimethoxysilane, 3-ureidopropyltrimethoxysilane, 3-ureidopropyltriethoxysilane, 3-(trialkoxysilyl)propylsuccinic anhydride, 3-mercaptopropyltrimethoxysilane, 3-mercaptopropyltriethoxysilane, 3-mercaptopropylmethyldimethoxysilane, mercaptomethyltrimethoxysilane, mercaptomethylmethyldimethoxysilane, 3-mercaptopropyldiethoxymethoxysilane, 3-mercaptopropylethoxydimethoxysilane, 3-mercaptopropyltripropoxysilane, 3-mercaptopropyldiethoxypropoxysilane, 3-mercaptopropylethoxydipropoxysilane, 3-mercaptopropyl propyldimethoxypropoxysilane, 3-mercaptopropylmethoxydipropoxysilane, 2-mercaptoethyltrimethoxysilane, 2-mercaptoethyldiethoxymethoxysilane, 2-mercaptoethylethoxydimethoxysilane, 2-mercaptoethyltripropoxysilane, 2-mercaptoethyltrippropoxysilane, 2-mercaptoethylethoxydipropoxysilane, 2-mercaptoethyldimethoxypropoxysilane, 2-mercaptoethylmethoxydipropoxysilane, 4-mercaptobutyltrimethoxysilane, 4-mercaptobutyltriethoxysilane, 4-mercaptobutyltrippropoxysilane, N-(3-triethoxysilylpropyl)urea, N-(3-trimethoxysilylpropyl)urea, compounds having an aminotriazine ring and an ethoxysilyl group, and the like. Among these, epoxysilane-based silane coupling agents containing an epoxy group and aminosilane-based silane coupling agents containing an amino group are preferred.

[0098] When the (D) silane coupling agent contains an epoxysilane-based silane coupling agent, the amount of the epoxysilane-based silane coupling agent is preferably 0.1% by mass or more, more preferably 0.2% by mass or more, even more preferably 0.3% by mass or more, and is preferably 5% by mass or less, more preferably 2% by mass or less, and even more preferably 1% by mass or less, relative to 100% by mass of the resin components in the resin composition. When the amount of the epoxysilane-based silane coupling agent is within the above range, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0099] When the (D) silane coupling agent contains an aminosilane-based silane coupling agent, the amount of the aminosilane-based silane coupling agent is preferably 0.1% by mass or more, more preferably 1% by mass or more, and even more preferably 2% by mass or more, relative to 100% by mass of the resin components in the resin composition, and is preferably 10% by mass or less, more preferably 8% by mass or less, and even more preferably 5% by mass or less. When the amount of the aminosilane-based silane coupling agent is within the above range, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0100] When the (D) silane coupling agent contains one or more silane coupling agents selected from the group consisting of epoxysilane-based silane coupling agents and aminosilane-based silane coupling agents, the total amount of the epoxysilane-based silane coupling agent and aminosilane-based silane coupling agent is preferably 0.1% by mass or more, more preferably 1% by mass or more, even more preferably 2% by mass or more, and preferably 10% by mass or less, more preferably 8% by mass or less, even more preferably 5% by mass or less, based on 100% by mass of the resin components in the resin composition. When the total amount of the epoxysilane-based silane coupling agent and aminosilane-based silane coupling agent is within the above range, the chemical resistance of the cured product of the resin composition can be particularly good, and the formation of flow marks can usually be effectively suppressed.

[0101] (D) The silane coupling agent may be a commercially available product. Examples of commercially available (D) silane coupling agents include "KBM403" (3-glycidoxypropyltrimethoxysilane), "KBM803" (3-mercaptopropyltrimethoxysilane), "KBE903" (3-aminopropyltriethoxysilane), "KBM573" (N-phenyl-3-aminopropyltrimethoxysilane), "SZ-31" (hexamethyldisilazane), "KBM103" (phenyltrimethoxysilane), "KBM-4803" (long-chain epoxy-type silane coupling agent), "KBM-7103" (3,3,3-trifluoropropyltrimethoxysilane), "LS1375" (3-mercaptopropylmethyldimethoxysilane), and "LS3610" (N-(3-trifluoropropyltrimethoxysilane)), all manufactured by Shin-Etsu Chemical Co., Ltd. (N-(3-triethoxysilylpropyl)urea); "Sila Ace S810" (3-mercaptopropyltrimethoxysilane) manufactured by Chisso Corporation; "SIM6475.0" (3-mercaptopropyltriethoxysilane), "SIM6474.0" (3-mercaptopropylmethyldimethoxysilane), "SIM6473.5C" (mercaptomethyltrimethoxysilane), "SIM6473.0" (mercaptomethylmethyldimethoxysilane), "SIU9055.0" (N-(3-triethoxysilylpropyl)urea), "SIU9058.0" (N-(3-trimethoxysilylpropyl)urea); "VD-5" (compound having an aminotriazine ring and an ethoxysilyl group) manufactured by Shikoku Chemicals Corporation; and the like.

[0102] The amount of (D) silane coupling agent is preferably 0.1% by mass or more, more preferably 0.2% by mass or more, even more preferably 0.3% by mass or more, and preferably 5% by mass or less, more preferably 2% by mass or less, and even more preferably 1% by mass or less, based on 100% by mass of nonvolatile components in the resin composition. Unless otherwise specified, the amount of (D) silane coupling agent includes both the amount of silane coupling agent adsorbed on inorganic material particles as a surface treatment agent and the amount of silane coupling agent not adsorbed on inorganic material particles but free in the resin component. When the amount of (D) silane coupling agent is within the above range, the chemical resistance of the cured resin composition can be particularly improved, and the formation of flow marks can usually be effectively suppressed.

[0103] The amount of (D) silane coupling agent is preferably 0.1% by mass or more, more preferably 1% by mass or more, and even more preferably 2% by mass or more, relative to 100% by mass of the resin components in the resin composition, and is preferably 10% by mass or less, more preferably 8% by mass or less, and even more preferably 5% by mass or less. When the amount of (D) silane coupling agent is within this range, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0104] The amount of (D) silane coupling agent is preferably 0.1% by mass or more, more preferably 0.5% by mass or more, and even more preferably 1% by mass or more, relative to 100% by mass of (A) epoxy resin in the resin composition, and is preferably 20% by mass or less, more preferably 10% by mass or less, and even more preferably 7% by mass or less. When the amount of (D) silane coupling agent is within this range, the chemical resistance of the cured product of the resin composition can be particularly improved, and usually the formation of flow marks can be effectively suppressed.

[0105] The amount of (D) silane coupling agent is preferably 2% by mass or more, more preferably 8% by mass or more, and even more preferably 14% by mass or more, relative to 100% by mass of (B) polymerizable alkylene oxide resin in the resin composition, and is preferably 60% by mass or less, more preferably 50% by mass or less, and even more preferably 40% by mass or less. When the amount of (D) silane coupling agent is within this range, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0106] The amount of (D) silane coupling agent is preferably 1% by mass or more, more preferably 5% by mass or more, and even more preferably 10% by mass or more, relative to 100% by mass of (C) curing agent in the resin composition, and is preferably 80% by mass or less, more preferably 50% by mass or less, and even more preferably 40% by mass or less. When the amount of (D) silane coupling agent is within this range, the chemical resistance of the cured product of the resin composition can be particularly improved, and further, the formation of flow marks can usually be effectively suppressed.

[0107] The amount of the silane coupling agent (D) that is not adsorbed to the inorganic material particles and remains free in the resin component is preferably 0.1% by mass or more, more preferably 0.2% by mass or more, even more preferably 0.3% by mass or more, and is preferably 5% by mass or less, more preferably 3% by mass or less, and even more preferably 1% by mass or less, relative to 100% by mass of the resin component in the resin composition. When the amount of the free silane coupling agent (D) is within the above range, the chemical resistance of the cured product of the resin composition can be particularly improved, and the formation of flow marks can usually be effectively suppressed.

[0108] <(E) Inorganic filler> The resin composition according to this embodiment may contain an inorganic filler (E) as an optional component. The inorganic filler (E) as component (E) is contained in the resin composition in the form of particles, and is usually contained in the cured product while maintaining this particulate state. In general, the inorganic filler (E) has a lower thermal expansion coefficient than the resin component, and therefore can reduce the thermal expansion of the cured product of the resin composition, thereby suppressing warpage of the circuit board.

[0109] (E) Inorganic fillers typically contain particles of inorganic materials. The inorganic material forming the (E) inorganic filler is typically an inorganic compound. Examples of inorganic materials include silica, alumina, glass, cordierite, silicon oxide, barium sulfate, barium carbonate, talc, clay, mica powder, zinc oxide, hydrotalcite, boehmite, aluminum hydroxide, magnesium hydroxide, calcium carbonate, magnesium carbonate, magnesium oxide, boron nitride, aluminum nitride, manganese nitride, aluminum borate, strontium carbonate, strontium titanate, calcium titanate, magnesium titanate, bismuth titanate, titanium oxide, zirconium oxide, barium titanate, barium titanate zirconate, barium zirconate, calcium zirconate, zirconium phosphate, and zirconium tungstate phosphate. Among these, silica and alumina are preferred, with silica being particularly preferred. Therefore, (E) Inorganic fillers preferably contain silica, but may also contain only silica. Examples of silica include amorphous silica, fused silica, crystalline silica, synthetic silica, and hollow silica. Spherical silica is preferred. (E) The inorganic filler may be used alone or in combination of two or more.

[0110] (E) Examples of commercially available inorganic fillers include "SP60-05" and "SP507-05" manufactured by Nippon Steel Chemical & Material Co., Ltd.; "YC100C," "YA050C," "YA050C-MJE," "YA010C," "SC2500SQ," "SO-C4," "SO-C2," and "SO-C1" manufactured by Admatechs Co., Ltd.; "UFP-30," "DAW-03," and "FB-105FD" manufactured by Denka Company, Limited; "Silfil NSS-3N," "Silfil NSS-4N," and "Silfil NSS-5N" manufactured by Tokuyama Corporation; "CellSpheres" and "MGH-005" manufactured by Taiheiyo Cement Corporation; and "Sferique" and "BA-1" manufactured by JGC Catalysts and Chemicals Co., Ltd.

