resin composition

Abstract

To provide a resin composition that has excellent adhesion and gives a cured product with less warpage, less occurrence of a flow mark after molding, and less occurrence of unevenness on the resin surface after curing; and a circuit board and a semiconductor chip package including the resin composition.SOLUTION: A resin composition contains (A-1) an epoxy resin with an epoxy equivalent of higher than 400 g / eq. and 1500 g / eq. or less, (B) an inorganic filler, and (C) a curing agent. When a nonvolatile component in the resin composition is 100 mass%, the content of (A-1) component is 0.2 mass% or more and less than 3 mass% and the content of (B) component is 70 mass% or more when the nonvolatile component in the resin composition is 100 mass%.SELECTED DRAWING: None

Description

[Technical Field]

[0001] The present invention relates to a resin composition. Furthermore, the present invention relates to a circuit board and a semiconductor chip package using the resin composition. [Background technology]

[0002] In recent years, the demand for high-performance electronic devices such as smartphones and tablet devices has been increasing, and accordingly, the insulating materials used in these small electronic devices are required to have even higher performance. Known examples of such insulating materials include those formed by curing a resin composition (see, for example, Patent Document 1). [Prior art documents] [Patent documents]

[0003] [Patent Document 1] Japanese Patent Application Publication No. 2017-82052 Summary of the Invention [Problem to be solved by the invention]

[0004] In recent years, there has been a demand for smaller semiconductor chip packages, and therefore thinner insulating or sealing layers are required for the semiconductor chip packages. Thinner insulating or sealing layers tend to be more susceptible to warping, so there is a demand for insulating or sealing layers that can suppress warping.

[0005] In order to suppress warping, it is conceivable to add a liquid component or a component that relieves stress to the resin composition.

[0006] However, in this case, the adhesion to the conductor layer or the like may be poor, and flow marks may occur after molding, and unevenness may occur on the resin surface after post-curing.

[0007] The present invention has been made in view of the above-mentioned problems, and aims to provide a resin composition that can give a cured product that has excellent adhesion and is suppressed in warpage, the occurrence of flow marks after molding, and the occurrence of unevenness on the resin surface after post-cure; and a circuit board and a semiconductor chip package that use the resin composition. [Means for solving the problem]

[0008] As a result of extensive research aimed at solving the above-mentioned problems, the present inventors have found that by incorporating a predetermined amount of an epoxy resin having a predetermined epoxy equivalent into a resin composition, it is possible to obtain a cured product that has excellent adhesion and is suppressed in terms of warping, the occurrence of flow marks after molding, and the occurrence of unevenness on the resin surface after post-cure, and have thus completed the present invention.

[0009] That is, the present invention includes the following. [1] (A-1) An epoxy resin having an epoxy equivalent of more than 400 g / eq. and not more than 1500 g / eq. (B) inorganic fillers, and (C) a curing agent, The content of the (A-1) component is 0.2% by mass or more and less than 3% by mass, when the total nonvolatile components in the resin composition is 100% by mass, A resin composition, wherein the content of component (B) is 70% by mass or more when the total nonvolatile components in the resin composition is 100% by mass. [2] The resin composition according to [1], wherein the component (A-1) includes one or more skeletons selected from the group consisting of a fluorene skeleton, a butadiene skeleton, an isoprene skeleton, an alkyleneoxy skeleton, a siloxane skeleton, and a bisphenol skeleton. [3] The resin composition according to [1] or [2], further comprising (A-2) an epoxy resin having an epoxy equivalent of 400 g / eq. or less, or an epoxy resin having an epoxy equivalent of more than 1500 g / eq. [4] The resin composition according to any one of [1] to [3], wherein the component (C) contains an acid anhydride curing agent. [5] The resin composition according to any one of [1] to [4], wherein the resin composition is liquid. [6] The resin composition according to any one of [1] to [5], which is a resin composition for sealing or insulation. [7] A circuit board comprising an insulating layer formed from a cured product of the resin composition according to any one of [1] to [6]. [8] A semiconductor chip package comprising the circuit board according to [7] and a semiconductor chip mounted on the circuit board. [9] A semiconductor chip package comprising a semiconductor chip and a cured product of the resin composition according to any one of [1] to [6] that encapsulates the semiconductor chip. [Effects of the Invention]