[0111] The average particle size of the (E) inorganic filler is preferably 0.01 μm or more, more preferably 0.05 μm or more, even more preferably 0.1 μm or more, and preferably 10 μm or less, more preferably 5 μm or less, even more preferably 3 μm or less, even more preferably 2 μm or less.

[0112] (E) The average particle size of an inorganic filler can be measured by a laser diffraction / scattering method based on Mie scattering theory. Specifically, a volumetric particle size distribution of the inorganic filler is created using a laser diffraction / scattering particle size distribution analyzer, and the median diameter is used as the average particle size. A measurement sample can be prepared by weighing 100 mg of inorganic filler and 10 g of methyl ethyl ketone into a vial and dispersing the mixture ultrasonically for 10 minutes. The volumetric particle size distribution of the inorganic filler is measured using a laser diffraction particle size distribution analyzer with blue and red wavelength light sources using a flow cell system, and the average particle size can be calculated as the median diameter from the particle size distribution obtained. Examples of laser diffraction particle size distribution analyzers include the LA-960 manufactured by Horiba, Ltd.

[0113] (E) The specific surface area of the inorganic filler is preferably 0.1 m 2 / g or more, more preferably 0.5m 2 / g or more, more preferably 1m 2 / g or more, particularly preferably 3m 2 / g or more, preferably 100m 2 / g or less, more preferably 70m 2 / g or less, more preferably 50m 2 / g or less, particularly preferably 40m 2 / g or less. (E) The specific surface area of the inorganic filler can be measured in accordance with the BET method by adsorbing nitrogen gas onto the surface of a sample using a specific surface area measuring device (Macsorb HM-1210 manufactured by Mountech Co., Ltd.) and calculating the specific surface area using the BET multipoint method.

[0114] The maximum cut diameter of the (E) inorganic filler is preferably 10 μm or less, more preferably 8 μm or less, even more preferably 6 μm or less, and is preferably 0.5 μm or more, more preferably 1 μm or more, even more preferably 2 μm or more. The maximum cut diameter is a reference diameter set when classifying the particles of the (E) inorganic filler, and particles classified to have a particle size of this maximum cut diameter or less are preferably used as the (E) inorganic filler.

[0115] The (E) inorganic filler is preferably treated with a surface treatment agent from the viewpoint of improving moisture resistance and dispersibility. The (E) inorganic filler thus treated with a surface treatment agent may contain inorganic material particles and the surface treatment agent adsorbed to the particles. Examples of the surface treatment agent include (D) silane coupling agents, titanate coupling agents, and other coupling agents; alkoxysilanes; organosilazane compounds; and the like. Among these, (D) silane coupling agents are preferred. Examples of silane coupling agents suitable for the surface treatment agent include fluorine-containing silane coupling agents, aminosilane-based silane coupling agents, epoxysilane-based silane coupling agents, and mercaptosilane-based silane coupling agents. One type of surface treatment agent may be used alone, or two or more types may be used in any combination.

[0116] Examples of commercially available surface treatment agents include Shin-Etsu Chemical Co., Ltd.'s "KBM403" (3-glycidoxypropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBM803" (3-mercaptopropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBE903" (3-aminopropyltriethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBM573" (N-phenyl-3-aminopropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "SZ-31" (hexamethyldisilazane), Shin-Etsu Chemical Co., Ltd.'s "KBM103" (phenyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBM-4803" (long-chain epoxy-type silane coupling agent), and Shin-Etsu Chemical Co., Ltd.'s "KBM-7103" (3,3,3-trifluoropropyltrimethoxysilane).

[0117] The degree of surface treatment with the surface treatment agent preferably falls within a specific range from the viewpoint of improving the dispersibility of the inorganic filler. Specifically, 100% by mass of the inorganic filler is preferably surface-treated with 0.2% to 5% by mass of the surface treatment agent, more preferably with 0.2% to 3% by mass of the surface treatment agent, and even more preferably with 0.3% to 2% by mass of the surface treatment agent.

[0118] The degree of surface treatment with the surface treatment agent can be evaluated by the amount of carbon per unit surface area of the inorganic filler. From the viewpoint of improving the dispersibility of the inorganic filler, the amount of carbon per unit surface area of the inorganic filler is set to 0.02 mg / m 2 More than 0.1 mg / m is preferable. 2 More preferably, 0.2 mg / m or more 2 On the other hand, from the viewpoint of preventing an increase in the melt viscosity of the resin composition layer, it is more preferable that the amount of the resin composition layer is 1.0 mg / m 2 Less than 0.8 mg / m is preferred 2 Less than 0.5 mg / m is more preferable. 2 The following is even more preferred:

[0119] (E) The amount of carbon per unit surface area of the inorganic filler can be measured after the surface-treated inorganic filler is washed with a solvent (e.g., methyl ethyl ketone (MEK)). Specifically, a sufficient amount of MEK as a solvent is added to the inorganic filler that has been surface-treated with a surface treatment agent, and ultrasonic cleaning is performed at 25°C for 5 minutes. After removing the supernatant and drying the solid content, the amount of carbon per unit surface area of the inorganic filler can be measured using a carbon analyzer. The carbon analyzer that can be used is the "EMIA-320V" manufactured by Horiba, Ltd.

[0120] The amount of the (E) inorganic filler is preferably 50% by mass or more, more preferably 60% by mass or more, even more preferably 70% by mass or more, and may be 80% by mass or more, based on 100% by mass of the nonvolatile components in the resin composition. The upper limit is preferably 90% by mass or less, more preferably 88% by mass or less, and even more preferably 85% by mass or less. When the (E) inorganic filler has been surface-treated, the amount of the (E) inorganic filler includes the amount of the surface treatment agent. When the amount of the (E) inorganic filler is within the above range, the chemical resistance of the cured resin composition can be particularly improved, and the formation of flow marks can usually be effectively suppressed.

[0121] The range of the amount of inorganic material particles in the (E) inorganic filler, excluding the surface treatment agent, is preferably 50% by mass or more, more preferably 60% by mass or more, even more preferably 70% by mass or more, and preferably 90% by mass or less, more preferably 88% by mass or less, even more preferably 85% by mass or less, based on 100% by mass of the nonvolatile components in the resin composition. When the amount of inorganic material particles in the (E) inorganic filler is within the above range, the chemical resistance of the cured resin composition can be particularly improved, and the formation of flow marks can usually be effectively suppressed.

[0122] <(F) Radical generator> The resin composition according to this embodiment may contain a (F) radical generator as an optional component. The (F) radical generator as the (F) component does not include those corresponding to the above-mentioned components (A) to (E). A thermal radical generator is usually used as the (F) radical generator. A thermal radical generator can generate radicals by applying thermal energy, and therefore can promote the reaction of the (B) polymerizable alkylene oxide resin. One type of (F) radical generator may be used alone, or two or more types may be used in combination.

[0123] Examples of thermal radical generators include dialkyl peroxides such as di-t-butyl peroxide, dicumyl peroxide, and t-hexylperoxy-2-ethylhexanoate; diacyl peroxides such as lauroyl peroxide, benzoyl peroxide, benzoyltoluyl peroxide, and toluyl peroxide; peresters such as t-butyl peracetate, t-butyl peroxyoctoate, and t-butyl peroxybenzoate; ketone peroxides; peroxycarbonates; peroxyketals such as 1,1-di(t-amylperoxy)cyclohexane; 2,2'-azobis(2,4-dimethylvaleronitrile), 2,2'-azobis(isobutyronitrile), and 2,2'-azobis(2-methylbutyronitrile). azonitrile compounds such as 2,2'-azobis(4-methoxy-2,4-dimethylvaleronitrile); azoamide compounds such as 2,2'-azobis{2-methyl-N-[1,1-bis(hydroxymethyl)-2-hydroxyethyl]propionamide}; azoamidine compounds such as 2,2'-azobis(2-amidinopropane) dihydrochloride and 2,2'-azobis[2-(2-imidazolin-2-yl)propane] dihydrochloride; azoalkane compounds such as 2,2'-azobis(2,4,4-trimethylpentane) and 4,4'-azobis(4-cyanopentanoic acid); azo compounds having an oxime skeleton such as 2,2'-azobis(2-methylpropionamide oxime); and azo compounds such as dimethyl 2,2'-azobis(isobutyrate).

[0124] The thermal radical generator is preferably one that is active at medium temperatures. Specifically, the 10-hour half-life temperature T10 (°C) of the thermal radical generator is preferably in the range of 50°C to 110°C, more preferably in the range of 50°C to 100°C, and even more preferably in the range of 50°C to 95°C. Examples of commercially available thermal radical generators that are active at medium temperatures include "Luperox 531M80" manufactured by Arkema Fuji Co., Ltd., "Perhexyl (registered trademark) O" manufactured by NOF Corporation, and "MAIB" manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.

[0125] As the (F) radical generator, a thermal radical generator is preferred in which the difference ΔT (°C) between the mold temperature Tc (°C) during compression molding and the 10-hour half-life temperature T10 (°C) of the thermal radical generator falls within a specific range. Specifically, the range of the temperature difference ΔT (°C) is preferably 20°C or more, more preferably 30°C or more, and preferably 80°C or less. Therefore, when the mold temperature Tc (°C) used during compression molding is known, it is preferable to use a thermal radical generator in which the temperature difference ΔT (°C) falls within the above range.

[0126] The amount of (F) radical generator is preferably 0.001% by mass or more, more preferably 0.01% by mass or more, even more preferably 0.05% by mass or more, relative to 100% by mass of nonvolatile components in the resin composition, and is preferably 5% by mass or less, more preferably 2% by mass or less, even more preferably 1% by mass or less.

[0127] The amount of (F) radical generator is preferably 0.01% by mass or more, more preferably 0.1% by mass or more, even more preferably 0.2% by mass or more, relative to 100% by mass of the resin component in the resin composition, and is preferably 5% by mass or less, more preferably 2% by mass or less, even more preferably 1% by mass or less.

[0128] <(G) Curing accelerator> The resin composition according to this embodiment may contain a (G) curing accelerator as an optional component. The (G) curing accelerator acts as a catalyst for the reaction of the (A) epoxy resin, thereby accelerating the curing of the resin composition. The (G) curing accelerator as the (G) component does not include those corresponding to the above-mentioned components (A) to (F). Furthermore, the (G) curing accelerator may be used alone or in combination of two or more types.

[0129] Examples of the (G) curing accelerator include phosphorus-based curing accelerators, urea-based curing accelerators, guanidine-based curing accelerators, imidazole-based curing accelerators, metal-based curing accelerators, and amine-based curing accelerators.

[0130] Examples of the phosphorus-based curing accelerator include aliphatic phosphonium salts such as tetrabutylphosphonium bromide, tetrabutylphosphonium chloride, tetrabutylphosphonium acetate, tetrabutylphosphonium decanoate, tetrabutylphosphonium laurate, bis(tetrabutylphosphonium)pyromellitate, tetrabutylphosphonium hydrogenhexahydrophthalate, tetrabutylphosphonium 2,6-bis[(2-hydroxy-5-methylphenyl)methyl]-4-methylphenolate, and di-tert-butyldimethylphosphonium tetraphenylborate; methyltriphenylphosphonium bromide, ethyltriphenylphosphonium bromide, propyltriphenylphosphonium bromide, butyltriphenylphosphonium bromide, benzyltriphenylphosphonium chloride, tetraphenylphosphonium bromide, p-tolyltriphenylphosphonium tetra-p-tolylborate, and tetraphenylphosphonium tetra-p-tolylborate. aromatic phosphonium salts such as tetraphenylborate, tetraphenylphosphonium tetra-p-tolylborate, triphenylethylphosphonium tetraphenylborate, tris(3-methylphenyl)ethylphosphonium tetraphenylborate, tris(2-methoxyphenyl)ethylphosphonium tetraphenylborate, (4-methylphenyl)triphenylphosphonium thiocyanate, tetraphenylphosphonium thiocyanate, and butyltriphenylphosphonium thiocyanate; aromatic phosphine-borane complexes such as triphenylphosphine-triphenylborane; aromatic phosphine-quinone adducts such as triphenylphosphine-p-benzoquinone adduct; aliphatic phosphines such as tributylphosphine, tri-tert-butylphosphine, trioctylphosphine, di-tert-butyl(2-butenyl)phosphine, di-tert-butyl(3-methyl-2-butenyl)phosphine, and tricyclohexylphosphine;Dibutylphenylphosphine, di-tert-butylphenylphosphine, methyldiphenylphosphine, ethyldiphenylphosphine, butyldiphenylphosphine, diphenylcyclohexylphosphine, triphenylphosphine, tri-o-tolylphosphine, tri-m-tolylphosphine, tri-p-tolylphosphine, tris(4-ethylphenyl)phosphine, tris(4-propylphenyl)phosphine, tris(4-isopropylphenyl)phosphine, tris(4-butylphenyl)phosphine, tris(4-tert-butylphenyl)phosphine, tris(2,4-dimethylphenyl)phosphine, tris(2,5-dimethylphenyl)phosphine, tris(2,6-dimethylphenyl)phosphine aromatic phosphines such as benzene, tris(3,5-dimethylphenyl)phosphine, tris(2,4,6-trimethylphenyl)phosphine, tris(2,6-dimethyl-4-ethoxyphenyl)phosphine, tris(2-methoxyphenyl)phosphine, tris(4-methoxyphenyl)phosphine, tris(4-ethoxyphenyl)phosphine, tris(4-tert-butoxyphenyl)phosphine, diphenyl-2-pyridylphosphine, 1,2-bis(diphenylphosphino)ethane, 1,3-bis(diphenylphosphino)propane, 1,4-bis(diphenylphosphino)butane, 1,2-bis(diphenylphosphino)acetylene, and 2,2'-bis(diphenylphosphino)diphenyl ether;

[0131] Examples of the urea-based curing accelerator include 1,1-dimethylurea; aliphatic dimethylureas such as 1,1,3-trimethylurea, 3-ethyl-1,1-dimethylurea, 3-cyclohexyl-1,1-dimethylurea, and 3-cyclooctyl-1,1-dimethylurea; 3-phenyl-1,1-dimethylurea, 3-(4-chlorophenyl)-1,1-dimethylurea, 3-(3,4-dichlorophenyl)-1,1-dimethylurea, 3-(3-chloro-4-methylphenyl)-1,1-dimethylurea, 3-(2-methylphenyl)-1,1-dimethylurea, 3-(4-methylphenyl)-1,1-dimethylurea, and 3-(3,4-dimethylphenyl)-1,1-dimethylurea. aromatic dimethylureas such as toluene bis(dimethylurea), 3-(4-isopropylphenyl)-1,1-dimethylurea, 3-(4-methoxyphenyl)-1,1-dimethylurea, 3-(4-nitrophenyl)-1,1-dimethylurea, 3-[4-(4-methoxyphenoxy)phenyl]-1,1-dimethylurea, 3-[4-(4-chlorophenoxy)phenyl]-1,1-dimethylurea, 3-[3-(trifluoromethyl)phenyl]-1,1-dimethylurea, N,N-(1,4-phenylene)bis(N',N'-dimethylurea), and N,N-(4-methyl-1,3-phenylene)bis(N',N'-dimethylurea) [toluene bisdimethylurea].

[0132] Examples of guanidine curing accelerators include dicyandiamide, 1-methylguanidine, 1-ethylguanidine, 1-cyclohexylguanidine, 1-phenylguanidine, 1-(o-tolyl)guanidine, dimethylguanidine, diphenylguanidine, trimethylguanidine, tetramethylguanidine, pentamethylguanidine, 1,5,7-triazabicyclo[4.4.0]dec-5-ene, 7-methyl-1,5,7-triazabicyclo[4.4.0]dec-5-ene, 1-methylbiguanide, 1-ethylbiguanide, 1-n-butylbiguanide, 1-n-octadecylbiguanide, 1,1-dimethylbiguanide, 1,1-diethylbiguanide, 1-cyclohexylbiguanide, 1-allylbiguanide, 1-phenylbiguanide, and 1-(o-tolyl)biguanide.

[0133] Examples of the imidazole curing accelerator include 2-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, 1-benzyl-2-methylimidazole, and 1-benzyl-2-methylimidazole. Phenylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2-ethyl-4-methylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2-phenylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6-[2'-methylimidazolyl -(1')]-ethyl-s-triazine, 2,4-diamino-6-[2'-undecylimidazolyl-(1')]-ethyl-s-triazine, 2,4-diamino-6-[2'-ethyl-4'-methylimidazolyl-(1')]-ethyl-s-triazine, 2,4-diamino-6-[2'-methylimidazolyl-(1')]-ethyl-s-triazine isocyanuric acid adduct, 2-phenylimidazole isocyanuric acid adduct Examples of imidazole compounds include 2-phenyl-4,5-dihydroxymethylimidazole, 2-phenyl-4-methyl-5-hydroxymethylimidazole, 2,3-dihydro-1H-pyrrolo[1,2-a]benzimidazole, 1-dodecyl-2-methyl-3-benzylimidazolium chloride, 2-methylimidazoline, and 2-phenylimidazoline, as well as adducts of imidazole compounds with epoxy resins. Commercially available imidazole curing accelerators include "1B2PZ," "2E4MZ," "2MZA-PW," "2MZ-OK," "2MA-OK," "2MA-OK-PW," "2PHZ," "2PHZ-PW," "Cl1Z," "Cl1Z-CN," "Cl1Z-CNS," and "C11Z-A" manufactured by Shikoku Chemicals Corporation; and "P200-H50" manufactured by Mitsubishi Chemical Corporation.

[0134] Examples of metal-based curing accelerators include organometallic complexes or organometallic salts of metals such as cobalt, copper, zinc, iron, nickel, manganese, and tin. Specific examples of organometallic complexes include organic cobalt complexes such as cobalt(II) acetylacetonate and cobalt(III) acetylacetonate, organic copper complexes such as copper(II) acetylacetonate, organic zinc complexes such as zinc(II) acetylacetonate, organic iron complexes such as iron(III) acetylacetonate, organic nickel complexes such as nickel(II) acetylacetonate, and organic manganese complexes such as manganese(II) acetylacetonate. Examples of organometallic salts include zinc octoate, tin octoate, zinc naphthenate, cobalt naphthenate, tin stearate, and zinc stearate.

[0135] Examples of the amine curing accelerator include trialkylamines such as triethylamine and tributylamine, 4-dimethylaminopyridine, benzyldimethylamine, 2,4,6-tris(dimethylaminomethyl)phenol, 1,8-diazabicyclo(5,4,0)-undecene, etc. Commercially available amine curing accelerators may be used, such as "MY-25" manufactured by Ajinomoto Fine-Techno Co., Inc.

[0136] The amount of (G) curing accelerator is preferably 0.001% by mass or more, more preferably 0.01% by mass or more, even more preferably 0.1% by mass or more, relative to 100% by mass of non-volatile components in the resin composition, and is preferably 5% by mass or less, more preferably 2% by mass or less, even more preferably 1% by mass or less.

[0137] The amount of (G) curing accelerator is preferably 0.01% by mass or more, more preferably 0.1% by mass or more, even more preferably 0.5% by mass or more, relative to 100% by mass of the resin component in the resin composition, and is preferably 10% by mass or less, more preferably 5% by mass or less, even more preferably 3% by mass or less.

[0138] <(H) Optional Additives> The resin composition according to the present embodiment may further contain (H) an optional additive as an optional component. The (H) optional additive as the (H) component does not include those corresponding to the above-mentioned components (A) to (G). Examples of the (H) optional additive include thermoplastic resins; organic fillers; organometallic compounds such as organocopper compounds, organozinc compounds, and organocobalt compounds; resin additives such as thickeners, antifoaming agents, leveling agents, and flame retardants; colorants; and the like. One type of the (H) optional additive may be used alone, or two or more types may be used in combination.