[0010] According to the present invention, it is possible to provide a resin composition that can give a cured product that has excellent adhesion and is suppressed in terms of warpage, the occurrence of flow marks after molding, and the occurrence of unevenness on the resin surface after post-cure; and a circuit board and a semiconductor chip package that use the resin composition. DETAILED DESCRIPTION OF THE INVENTION

[0011] The present invention will be described in detail below with reference to embodiments and examples. However, the present invention is not limited to the embodiments and examples described below, and can be implemented with any modifications within the scope of the claims of the present invention and their equivalents.

[0012] [Resin composition] The resin composition of the present invention comprises (A-1) an epoxy resin having an epoxy equivalent greater than 400 g / eq. and less than 1500 g / eq., (B) an inorganic filler, and (C) a curing agent, wherein the content of component (A-1) is 0.2% by mass or more but less than 3% by mass, based on 100% by mass of the nonvolatile components in the resin composition, and the content of component (B) is 70% by mass or more, based on 100% by mass of the nonvolatile components in the resin composition. By containing components (A-1), (B), and (C) in combination and setting the contents of components (A-1) and (B) within the specified ranges, the resin composition can achieve the desired effects of the present invention, namely, a cured product having excellent adhesion and suppressing warpage, the occurrence of flow marks after molding, and unevenness on the resin surface after post-cure.

[0013] Taking advantage of its excellent properties, the cured product of this resin composition can be preferably used as an insulating layer or sealing layer for circuit boards and semiconductor chip packages, and can be particularly preferably used as a sealing layer.

[0014] The resin composition may further contain optional components in addition to the components (A-1), (B), and (C). Examples of optional components include (A-2) an epoxy resin having an epoxy equivalent of 400 g / eq. or less, or an epoxy resin having an epoxy equivalent of more than 1500 g / eq., and (D) a curing accelerator. In this specification, the components (A-1) and (A-2) are sometimes collectively referred to as "(A) epoxy resin." Each component contained in the resin composition will be described below.

[0015] <(A-1) Epoxy resin with an epoxy equivalent greater than 400 g / eq. and less than or equal to 1500 g / eq.> The resin composition contains, as component (A-1), an epoxy resin (A-1) having an epoxy equivalent greater than 400 g / eq. and not greater than 1500 g / eq. Because component (A-1) has an epoxy equivalent greater than 400 g / eq. and not greater than 1500 g / eq., a cured product having a crosslink density within a specific appropriate range can be obtained. Therefore, the cured product of a resin composition containing component (A-1) is thought to have improved toughness, and as a result, improved adhesion. Furthermore, by including component (A-1) in the resin composition, the occurrence of cure shrinkage during curing of the resin composition is suppressed. As a result, the amount of warpage is thought to be suppressed.

[0016] The epoxy equivalent of component (A-1) is greater than 400 g / eq., preferably 410 g / eq. or greater, more preferably 420 g / eq. or greater, and is 1500 g / eq. or less, preferably 1000 g / eq. or less, more preferably 800 g / eq. or less, and 500 g / eq. or less. By keeping the epoxy equivalent of component (A-1) within this range, the desired effects of the present invention can be achieved. The epoxy equivalent can be measured according to JIS K7236 and is the mass of a resin containing one equivalent of epoxy groups.

[0017] The content of component (A-1) is 0.2% by mass or more, preferably 0.3% by mass or more, more preferably 0.5% by mass or more, and less than 3% by mass, preferably 2.5% by mass or less, more preferably 2% by mass or less, and 1.5% by mass or less, when the total nonvolatile components in the resin composition is taken as 100% by mass. By keeping the content of component (A-1) within this range, it is possible to lower the glass transition temperature of the resin composition and further suppress the amount of warpage. In the present invention, the content of each component in the resin composition is a value when the total nonvolatile components in the resin composition is taken as 100% by mass, unless otherwise specified.