[0139] Examples of colorants include phthalocyanine blue, phthalocyanine green, iodine green, diazo yellow, crystal violet, carbon black, naphthalene black, etc. The amount of colorant is preferably 0.001% by mass or more, more preferably 0.01% by mass or more, and even more preferably 0.1% by mass or more, relative to 100% by mass of nonvolatile components in the resin composition, and is preferably 5% by mass or less, more preferably 1% by mass or less, and even more preferably 0.5% by mass or less.

[0140] <(I) Solvent> The resin composition according to this embodiment may further contain (I) a solvent as an optional volatile component in addition to the non-volatile components (A) to (H) described above. The (I) solvent is typically an organic solvent. Examples of the organic solvent include ketone-based solvents such as acetone, methyl ethyl ketone, methyl isobutyl ketone, and cyclohexanone; ester-based solvents such as methyl acetate, ethyl acetate, butyl acetate, isobutyl acetate, isoamyl acetate, methyl propionate, ethyl propionate, and γ-butyrolactone; ether-based solvents such as tetrahydropyran, tetrahydrofuran, 1,4-dioxane, diethyl ether, diisopropyl ether, dibutyl ether, diphenyl ether, and anisole; alcohol-based solvents such as methanol, ethanol, propanol, butanol, and ethylene glycol; 2-ethoxyethyl acetate, propylene glycol monomethyl ether acetate, diethylene glycol monoethyl ether acetate, ethyl diglycol acetate, γ-butyrolactone, and methyl methoxypropionate. Examples of suitable solvents include ether ester solvents such as ethyl acetate; ester alcohol solvents such as methyl lactate, ethyl lactate, and methyl 2-hydroxyisobutyrate; ether alcohol solvents such as 2-methoxypropanol, 2-methoxyethanol, 2-ethoxyethanol, propylene glycol monomethyl ether, and diethylene glycol monobutyl ether (butyl carbitol); amide solvents such as N,N-dimethylformamide, N,N-dimethylacetamide, and N-methyl-2-pyrrolidone; sulfoxide solvents such as dimethyl sulfoxide; nitrile solvents such as acetonitrile and propionitrile; aliphatic hydrocarbon solvents such as hexane, cyclopentane, cyclohexane, and methylcyclohexane; and aromatic hydrocarbon solvents such as benzene, toluene, xylene, ethylbenzene, and trimethylbenzene. (I) The solvents may be used singly or in combination of two or more.

[0141] The amount of (I) solvent is preferably small. The amount of (I) solvent in the resin composition is preferably 10% by mass or less, more preferably 5% by mass or less, even more preferably 1% by mass or less, even more preferably 0.5% by mass or less, and even more preferably 0.1% by mass or less, relative to 100% by mass of the total amount of the resin composition. The lower limit may be 0% by mass or may be 0.0001% by mass or more.

[0142] <Method of manufacturing resin composition> The resin composition according to this embodiment can be produced, for example, by mixing components that can be contained in the resin composition. Therefore, the resin composition can be produced by a production method that includes a step of mixing components (A) to (D). This production method may also include a step of mixing optional components such as components (E) to (I). Components (A) to (I) may be mixed in part or all at the same time, or they may be mixed sequentially.

[0143] When producing a resin composition containing an inorganic filler (E) surface-treated with a surface treatment agent, the resin composition is preferably produced by a production method including the steps of: mixing the surface treatment agent with an inorganic filler (usually particles of an inorganic material) before surface treatment to obtain a surface-treated inorganic filler (E); and mixing the surface-treated inorganic filler (E) with other components. Generally, the surface treatment agent is adsorbed to the inorganic material particles of the inorganic filler (E), and therefore all or most of it does not become free in the resin components.

[0144] Furthermore, when producing a resin composition containing a silane coupling agent (D) that is not adsorbed to inorganic material particles but is free in the resin component, the method for producing a resin composition may include a step of mixing the silane coupling agent (D) simultaneously with or after mixing the inorganic filler (E) with components other than the inorganic filler (E). Since part or all of the silane coupling agent (D) mixed in this way is not adsorbed to the inorganic material particles, a resin composition containing a free silane coupling agent (D) in the resin component can be produced.

[0145] In the method for producing the resin composition, the temperature may be appropriately set during the process of mixing the components, and thus heating and / or cooling may be performed temporarily or throughout the process. Furthermore, stirring or shaking may be performed during the process of mixing the components.

[0146] <Physical properties of resin composition and its cured product> There are no limitations on the state of the resin composition according to this embodiment. The resin composition may be, for example, liquid or solid. As a specific example, the resin composition may be a liquid paste. Hereinafter, a liquid resin composition may be referred to as a "resin paste." A resin paste can generally have a low viscosity. In one example, the viscosity of the resin paste at 25°C may range from 20 Pa·s to 1000 Pa·s. From the viewpoint of suppressing the generation of voids, the loss on heating of the resin paste is preferably 5% or less.

[0147] The resin composition may also be in a solid state. Generally, a solid resin composition is formed into a molded article having a shape appropriate for its intended use. Examples of such a molded article include a sheet, a powder, granules, and pellets. These molded articles usually contain only the resin composition. These molded articles can be produced by an appropriate molding method such as compression molding.

[0148] By curing the resin composition according to this embodiment, a cured product of the resin composition can be obtained. This cured product can then be used to form a sealing layer and an insulating layer of a circuit board. Since heat is typically applied during curing of the resin composition, volatile components such as (I) the solvent, among the components contained in the resin composition, can volatilize due to the heat during curing. Therefore, the cured product obtained by curing the resin composition can contain non-volatile components such as components (A) to (H) or their reaction products.

[0149] The resin composition according to this embodiment can produce a cured product with excellent chemical resistance. Specifically, the cured product of the resin composition according to this embodiment can have high resistance to alkaline solutions. For example, a chemical resistance evaluation test can be performed by immersing the cured product in a strong alkaline solution at 70°C for one hour, then washing with distilled water and drying at 130°C for one hour. In this case, the amount of thickness loss of the cured product can be reduced. In one example, the amount of thickness loss is preferably 50 μm or less, more preferably 30 μm or less. When the sample is a resin composition before curing, the resin composition can be molded onto a silicon wafer by compression molding at a temperature of 130°C, a pressure of 6 MPa, and a cure time of 10 minutes, and then thermally cured at 150°C for 60 minutes to obtain a cured product sample, and the chemical resistance evaluation test can be performed. A specific method for evaluating chemical resistance can be the method described in "Test 1. Chemical Resistance Evaluation Test" in the Examples below.

[0150] The resin composition according to this embodiment can generally suppress the formation of flow marks. Therefore, when the resin composition is molded by compression molding, the formation of flow marks in the molded resin composition and its cured product can be suppressed. "Flow marks" refer to traces of flow formed by the flow of the resin composition during molding. For example, the resin composition is molded onto a silicon wafer by compression molding at a temperature of 130°C, a pressure of 6 MPa, and a cure time of 10 minutes, and then thermally cured to form a cured product. In this case, the area of flow marks formed on the surface of the cured product can be reduced, and preferably the area occupied by flow marks can be reduced to less than 20% of the 100% area of the cured product. A specific method for evaluating flow marks can be the method described in "Test 2. Flow Mark Evaluation Test" in the Examples below.

[0151] The cured product of the resin composition according to this embodiment can usually have excellent dielectric properties, specifically, a low dielectric loss tangent Df. In one example, the dielectric loss tangent Df of the cured product is preferably 0.020 or less, more preferably 0.010 or less, and even more preferably 0.005 or less. There is no particular lower limit, and the dielectric loss tangent can be, for example, 0.0001 or more. The dielectric loss tangent can be measured by a cavity resonance perturbation method at a measurement frequency of 5.8 GHz and a measurement temperature of 23°C. When the sample is a resin composition before curing, the resin composition may be thermally cured at 150°C for 60 minutes to obtain a cured product, and the dielectric loss tangent of the cured product may be measured.

[0152] <Applications of resin composition> The resin composition according to this embodiment can be used, for example, as an insulating layer-forming resin composition for forming an insulating layer or a sealing layer-forming resin composition for forming a sealing layer. The insulating layer and sealing layer are cured layers formed by the cured product of the resin composition, and therefore contain the cured product, and usually contain only the cured product. These insulating layers and sealing layers are preferably applied to circuit boards such as printed wiring boards and semiconductor chip packages, taking advantage of the excellent dielectric properties of the cured product.

[0153] The resin composition according to this embodiment can have excellent chemical resistance. Therefore, it is preferable to use the resin composition in applications where its chemical resistance can be utilized. For example, a conductor layer may be formed on the sealing layer and insulating layer of a circuit board, and chemicals such as alkaline solutions may be used in the process of forming the conductor layer. Therefore, the resin composition according to this embodiment is preferably used to form the sealing layer or conductor layer on which the conductor layer is formed, as described above. Specifically, the resin composition according to this embodiment may be used to form the sealing layer and rewiring formation layer of a semiconductor chip package, as well as the interlayer insulating layer of a printed wiring board. Unless otherwise specified, the term "rewiring formation layer" refers to the insulating layer on which a rewiring layer as a conductor layer is formed on the insulating layer.

[0154] Furthermore, since the resin composition according to this embodiment can generally suppress the formation of flow marks, it is preferably used as a resin composition for molding, and more preferably as a resin composition for compression molding. Even when used for these molding applications, the resin composition according to this embodiment can suppress the formation of flow marks and produce a cured product with a good appearance. As a specific example, the resin composition according to this embodiment may be used as a resin composition for forming a cured product layer by compression molding. The cured product layer thus formed can function as the insulating layer or sealing layer described above.

[0155] The resin composition according to the present embodiment may be used for applications other than those described above, such as a resin sheet, a solder resist, an underfill material, a die bonding material, a hole filling resin, and a component embedding resin.

[0156] <Resin sheet> A resin sheet according to one embodiment of the present invention includes a support and a resin composition layer formed on the support. The resin composition layer contains the resin composition described above, and preferably contains only the resin composition described above.

[0157] From the viewpoint of thinning, the thickness of the resin composition layer provided in the resin sheet is preferably 600 μm or less, more preferably 500 μm or less, even more preferably 400 μm or less, even more preferably 300 μm or less, even more preferably 200 μm or less, and even more preferably 100 μm or less. The lower limit of the thickness of the resin composition layer can be, for example, 1 μm or more, 3 μm or more, 5 μm or more, 10 μm or more, 50 μm or more, etc.

[0158] Examples of the support include plastic film, metal foil, and release paper, with plastic film and metal foil being preferred.

[0159] When a film of a plastic material is used as the support, examples of the plastic material include polyesters such as polyethylene terephthalate (hereinafter sometimes abbreviated as "PET") and polyethylene naphthalate (hereinafter sometimes abbreviated as "PEN"), polycarbonate (hereinafter sometimes abbreviated as "PC"), acrylics such as polymethyl methacrylate (PMMA), cyclic polyolefins, triacetyl cellulose (TAC), polyether sulfide (PES), polyether ketone, polyimide, etc. Among these, polyethylene terephthalate and polyethylene naphthalate are preferred, with inexpensive polyethylene terephthalate being particularly preferred.

[0160] When a metal foil is used as the support, examples of the metal foil include copper foil and aluminum foil, with copper foil being preferred. The copper foil may be a foil made of a single metal, copper, or an alloy of copper and another metal (e.g., tin, chromium, silver, magnesium, nickel, zirconium, silicon, titanium, etc.).

[0161] The surface of the support that is to be bonded to the resin composition layer may be subjected to a surface treatment such as matte treatment, corona treatment, or antistatic treatment.

[0162] The support may be a support with a release layer, which has a release layer on the surface that bonds with the resin composition layer. Examples of the release agent used in the release layer of the support with a release layer include one or more release agents selected from the group consisting of alkyd-based release agents, polyolefin-based release agents, urethane-based release agents, and silicone-based release agents. Commercially available products may be used as the support with a release layer, including PET films having a release layer primarily composed of a silicone-based release agent or an alkyd resin-based release agent, such as "PET501010," "SK-1," "AL-5," and "AL-7" manufactured by Lintec Corporation; "Lumirror T60" manufactured by Toray Industries, Inc.; "Purex" manufactured by Teijin Limited; and "Uni-Peel" manufactured by Unitika Limited.

[0163] The thickness of the support is not particularly limited, but is preferably 1 μm or more, more preferably 5 μm or more, even more preferably 10 μm or more, and is preferably 75 μm or less, more preferably 60 μm or less, even more preferably 50 μm or less. When a support with a release layer is used, it is preferable that the thickness of the entire support with a release layer is within the above range.

[0164] The resin sheet may include any optional member as needed. For example, the resin sheet may include a protective film for protecting the resin composition layer. The protective film is usually provided on the surface of the resin composition layer that is not bonded to the support (i.e., the surface opposite to the support). The thickness of the protective film is not particularly limited, but is, for example, 1 μm to 40 μm. When the protective film is provided, adhesion of dust and scratches to the surface of the resin composition layer can be suppressed.

[0165] The resin sheet can be produced, for example, by a method including forming a resin composition layer on a support. Specifically, the resin sheet can be produced by applying a liquid (varnish-like) resin composition directly or by mixing a solvent and the resin composition to prepare a liquid (varnish-like) resin composition, applying the liquid (varnish-like) resin composition to a support, and then drying it as necessary to form a resin composition layer. The solvent may be the same as the (I) solvent described as a component of the resin composition.

[0166] The resin composition can be applied using a coating device such as a die coater. Drying can be performed by a drying method such as heating or hot air blowing. The drying conditions are not particularly limited, but drying is typically performed so that the solvent content in the resin composition layer is 10% by mass or less, preferably 5% by mass or less. Although this may vary depending on the boiling point of the solvent, for example, when a resin composition containing 30% by mass to 60% by mass of solvent is used, a resin composition layer can be formed by drying at 50°C to 150°C for 3 to 10 minutes.

[0167] The produced resin sheet can be stored by being wound up in a roll. When the resin sheet has a protective film, the resin sheet can usually be used by peeling off the protective film.

[0168] The resin sheet can be used for the same purposes as the above-mentioned resin composition. Therefore, the resin sheet can be used, for example, as a resin sheet for forming an insulating layer or a sealing layer, and is preferably used as a resin sheet for forming an insulating layer or a sealing layer of a circuit board. From the viewpoint of utilizing the excellent chemical resistance of the resin composition, the insulating layer or sealing layer may be formed as a sealing layer and a rewiring formation layer of a semiconductor chip package, and an interlayer insulating layer of a printed wiring board. Furthermore, from the viewpoint of utilizing the advantage of being able to suppress the formation of flow marks, the resin sheet is preferably used in a molding method such as a compression molding method.

[0169] <Circuit board> A circuit board according to one embodiment of the present invention comprises a cured product of the resin composition described above. Typically, the circuit board comprises a cured product layer, which comprises a cured product of the resin composition. The cured product layer may comprise only a cured product of the resin composition. The cured product layer can function as one or both of an insulating layer and a sealing layer. The thickness of the cured product layer is not particularly limited and may be, for example, in the same range as the thickness of the resin composition layer provided in the resin sheet. Furthermore, the cured product layer can typically have properties similar to those of the cured product of the resin composition described above.

[0170] The circuit board may be, for example, Step (I) of forming a resin composition layer; a step (II) of curing the resin composition layer; The composition can be produced by a production method including the steps of:

[0171] In step (I), a resin composition layer is typically formed on a suitable substrate. The formed resin composition layer contains the above-mentioned resin composition, preferably containing only the resin composition. For example, an inner layer substrate may be used as the substrate. The "inner layer substrate" refers to a member that serves as the base material for a circuit board, and examples include glass epoxy substrates, metal substrates (stainless steel, cold-rolled steel sheet (SPCC), etc.), polyester substrates, polyimide substrates, BT resin substrates, and thermosetting polyphenylene ether substrates. The inner layer substrate may also have a conductor layer on one or both sides. The conductor layer provided on the inner layer substrate may be patterned. An inner layer substrate having a conductor layer (circuit) formed on one or both sides of the substrate may be referred to as an "inner layer circuit substrate." Furthermore, the term "inner layer substrate" also includes intermediate products on which an insulating layer and / or a conductor layer should be further formed during the production of a circuit board. Furthermore, an inner layer substrate provided with components such as semiconductor chips may also be used.

[0172] Furthermore, for example, a removable temporary substrate may be used as the substrate. Specifically, a component may be temporarily fixed onto the removable temporary substrate, and a resin composition layer may be formed to embed the component. In this case, the resin composition layer is cured in step (II) described below to form a cured product layer, and then the temporary substrate is removed, thereby obtaining a cured product layer with the component embedded therein. Such a removable temporary substrate can be produced, for example, by laminating a substrate and a temporary fixing film. Examples of the substrate include silicon wafers; glass wafers; glass substrates; metal substrates such as copper, titanium, stainless steel, and cold-rolled steel sheets (SPCC); substrates such as FR-4 substrates in which glass fibers are impregnated with epoxy resin or the like and then thermally cured; and substrates made of bismaleimide triazine resins such as BT resin. Furthermore, the temporary fixing film may be a film that can be peeled from the component and temporarily fix the component, such as "Riva Alpha" manufactured by Nitto Denko Corporation.

[0173] The resin composition layer may be formed, for example, by a coating method including applying a resin composition to a substrate and drying it as necessary. Alternatively, the resin composition layer may be formed, for example, by a lamination method in which a substrate and a resin sheet are laminated together so that the substrate and the resin composition layer are bonded. From the viewpoint of utilizing the advantage of being able to suppress the formation of flow marks, the resin composition layer is preferably formed by a compression molding method.

[0174] In the compression molding method, a resin composition is usually placed in a mold, and pressure and, if necessary, heat are applied to the resin composition in the mold to form a resin composition layer. When a resin composition layer is formed on a substrate, the substrate may also be placed in the mold. The resin composition placed in the mold may be in a liquid state or a solid state. Therefore, the resin composition placed in the mold may be, for example, a resin paste, a powder of the resin composition, granules of the resin composition, pellets of the resin composition, or the like. Alternatively, the above-mentioned resin sheet may be placed in the mold.

[0175] Compression molding may be performed, for example, as follows: An upper mold and a lower mold are prepared as molds for compression molding. A resin composition is placed on a substrate. The substrate on which the resin composition is placed is attached to the lower mold. Thereafter, the upper and lower molds are clamped together, and heat and pressure are applied to the resin composition to perform compression molding.

[0176] Compression molding may be performed, for example, as follows: An upper mold and a lower mold are prepared as molds for compression molding. A resin composition is placed on the lower mold. A substrate is attached to the upper mold. The upper and lower molds are then clamped together so that the resin composition placed on the lower mold is in contact with the substrate attached to the upper mold, and heat and pressure are applied to perform compression molding.

[0177] Furthermore, the compression molding method may be carried out by, for example, discharging the resin composition filled in a cartridge into a mold, and applying heat and pressure to the resin composition in the mold to perform compression molding.

[0178] Molding conditions vary depending on the composition of the resin composition, but for example, the mold temperature during molding is preferably 80°C or higher, more preferably 100°C or higher, even more preferably 120°C or higher, and preferably 200°C or lower, more preferably 170°C or lower, and even more preferably 150°C or lower. The pressure applied during molding is preferably 1 MPa or higher, more preferably 3 MPa or higher, even more preferably 5 MPa or higher, and preferably 50 MPa or lower, more preferably 30 MPa or lower, and even more preferably 20 MPa or lower. The cure time is preferably 1 minute or longer, more preferably 2 minutes or longer, even more preferably 5 minutes or longer, and preferably 60 minutes or shorter, more preferably 30 minutes or shorter, and even more preferably 20 minutes or shorter.