[0018] From the viewpoint of obtaining the desired effects of the present invention, the component (A-1) preferably has one or more epoxy groups in one molecule, more preferably has two or more epoxy groups in one molecule, and even more preferably has three or more epoxy groups in one molecule.

[0019] The component (A-1) may be a liquid component (A-1) at 20° C. or a solid component (A-1) at 20° C. From the viewpoint of achieving the desired effects of the present invention, the component (A-1) is preferably a liquid component. The component (A-1) may be used alone or in combination of two or more types.

[0020] The component (A-1) preferably contains, for example, one or more skeletons selected from the group consisting of a fluorene skeleton, a butadiene skeleton, an isoprene skeleton, an alkyleneoxy skeleton, a siloxane skeleton, and a bisphenol skeleton.

[0021] The alkyleneoxy skeleton refers to a structure having an alkyleneoxy group in which an alkylene group and an oxygen atom are bonded, and the alkylene group is preferably an alkylene group having 1 to 10 carbon atoms, more preferably an alkylene group having 1 to 6 carbon atoms, and even more preferably an alkylene group having 3 to 6 carbon atoms.

[0022] Examples of the bisphenol skeleton include bisphenol A, bisphenol F, bisphenol AD, bisphenol S, and 4,4'-(9-fluorenylidene)bisphenol.

[0023] Among these, it is more preferable that the component (A-1) contains one or more skeletons selected from the group consisting of a fluorene skeleton, a butadiene skeleton, an alkyleneoxy skeleton, a siloxane skeleton, and a bisphenol skeleton.

[0024] Commercially available products of component (A-1) include, for example, "EG-280" and "EG-250" manufactured by Osaka Gas Chemicals Co., Ltd., "R-45EPT", "R-15EPT", "DLC-204", "EX-145", "EX-171", "EX-991L", "EX-992L", and "FCA-635" manufactured by Nagase ChemteX Corporation, "SR-PTMG" manufactured by Sakamoto Pharmaceutical Co., Ltd., "KF-105" manufactured by Shin-Etsu Chemical Co., Ltd., "EXA-4816" and "EXA-4850" manufactured by DIC Corporation, "EP-4003S" manufactured by ADEKA Corporation, "LCE-2615" manufactured by Nippon Kayaku Co., Ltd., and "YX-7400", "YX-7105", and "YX-7110" manufactured by Mitsubishi Chemical Corporation. These may be used alone or in combination of two or more types.

[0025] From the viewpoint of significantly achieving the desired effects of the present invention, the weight average molecular weight (Mw) of the component (A-1) is preferably at least 100, more preferably at least 250, even more preferably at least 400, and is preferably at most 5000, more preferably at most 3000, even more preferably at most 1500. The weight average molecular weight of the component (A-1) is the weight average molecular weight in terms of polystyrene measured by gel permeation chromatography (GPC).

[0026] <(A-2) Epoxy resins with an epoxy equivalent of 400 g / eq. or less, or epoxy resins with an epoxy equivalent of more than 1500 g / eq.> The resin composition may contain, as (A-2), an epoxy resin having an epoxy equivalent of 400 g / eq or less, or an epoxy resin having an epoxy equivalent of more than 1500 g / eq. By including component (A-2) in the resin composition, the effects of the present invention can be significantly achieved.

[0027] Examples of component (A-2) 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, 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, cyclohexanedimethanol-type epoxy resins, naphthylene ether-type epoxy resins, trimethylol-type epoxy resins, and tetraphenylethane-type epoxy resins. Component (A-2) may be used singly or in combination of two or more.