[0179] The method for producing a circuit board according to this example includes a step (II) of curing the resin composition layer after the step (I). By curing the resin composition layer in the step (II), a cured material layer containing a cured product of the resin composition can be formed.

[0180] The resin composition layer is usually cured by thermal curing. The thermal curing conditions for the resin composition layer may vary depending on the type of resin composition. For example, the curing temperature is preferably 120°C to 240°C, more preferably 130°C to 220°C, and even more preferably 140°C to 210°C. The curing time is preferably 5 minutes to 120 minutes, more preferably 10 minutes to 100 minutes, and even more preferably 15 minutes to 100 minutes.

[0181] The method for producing a circuit board may include preheating the resin composition layer at a temperature lower than the curing temperature before thermally curing the resin composition layer. For example, prior to thermally curing the resin composition layer, the resin composition layer may be preheated for typically 5 minutes or more, preferably 5 minutes to 150 minutes, more preferably 15 minutes to 120 minutes, and even more preferably 15 minutes to 100 minutes, at a temperature of typically 50°C to 150°C, preferably 60°C to 140°C, and more preferably 70°C to 130°C. Preheating is usually performed after step (I).

[0182] The method for producing a circuit board may further include any step in combination with the above steps (I) and (II).

[0183] The method for producing a circuit board may include, for example, step (III) of forming holes such as via holes or through holes in the cured material layer after step (II). The method for forming the holes may be selected depending on factors such as the composition of the resin composition used to form the cured material layer. For example, holes may be formed by processing methods such as drilling, laser processing, and plasma processing, with laser processing being preferred. The dimensions and shape of the holes may be determined appropriately depending on the design of the circuit board.

[0184] The method for manufacturing a circuit board may include, for example, step (IV) of subjecting the cured material layer to a roughening treatment. The roughening treatment can roughen the surface of the cured material layer. Furthermore, the roughening treatment can remove smears (resin residues) from the cured material layer. Therefore, this roughening treatment is sometimes called a "desmear treatment." When holes are formed in step (III), smears may form in the holes. Therefore, it is preferable to perform the roughening treatment of step (IV) after step (III) to remove the smears.

[0185] The procedure and conditions for the roughening treatment are not particularly limited. For example, the roughening treatment may be performed by subjecting the cured material layer to a swelling treatment using a swelling liquid, an oxidation treatment using an oxidizing agent, and a neutralization treatment using a neutralizing liquid in this order.

[0186] Examples of swelling liquids used in the roughening treatment include alkaline solutions and surfactant solutions, with alkaline solutions being preferred. Sodium hydroxide solutions and potassium hydroxide solutions are more preferred as alkaline solutions. Commercially available swelling liquids include "Swelling Dip Securiganth P" and "Swelling Dip Securiganth SBU" manufactured by Atotech Japan. Swelling treatment with a swelling liquid can be performed, for example, by immersing the cured material layer in the swelling liquid at 30°C to 90°C for 1 to 20 minutes. To keep the swelling of the resin in the cured material layer to an appropriate level, it is preferable to immerse the cured material layer in the swelling liquid at 40°C to 80°C for 5 to 15 minutes.

[0187] Examples of oxidizing agents used in the roughening treatment include alkaline permanganate solutions prepared by dissolving potassium permanganate or sodium permanganate in an aqueous solution of sodium hydroxide. The oxidation treatment using an oxidizing agent such as alkaline permanganate solution is preferably carried out by immersing the cured material layer in an oxidizing agent solution heated to 60°C to 100°C for 10 to 30 minutes. The concentration of permanganate in the alkaline permanganate solution is preferably 5% by mass to 10% by mass. Commercially available oxidizing agents include alkaline permanganate solutions such as "Concentrate Compact CP" and "Dosing Solution Securigance P" manufactured by Atotech Japan.

[0188] The neutralizing solution used in the roughening treatment is preferably an acidic aqueous solution, and a commercially available product such as "Reduction Solution Securigant P" manufactured by Atotech Japan can be cited as an example. Neutralization treatment using a neutralizing solution can be carried out by immersing the surface that has been oxidized with an oxidizing agent in a neutralizing solution at 30°C to 80°C for 5 to 30 minutes. From the standpoint of workability, a preferred method is to immerse the object that has been oxidized with an oxidizing agent in a neutralizing solution at 40°C to 70°C for 5 to 20 minutes.

[0189] The method for producing a circuit board may include step (V) of forming a conductor layer on the cured product layer. When the method for producing a circuit board includes step (III) or (IV), step (V) of forming the conductor layer is preferably carried out after steps (III) and (IV).

[0190] The conductive material used for the conductor layer is not particularly limited. In a preferred embodiment, the conductor layer contains one or more metals selected from the group consisting of gold, platinum, palladium, silver, copper, aluminum, cobalt, chromium, zinc, nickel, titanium, tungsten, iron, tin, and indium. The conductor layer may be a single metal layer or an alloy layer. Examples of alloy layers include layers formed from an alloy of two or more metals selected from the above group (e.g., nickel-chromium alloy, copper-nickel alloy, and copper-titanium alloy). Among these, from the viewpoints of versatility in forming the conductor layer, cost, ease of patterning, etc., single metal layers of chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, or copper, or alloy layers of nickel-chromium alloy, copper-nickel alloy, or copper-titanium alloy are preferred. Single metal layers of chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, or copper, or alloy layers of nickel-chromium alloy are more preferred, and single metal layers of copper are even more preferred.

[0191] The conductor layer may have a single layer structure or a multi-layer structure including two or more single metal or alloy layers made of different types of metals or alloys. When the conductor layer has a multi-layer structure, the layer in contact with the cured material layer is preferably a single metal layer of chromium, zinc, or titanium, or an alloy layer of nickel-chromium alloy.

[0192] The thickness of the conductor layer depends on the design of the circuit board, but is preferably 3 μm to 35 μm, and more preferably 5 μm to 30 μm.

[0193] The conductor layer may be formed by plating. For example, a conductor layer having a desired wiring pattern can be formed by plating the surface of the cured layer using a conventionally known technique such as a semi-additive method or a full-additive method. From the viewpoint of ease of production, the semi-additive method is preferred. An example of forming a conductor layer by a semi-additive method will be described below.

[0194] First, an electroless plated layer (plating seed layer) is formed on the surface of the cured material layer by electroless plating. Next, a mask pattern is formed on the formed electroless plated layer, exposing a portion of the electroless plated layer corresponding to the desired wiring pattern. After forming an electroless plated layer on the exposed electroless plated layer by electrolytic plating, the mask pattern is removed. Thereafter, unnecessary electroless plated layer is removed by etching, thereby forming a conductor layer having the desired wiring pattern.

[0195] When a conductor layer is formed on the cured material layer, the method for producing a circuit board may include performing an annealing treatment after the formation of the conductor layer. Annealing treatment can improve adhesion between the cured material layer and the conductor layer. The annealing treatment can be performed, for example, by heating at 150°C to 210°C for 20 to 180 minutes.

[0196] When a resin sheet is used to form the resin composition layer in step (I), the method for producing a circuit board may include removing the support of the resin sheet after the formation of the resin composition layer. The removal of the support may be performed before step (I), between step (I) and step (II), between step (II) and step (III), between step (III) and step (IV), or between step (IV) and step (V).

[0197] The method for producing a circuit board may include, for example, polishing the surface of the cured layer after forming the cured layer. Specifically, the surface of the cured layer may be polished after step (II), and then steps (III) to (V) may be performed. Examples of polishing methods include chemical mechanical polishing using a chemical mechanical polishing device; and mechanical polishing methods such as belt polishing, buff polishing, ceramic polishing, grinding using a surface grinder, and surface grinding using a rotating grinding wheel.

[0198] In the method for manufacturing a circuit board, each of the above steps may be performed only once or may be repeated two or more times. For example, steps (I) to (V) may be performed repeatedly to manufacture a circuit board having a multilayer structure, such as a multilayer printed wiring board having a plurality of insulating layers and conductor layers.

[0199] Examples of the circuit board according to this embodiment include a printed wiring board and a semiconductor chip package. Examples of the semiconductor chip package include a fan-in package and a fan-out package. Specific examples include an FC-CSP, an MIS-BGA package, an ETS-BGA package, a fan-out wafer level package (WLP), a fan-in WLP, a fan-out panel level package (PLP), and a fan-in PLP. In these semiconductor chip packages, it is preferable to form a sealing layer or a rewiring formation layer using a cured product layer containing a cured product of the resin composition described above. However, the circuit board is not limited to those exemplified here.

[0200] For example, a semiconductor chip package may include a printed wiring board having a cured material layer and a semiconductor chip mounted on the printed wiring board. Alternatively, for example, a semiconductor chip package may include a semiconductor chip and a cured material layer that encapsulates at least a portion of the semiconductor chip. The cured material layer that encapsulates at least a portion of the semiconductor chip can function as an encapsulating layer. Furthermore, these may be combined to obtain a semiconductor chip package that includes a printed wiring board, a semiconductor chip mounted on the printed wiring board, and a cured material layer that encapsulates at least a portion of the semiconductor chip.

[0201] Such a semiconductor chip package can be manufactured by a manufacturing method including a step of bonding a semiconductor chip to a printed wiring board. The bonding conditions between the printed wiring board and the semiconductor chip can be any conditions that allow conductive connection between the terminal electrodes of the semiconductor chip and the circuit wiring of the printed wiring board. For example, the conditions used in flip-chip mounting of semiconductor chips can be used.

[0202] An example of a bonding method is a method in which a semiconductor chip is pressure-bonded to a printed wiring board. Pressure-bonding conditions include a pressure-bonding temperature typically in the range of 120°C to 240°C (preferably in the range of 130°C to 200°C, more preferably in the range of 140°C to 180°C), and a pressure-bonding time typically in the range of 1 second to 60 seconds (preferably in the range of 5 seconds to 30 seconds). Another example of a bonding method is a method in which a semiconductor chip is placed on a printed wiring board and bonded by reflow. Reflow conditions may be in the range of 120°C to 300°C. Bonding may be performed using an insulating adhesive between the semiconductor chip and the printed wiring board.

[0203] Furthermore, the method for manufacturing a semiconductor chip may include, after bonding the semiconductor chip to the printed wiring board, filling a gap between the semiconductor chip and the printed wiring board with an underfill material, in which case the above-mentioned resin composition may be used as the underfill material.

[0204] The method for producing a semiconductor chip may include a step of forming an encapsulating layer as a cured layer that encapsulates at least a portion of the semiconductor chip. The encapsulating layer is usually formed after bonding the semiconductor chip to a printed wiring board. The encapsulating layer can be formed by a method including the above-mentioned steps (I) and (II).

[0205] FIG. 1 is a cross-sectional view schematically illustrating a semiconductor chip package as a circuit board according to an embodiment of the present invention. Another example of a circuit board is a semiconductor chip package 100 including a rewiring formation layer 130 and a rewiring layer 140, as shown in FIG. 1 . The semiconductor chip package 100 includes a semiconductor chip 110; a sealing layer 120 formed to cover the periphery of the semiconductor chip 110; the rewiring formation layer 130 as an insulating layer provided on the surface of the semiconductor chip 110 opposite the sealing layer 120; the rewiring layer 140 as a conductor layer; a solder resist layer 150; and bumps 160. In this example, one or both of the sealing layer 120 and the rewiring formation layer 130 may be formed from a cured material layer containing a cured product of the resin composition described above.

[0206] This semiconductor chip package, for example, (1) A step of laminating a temporary fixing film on a substrate to obtain a temporary base material; (2) A step of temporarily fixing a semiconductor chip onto a temporary fixing film of a temporary substrate; (3) forming an encapsulation layer on the semiconductor chip; (4) peeling the temporary substrate from the semiconductor chip; (5) forming a rewiring formation layer on the surface of the semiconductor chip from which the temporary substrate has been peeled off; and (6) A step of forming a rewiring layer as a conductor layer on the rewiring formation layer. In this manufacturing method, the formation of the sealing layer in step (3) or the formation of the rewiring formation layer in step (5) may be performed by a method including the above-mentioned steps (I) to (II).

[0207] In step (1), a temporary fixing film is laminated on a substrate to obtain a temporary base material. As the substrate and the temporary fixing film, for example, those described above are used.

[0208] In step (2), the semiconductor chip is temporarily fixed on the temporary fixing film of the temporary substrate. Typically, the semiconductor chip is temporarily fixed on the temporary fixing film so that the electrode pad surface of the semiconductor chip is bonded to the temporary fixing film. Temporary fixing of the semiconductor chip can be performed using a known device such as a flip chip bonder or a die bonder. The layout and number of semiconductor chips to be arranged can be appropriately set depending on the shape and size of the temporary fixing film and the desired number of semiconductor chip packages to be produced. For example, the semiconductor chips may be temporarily fixed by arranging them in a matrix of multiple rows and multiple columns.

[0209] In step (3), an encapsulating layer is formed on the semiconductor chip. The encapsulating layer may be formed from a cured material layer using a method including the above-mentioned steps (I) and (II).

[0210] In step (4), the temporary substrate is peeled off from the semiconductor chip. The method for peeling off the release substrate can be appropriately selected depending on the material of the temporary fixing film. Examples include a method in which the temporary fixing film is heated and foamed (or expanded) to peel off, and a method in which the adhesive strength of the temporary fixing film is reduced by irradiating it with ultraviolet light through the substrate to peel off. In the method in which the temporary fixing film is heated and foamed (or expanded) to peel off, the heating conditions are typically 100°C to 250°C for 1 second to 90 seconds or 5 minutes to 15 minutes. In the method in which the adhesive strength of the temporary fixing film is reduced by irradiating it with ultraviolet light to peel off, the irradiation dose of ultraviolet light is typically 10 mJ / cm. 2 ~1000mJ / cm 2 is.

[0211] In step (5), a rewiring formation layer is formed on the surface of the semiconductor chip from which the temporary substrate has been peeled off. The rewiring formation layer may be formed from a cured material layer using a method including the above-mentioned steps (I) and (II). After forming the rewiring formation layer, via holes may be formed in the rewiring formation layer to establish interlayer connection between the semiconductor chip and a conductor layer, which will be described later. The via holes can be formed, for example, by the method described in step (III).

[0212] In step (6), a rewiring layer is formed as a conductor layer on the rewiring formation layer. The rewiring layer can be formed, for example, by the method described in step (V). Steps (5) and (6) may be repeated to alternately stack (build up) conductor layers (rewiring layers) and rewiring formation layers (insulating layers).

[0213] The method for manufacturing a semiconductor chip package may further include the steps of (7) forming a solder resist layer on the conductor layer (rewiring layer), (8) forming bumps, and (9) dicing and singulating the multiple semiconductor chip packages into individual semiconductor chip packages.

[0214] The above-mentioned manufacturing method is a method of first providing a semiconductor chip and then forming a rewiring layer on the electrode pad surface (i.e., chip 1st (Chip-1 st In addition to the chip 1st method, semiconductor chip packages can also be manufactured using a method in which a rewiring layer is first provided, and then a semiconductor chip is provided on the rewiring layer in a state in which the electrode pad surface can be electrically connected to the rewiring layer, and then the semiconductor chip is sealed (i.e., a rewiring layer 1st (RDL-1) method). st The resin composition according to the embodiment described above may be manufactured by Chip-1. st Construction method and RDL-1 st It can be applied regardless of the construction method.

[0215] <Semiconductor device> The circuit board can be used to manufacture a semiconductor device. The semiconductor device includes the circuit board described above. Examples of the semiconductor device include various semiconductor devices used in electrical appliances (e.g., computers, mobile phones, smartphones, tablet devices, wearable devices, digital cameras, medical equipment, and televisions) and vehicles (e.g., motorcycles, automobiles, trains, ships, and aircraft). [Example]

[0216] The present invention will be specifically described below with reference to examples. However, the present invention is not limited to the following examples. In the following description, the units "parts" and "%" used to represent amounts are based on mass unless otherwise specified. Furthermore, the operations described below were carried out in an atmospheric environment at room temperature and normal pressure (23°C, 1 atm) unless otherwise specified.

[0217] <Explanation of inorganic fillers> Inorganic filler 1: Spherical silica surface-treated with a surface treatment agent (Shin-Etsu Chemical Co., Ltd. "KBM573", N-phenyl-3-aminopropyltrimethoxysilane). Average particle size: 0.5 μm, specific surface area: 10 m 2 / g, maximum cut diameter: 5 μm. The amount of the surface treatment agent in 100% by mass of the total amount of inorganic filler 1 was 0.7% by mass.

[0218] Inorganic filler 2: Spherical silica surface-treated with a surface treatment agent (Shin-Etsu Chemical Co., Ltd. "KBM573", N-phenyl-3-aminopropyltrimethoxysilane). Average particle size: 1.2 μm, specific surface area: 4.7 m 2 / g, maximum cut diameter: 3 μm. The amount of the surface treatment agent in 100% by mass of the total amount of the inorganic filler 2 was 0.6% by mass.

[0219] Inorganic filler 3: Spherical silica surface-treated with a surface treatment agent (Shin-Etsu Chemical Co., Ltd. "KBM573", N-phenyl-3-aminopropyltrimethoxysilane). Average particle size: 1.5 μm, specific surface area: 3.5 m 2 / g, maximum cut diameter: 5 μm. The amount of the surface treatment agent in 100% by mass of the total amount of the inorganic filler 3 was 0.5% by mass.

[0220] Example 1 Naphthalene-type epoxy resin (DIC "HP-4032D", 1,6-bis(glycidyloxy)naphthalene, epoxy equivalent approximately 142 g / eq.) 3 parts, glycidylamine-type epoxy resin (ADEKA "EP-3950L", epoxy equivalent 95 g / eq.) 7 parts, thermal radical generator (Arkema Fuji "Luperox 531M80", 10-hour half-life temperature T10: 93.0°C, hydrocarbon solution with 80% peroxide content) 0.15 parts, inorganic filler 1 80 parts, polymerizable alkylene oxide resin (Shin-Nakamura Chemical A resin composition was prepared by uniformly dispersing 4 parts of an acid anhydride curing agent ("M-130G" manufactured by Gakushu Kogyo Co., Ltd., methoxypolyethylene glycol methacrylate), 5 parts of an acid anhydride curing agent ("HN-2200" manufactured by Resonac Corporation, methyltetrahydrophthalic anhydride), 0.1 parts of a silane coupling agent ("KBM-403" manufactured by Shin-Etsu Chemical Co., Ltd., 3-glycidoxypropyltrimethoxysilane), 0.5 parts of a curing accelerator ("2MA-OK-PW" imidazole curing accelerator manufactured by Shikoku Chemical Industry Co., Ltd.), and 0.3 parts of carbon black using a mixer.

[0221] <Example 2> The amount of glycidylamine type epoxy resin (ADEKA Corporation "EP-3950L") was changed to 4 parts. In addition, 3 parts of bisphenol A type epoxy resin (DIC Corporation "EXA-850CRP", epoxy equivalent 172.5 g / eq.) was added. Furthermore, 80 parts of inorganic filler 1 was changed to 80 parts of inorganic filler 2. Apart from the above, a resin composition was produced in the same manner as in Example 1.

[0222] Example 3 The amount of polymerizable alkylene oxide resin ("M-130G" manufactured by Shin-Nakamura Chemical Co., Ltd.) was changed to 2 parts. In addition, 80 parts of inorganic filler 2 was changed to 80 parts of inorganic filler 3. Apart from the above, a resin composition was produced in the same manner as in Example 2.

[0223] Example 4 The amount of acid anhydride curing agent ("HN-2200" manufactured by Resonac Co., Ltd.) was changed to 3 parts. In addition, 80 parts of inorganic filler 2 was changed to 80 parts of inorganic filler 1. Apart from the above, a resin composition was produced in the same manner as in Example 2.