[0028] The resin composition preferably contains, as component (A-2), an epoxy resin having two or more epoxy groups per molecule. From the viewpoint of significantly achieving the desired effects of the present invention, the proportion of component (A-2) having two or more epoxy groups per molecule is preferably 50% by mass or more, more preferably 60% by mass or more, and particularly preferably 70% by mass or more, relative to 100% by mass of the non-volatile components of component (A-2).

[0029] The (A-2) component includes an (A-2) component that is liquid at a temperature of 20° C. and an (A-2) component that is solid at a temperature of 20° C. The resin composition may use a liquid (A-2) component as the (A-2) component, a solid (A-2) component, or a combination of a liquid (A-2) component and a solid (A-2) component. Of these, from the viewpoint of reducing the viscosity of the resin composition, it is preferable to use a liquid (A-2) component as the (A-2) component.

[0030] As the liquid component (A-2), a liquid component (A-2) having two or more epoxy groups in one molecule is preferred.

[0031] Preferred examples of the liquid component (A-2) include bisphenol A epoxy resins, bisphenol F epoxy resins, bisphenol AF epoxy resins, naphthalene epoxy resins; glycidyl ester epoxy resins, glycidyl amine epoxy resins, phenol novolac epoxy resins, alicyclic epoxy resins such as alicyclic epoxy resins having an ester skeleton, cyclohexane epoxy resins, cyclohexanedimethanol epoxy resins, glycidyl amine epoxy resins, and epoxy resins having a butadiene structure, with glycidyl amine epoxy resins, bisphenol A epoxy resins, bisphenol F epoxy resins, and alicyclic epoxy resins being more preferred.

[0032] Specific examples of the liquid component (A-2) include "HP4032," "HP4032D," and "HP4032SS" (naphthalene-type epoxy resins) manufactured by DIC Corporation; "828US," "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" and "630LSD" (glycidylamine-type epoxy resins) manufactured by Mitsubishi Chemical Corporation; and Nippon Steel & Sumitomo Metal Chemical Co., Ltd. Examples of epoxy resins include "ZX1059" manufactured by Nagase ChemteX Corporation (a mixture of bisphenol A-type epoxy resin and bisphenol F-type epoxy resin); "EX-721" (glycidyl ester-type epoxy resin) manufactured by Daicel Corporation; "CEL-do 2021P" (alicyclic epoxy resin having an ester skeleton) manufactured by Daicel Corporation; "PB-3600" (epoxy resin having a butadiene structure) manufactured by Daicel Corporation; "ZX1658" and "ZX1658GS" (liquid 1,4-glycidylcyclohexane-type epoxy resin) manufactured by Nippon Steel & Sumikin Chemical Co., Ltd.; and "EP3950L" (glycidylamine-type epoxy resin) manufactured by ADEKA Corporation. These may be used alone or in combination of two or more.

[0033] As the solid component (A-2), a solid component (A-2) having three or more epoxy groups in one molecule is preferred, and an aromatic solid component (A-2) having three or more epoxy groups in one molecule is more preferred.

[0034] As the solid component (A-2), bixylenol-type epoxy resins, naphthalene-type epoxy resins, naphthalene-type tetrafunctional epoxy resins, cresol novolac-type epoxy resins, dicyclopentadiene-type epoxy resins, trisphenol-type epoxy resins, naphthol-type epoxy resins, biphenyl-type epoxy resins, naphthylene ether-type epoxy resins, anthracene-type epoxy resins, bisphenol A-type epoxy resins, bisphenol AF-type epoxy resins, and tetraphenylethane-type epoxy resins are preferred, with biphenyl-type epoxy resins being more preferred.

[0035] Specific examples of the solid component (A-2) include "HP4032H" (naphthalene-type epoxy resin) manufactured by DIC Corporation; "HP-4700" and "HP-4710" (naphthalene-type tetrafunctional epoxy resins) manufactured by DIC Corporation; "N-690" (cresol novolac-type epoxy resin) manufactured by DIC Corporation; "N-695" (cresol novolac-type epoxy resin) manufactured by DIC Corporation; "HP-7200", "HP-7200HH", and "HP-7200H" (dicyclo epoxy resins) manufactured by DIC Corporation. pentadiene type epoxy resins); DIC Corporation's "EXA-7311", "EXA-7311-G3", "EXA-7311-G4", "EXA-7311-G4S", and "HP6000" (naphthylene ether type epoxy resins); Nippon Kayaku Co., Ltd.'s "EPPN-502H" (trisphenol type epoxy resin); Nippon Kayaku Co., Ltd.'s "NC7000L" (naphthol novolac type epoxy resin); Nippon Kayaku Co., Ltd.'s "NC3000H", "NC3000", and "N C3000L, NC3100 (biphenyl-type epoxy resin); Nippon Steel & Sumitomo Metal Chemical's ESN475V (naphthol-type epoxy resin); Nippon Steel & Sumitomo Metal Chemical's ESN485 (naphthol novolac-type epoxy resin); Mitsubishi Chemical's YX4000H, YX4000, YL6121 (biphenyl-type epoxy resin); Mitsubishi Chemical's YX4000HK (bixylenol-type epoxy resin); Mitsubishi Chemical's YX Examples of epoxy resins include "8800" (anthracene-type epoxy resin), "PG-100" and "CG-500" manufactured by Osaka Gas Chemicals Co., Ltd., "YL7760" (bisphenol AF-type epoxy resin) manufactured by Mitsubishi Chemical Corporation, "YL7800" (fluorene-type epoxy resin) manufactured by Mitsubishi Chemical Corporation, "jER1010" (solid bisphenol A-type epoxy resin) manufactured by Mitsubishi Chemical Corporation, and "jER1031S" (tetraphenylethane-type epoxy resin) manufactured by Mitsubishi Chemical Corporation. These may be used alone or in combination of two or more.

[0036] When a liquid (A-2) component and a solid (A-2) component are used in combination as the (A-2) component, the ratio by mass of the liquid (A-2) component to the solid (A-2) component is preferably 1:0.01 to 1:20, more preferably 1:0.05 to 1:10, and particularly preferably 1:0.1 to 1:1. When the ratio of the liquid (A-2) component to the solid (A-2) component is within this range, the desired effects of the present invention can be significantly achieved.

[0037] When component (A-2) is an epoxy resin with an epoxy equivalent of 400 g / eq. or less, the epoxy equivalent is preferably 400 g / eq. or less, more preferably 300 g / eq. or less, even more preferably 200 g / eq. or less, and is preferably 50 g / eq. or more, more preferably 80 g / eq. or more, and even more preferably 90 g / eq. or more. When the epoxy equivalent is within this range, the cured product of the resin composition has a sufficient crosslink density, and an insulating layer with low surface roughness can be obtained.

[0038] When component (A-2) is an epoxy resin with an epoxy equivalent greater than 1500 g / eq., the epoxy equivalent is preferably greater than 1500 g / eq., more preferably 1600 g / eq. or more, even more preferably 1700 g / eq. or more, and is preferably 5000 g / eq. or less, more preferably 3000 g / eq. or less, and even more preferably 2000 g / eq. or less. When the epoxy equivalent is within this range, the cured product of the resin composition will have a sufficient crosslink density, and an insulating layer with low surface roughness can be obtained.

[0039] The weight average molecular weight (Mw) of the component (A-2) is preferably 100 to 5,000, more preferably 250 to 3,000, and even more preferably 400 to 1,500, from the viewpoint of significantly achieving the desired effects of the present invention.

[0040] The content of component (A-2) is preferably 1% by mass or more, more preferably 3% by mass or more, and even more preferably 5% by mass or more, based on 100% by mass of the nonvolatile components in the resin composition, from the viewpoint of obtaining an insulating layer exhibiting good mechanical strength and insulating reliability. The upper limit of the content of the epoxy resin is preferably 20% by mass or less, more preferably 15% by mass or less, and particularly preferably 10% by mass or less, from the viewpoint of significantly obtaining the desired effects of the present invention.