[0224] <Example 5> Three parts of an acid anhydride curing agent ("HN-2200" manufactured by Resonac Corporation) was changed to one part of an amine curing agent ("Kayahard AA" manufactured by Nippon Kayaku Co., Ltd.). In addition, 0.5 parts of a curing accelerator ("2MA-OK-PW" manufactured by Shikoku Chemicals Corporation) was changed to 0.2 parts of a curing accelerator ("2E4MZ" imidazole curing accelerator manufactured by Shikoku Chemicals Corporation). Aside from the above, a resin composition was produced in the same manner as in Example 4.

[0225] Example 6 The amount of naphthalene-type epoxy resin (DIC Corporation, "HP-4032D") was changed to 5 parts. The amount of glycidylamine-type epoxy resin (ADEKA Corporation, "EP-3950L") was also changed to 5 parts. The amount of polymerizable alkylene oxide resin (Shin-Nakamura Chemical Co., Ltd., "M-130G") was also changed to 1.5 parts. The amount of acid anhydride-based curing agent (Resonac Corporation, "HN-2200") was also changed to 3 parts. Apart from the above, a resin composition was produced in the same manner as in Example 3.

[0226] Example 7 80 parts of inorganic filler 1 was changed to 80 parts of inorganic filler 2. In addition, the amount of acid anhydride curing agent ("HN-2200" manufactured by Resonac Co., Ltd.) was changed to 5 parts. Aside from the above, a resin composition was produced in the same manner as in Example 4.

[0227] Example 8 A resin composition was produced in the same manner as in Example 7, except that 4 parts of a polymerizable alkylene oxide resin ("M-130G" manufactured by Shin-Nakamura Chemical Co., Ltd.) was changed to 4 parts of a polymerizable alkylene oxide resin ("BPE-1300N" manufactured by Shin-Nakamura Chemical Co., Ltd., ethoxylated bisphenol A dimethacrylate).

[0228] Example 9 A resin composition was produced in the same manner as in Example 7, except that 4 parts of a polymerizable alkylene oxide resin ("M-130G" manufactured by Shin-Nakamura Chemical Co., Ltd.) was changed to 4 parts of a polymerizable alkylene oxide resin ("M-40G" manufactured by Shin-Nakamura Chemical Co., Ltd., methoxytetraethylene glycol methacrylate).

[0229] Example 10 A resin composition was produced in the same manner as in Example 7, except that 4 parts of a polymerizable alkylene oxide resin ("M-130G" manufactured by Shin-Nakamura Chemical Co., Ltd.) was changed to 4 parts of a polymerizable alkylene oxide resin ("M-20G" manufactured by Shin-Nakamura Chemical Co., Ltd., methoxydiethylene glycol methacrylate).

[0230] Example 11 A resin composition was produced in the same manner as in Example 7, except that 4 parts of a polymerizable alkylene oxide resin ("M-130G" manufactured by Shin-Nakamura Chemical Co., Ltd.) was changed to 4 parts of a polymerizable alkylene oxide resin ("A-3000PER" polyethylene polypropylene glycol diacrylate manufactured by Shin-Nakamura Chemical Co., Ltd.).

[0231] Example 12 A resin composition was produced in the same manner as in Example 7, except that 4 parts of a polymerizable alkylene oxide resin ("M-130G" manufactured by Shin-Nakamura Chemical Co., Ltd.) was changed to 4 parts of a polymerizable alkylene oxide resin ("PHG-1G" manufactured by Shin-Nakamura Chemical Co., Ltd., phenoxyethylene glycol methacrylate).

[0232] Example 13 A resin composition was produced in the same manner as in Example 7, except that 4 parts of a polymerizable alkylene oxide resin ("M-130G" manufactured by Shin-Nakamura Chemical Co., Ltd.) was changed to 4 parts of a polymerizable alkylene oxide resin ("A-LEN-10" manufactured by Shin-Nakamura Chemical Co., Ltd., ethoxylated-o-phenylphenol acrylate).

[0233] <Comparative Example 1> The amount of bisphenol A type epoxy resin (DIC Corporation, "EXA-850CRP") was changed to 2 parts. The amount of naphthalene type epoxy resin (DIC Corporation, "HP-4032D") was changed to 2 parts. The amount of glycidylamine type epoxy resin (ADEKA Corporation, "EP-3950L") was changed to 3 parts. The amount of acid anhydride type curing agent (Resonac Corporation, "HN-2200") was changed to 8 parts. The amount of silane coupling agent (Shin-Etsu Chemical Co., Ltd., "KBM-403") was changed to 0.03 parts. Except for the above changes, the resin composition was produced in the same manner as in Example 7.

[0234] <Comparative Example 2> Bisphenol A type epoxy resin (DIC Corporation, "EXA-850CRP") was not used. In addition, the amount of polymerizable alkylene oxide resin (Shin-Nakamura Chemical Co., Ltd., "M-130G") was changed to 5 parts. Furthermore, the amount of acid anhydride curing agent (Resonac Corporation, "HN-2200") was changed to 7 parts. Apart from the above, a resin composition was produced in the same manner as in Example 4.

[0235] <Test 1. Chemical resistance evaluation test> The resin composition was compression molded onto a 12-inch disk-shaped silicon wafer (thickness: 775 μm) using a compression molding machine (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes). By this compression molding, a resin composition layer having a thickness of 300 μm was formed on the silicon wafer.

[0236] The resin composition layer was then thermally cured by heating at 150°C for 60 minutes to form a cured layer. This resulted in a laminated sample (i.e., a silicon wafer with a cured layer) comprising a silicon wafer and a cured layer formed on the silicon wafer. This laminated sample was cut into squares with sides of 5 cm to obtain multiple test pieces.

[0237] A strong alkaline solution containing 75% dimethyl sulfoxide, 13% glycol derivative, 10% N-methyl-2-pyrrolidone, and 2% tetramethylammonium hydroxide was prepared. The test specimens were immersed in the strong alkaline solution at 70°C for 1 hour. The test specimens were then removed from the strong alkaline solution, washed with distilled water, and dried in an oven at 130°C for 1 hour to obtain test specimens after the chemical immersion test.

[0238] The thickness of the cured layer of the test piece after immersion in the chemical was measured. A thickness of 270 μm or more of the cured layer was judged as "excellent," a thickness of less than 270 μm and 250 μm or more was judged as "good," and a thickness of less than 250 μm was judged as "poor."

[0239] <Test 2. Flow mark evaluation test> The resin composition was compression molded onto a 12-inch disk-shaped silicon wafer (thickness: 775 μm) using a compression molding machine (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes). By this compression molding, a resin composition layer having a thickness of 300 μm was formed on the silicon wafer.

[0240] Thereafter, the resin composition layer was thermally cured by heating at 150°C for 60 minutes to obtain a cured layer. This cured layer was observed and evaluated for flow marks according to the following criteria. "Good": The area of flow marks is less than 20% of the entire surface of the cured layer. "Poor": Flow marks occupy 20% or more of the entire surface area of the cured layer.

[0241] <Result> The results of the Examples and Comparative Examples are shown in the following table. In the table, the abbreviations have the following meanings: "Acid anhydride group / epoxy group": The ratio of the number of active groups (number of acid anhydride groups) in the acid anhydride resin to the number of epoxy groups in the (A) epoxy resin. "Amine active hydrogen / epoxy group": The ratio of the number of active groups (number of amine active hydrogens) in the amine resin to the number of epoxy groups in the (A) epoxy resin. "Silane coupling agent / component (B)": The ratio of the silane coupling agent (including the surface treatment agent) to 100% by mass of the polymerizable alkylene oxide resin (B). "Silane coupling agent / Component (C)": The ratio of silane coupling agent (including surface treatment agent) to 100% by mass of (C) curing agent "A / (B+C)": The ratio of (A) epoxy resin to the total of (B) polymerizable alkylene oxide resin and (C) curing agent (100% by mass)

[0242] [Table 1]

[0243] [Table 2] [Explanation of symbols]

[0244] 100 Semiconductor chip packages 110 Semiconductor Chips 120 sealing layer 130 Rewiring formation layer 140 Redistribution layer 150 solder resist layer 160 Bump

Claims

1. A resin composition comprising (A) an epoxy resin, (B) a resin containing a radically polymerizable unsaturated group and an alkylene oxide structure, (C) a curing agent, and two or more types of (D) silane coupling agents, A resin composition, wherein the amount of component (A) is more than 100% by mass, relative to 100% by mass of the total of components (B) and (C).

2. 2. The resin composition according to claim 1, wherein the ratio of the number of active groups in component (C) to the number of epoxy groups in component (A) is 0.35 or less.

3. The resin composition according to claim 1, further comprising (E) an inorganic filler.

4. The resin composition according to claim 3, wherein the amount of component (E) is 50% by mass or more based on 100% by mass of the nonvolatile components of the resin composition.

5. The resin composition according to claim 1, wherein the amount of the component (D) is 2% by mass or more relative to 100% by mass of the component (B).

6. The resin composition according to claim 1, wherein the amount of the component (D) is 1% by mass or more relative to 100% by mass of the component (C).

7. The resin composition according to claim 1 for forming an insulating layer or a sealing layer.

8. The resin composition according to claim 1 for forming a cured product layer by compression molding.

9. A support and a resin composition layer provided on the support, A resin sheet, wherein the resin composition layer comprises the resin composition according to any one of claims 1 to 8.

10. A cured product of the resin composition according to any one of claims 1 to 8.

11. A circuit board comprising a cured product of the resin composition according to any one of claims 1 to 8.

12. A semiconductor device comprising the circuit board according to claim 11.

13. Step (I) of forming a resin composition layer containing the resin composition according to any one of claims 1 to 8; Step (II) of curing the resin composition layer; A method for manufacturing a circuit board, comprising:

14. The method for producing a circuit board according to claim 13 , wherein step (I) comprises forming a resin composition layer by a compression molding method.

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