[0041] When the content of the nonvolatile components of the resin composition of component (A-1) is defined as A1 when the total mass of the nonvolatile components is 100% by mass, and the content of the nonvolatile components of the resin composition of component (A-2) is defined as A2 when the total mass of the nonvolatile components is 100% by mass, from the viewpoint of significantly obtaining the effects of the present invention, A1 / A2 is preferably 0.01 or more, more preferably 0.03 or more, even more preferably 0.05 or more, and is preferably 1 or less, more preferably 0.8 or less, even more preferably 0.5 or less.

[0042] <(B) Inorganic filler> The resin composition contains an inorganic filler as component (B). By using the inorganic filler (B), the insulating performance of the cured product of the resin composition can be improved.

[0043] From the viewpoint of obtaining an insulating layer having excellent insulating performance, the content of the (B) inorganic filler is 70% by mass or more, preferably 75% by mass or more, more preferably 80% by mass or more, even more preferably 85% by mass or more, and preferably 95% by mass or less, more preferably 90% by mass or less, even more preferably 88% by mass or less, when the non-volatile components in the resin composition are taken as 100% by mass.

[0044] (B) An inorganic compound is used as the inorganic filler material. Examples of inorganic filler 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 is particularly preferred. Examples of silica include amorphous silica, fused silica, crystalline silica, synthetic silica, and hollow silica. Spherical silica is preferred. (B) The inorganic filler may be used alone or in combination of two or more.

[0045] (B) Examples of commercially available inorganic fillers include "SP60-05" and "SP507-05" manufactured by Nippon Steel & Sumikin Materials Co., Ltd.; "YC100C," "YA050C," "YA050C-MJE," and "YA010C" manufactured by Admatechs Co., Ltd.; "UFP-30" manufactured by Denka Company Limited; "Silfill NSS-3N," "Silfill NSS-4N," and "Silfill NSS-5N" manufactured by Tokuyama Corporation; and "SC2500SQ," "SO-C4," "SO-C2," and "SO-C1" manufactured by Admatechs Co., Ltd.

[0046] From the viewpoint of significantly achieving the desired effects of the present invention, the average particle size of (B) the inorganic filler is preferably 0.01 μm or more, more preferably 0.05 μm or more, particularly preferably 0.1 μm or more, and is preferably 5 μm or less, more preferably 2 μm or less, and even more preferably 1 μm or less.

[0047] The average particle size of (B) 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 (B) 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 is 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.

[0048] The specific surface area of ​​the (B) inorganic filler is preferably 1 m² from the viewpoint of significantly achieving the desired effects of the present invention. 2 / g or more, more preferably 2m 2 / g or more, particularly preferably 3m 2 / g or more. There is no particular upper limit, but it is preferably 60m 2 / g or less, 50m 2 / g or less or 40m 2 The specific surface area is determined 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.) according to the BET method, and then calculating the specific surface area using the BET multipoint method.

[0049] (B) The inorganic filler is preferably treated with a surface treatment agent from the viewpoint of improving moisture resistance and dispersibility. Examples of the surface treatment agent include a fluorine-containing silane coupling agent, an aminosilane coupling agent, an epoxysilane coupling agent, a mercaptosilane coupling agent, a silane coupling agent, an alkoxysilane, an organosilazane compound, and a titanate coupling agent. The surface treatment agent may be used alone or in any combination of two or more.

[0050] 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).

[0051] The degree of surface treatment with the surface treatment agent is preferably within a predetermined range from the viewpoint of improving the dispersibility of the inorganic filler. Specifically, 100 parts by mass of the inorganic filler is preferably surface-treated with 0.2 to 5 parts by mass of the surface treatment agent, more preferably 0.2 to 3 parts by mass, and even more preferably 0.3 to 2 parts by mass.

[0052] 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 suppressing an increase in the melt viscosity of the resin varnish and the melt viscosity of the resin composition layer, it is more preferable that the amount of the resin varnish is 1 mg / m 2 Preferably less than 0.8 mg / m 2 Less than 0.5 mg / m is more preferable. 2 The following is even more preferred:

[0053] The carbon amount 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 carbon amount 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.

[0054] When the content of the nonvolatile components of the resin composition of component (A-1) is defined as A1 when the total mass of the nonvolatile components is 100% by mass, and the content of the nonvolatile components of the resin composition of component (B) is defined as B1 when the total mass of the nonvolatile components is 100% by mass, A1 / B1 is preferably 0.001 or more, more preferably 0.005 or more, even more preferably 0.01 or more, and is preferably 0.5 or less, more preferably 0.3 or less, even more preferably 0.1 or less, from the viewpoint of significantly obtaining the effects of the present invention.

[0055] <(C) Hardener> The resin composition contains a curing agent as component (C). The curing agent (C) usually has the function of reacting with component (A) to cure the resin composition. The curing agent (C) may be used alone or in combination of two or more types in any ratio.

[0056] As the (C) curing agent, a compound capable of reacting with the (A) epoxy resin to cure the resin composition can be used, and examples thereof include acid anhydride-based curing agents, amine-based curing agents, phenol-based curing agents, active ester-based curing agents, cyanate ester-based curing agents, benzoxazine-based curing agents, carbodiimide-based curing agents, etc. Among these, acid anhydride-based curing agents are preferred from the viewpoint of significantly obtaining the effects of the present invention.

[0057] Examples of acid anhydride curing agents include curing agents having one or more acid anhydride groups in one molecule. Specific examples of acid anhydride curing agents include phthalic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, methyltetrahydrophthalic anhydride, 4-methylhexahydrophthalic 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 benzophenone. Examples of suitable curing agents include tetracarboxylic dianhydrides, 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 acid anhydrides such as styrene-maleic acid resins (copolymers of styrene and maleic acid). Commercially available acid anhydride curing agents are also available, such as "MH-700" manufactured by New Japan Chemical Co., Ltd.

[0058] Examples of the amine curing agent include curing agents having one or more amino groups in one molecule, such as aliphatic amines, polyether amines, alicyclic amines, and aromatic amines. Among these, aromatic amines are preferred from the viewpoint of achieving the desired effects of the present invention. The amine curing agent is preferably a primary amine or a secondary amine, and more preferably a primary amine. Specific examples of amine-based curing agents include 4,4'-methylenebis(2,6-dimethylaniline), diphenyldiaminosulfone, 4,4'-diaminodiphenylmethane, 4,4'-diaminodiphenylsulfone, 3,3'-diaminodiphenylsulfone, 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-hydroxybenzoyl). Examples of suitable amine curing agents include 4,4'-bis(4-aminophenoxy)biphenyl, bis(4-(4-aminophenoxy)phenyl)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 curing agents may be used, such as "KAYABOND C-200S," "KAYABOND C-100," "KAYAHARD AA," "KAYAHARD AB," and "KAYAHARD AS" manufactured by Nippon Kayaku Co., Ltd., and "Epicure W" manufactured by Mitsubishi Chemical Corporation.

[0059] Examples of phenolic curing agents include curing agents having one or more, preferably two or more, hydroxyl groups bonded to an aromatic ring (such as a benzene ring or a naphthalene ring) per molecule. Among these, compounds having a hydroxyl group bonded to a benzene ring are preferred. Furthermore, from the viewpoint of heat resistance and water resistance, phenolic curing agents having a novolac structure are preferred. Furthermore, from the viewpoint of adhesion, nitrogen-containing phenolic curing agents are preferred, and triazine skeleton-containing phenolic curing agents are more preferred. In particular, from the viewpoint of achieving high levels of heat resistance, water resistance, and adhesion, triazine skeleton-containing phenolic novolac curing agents are preferred.

[0060] Specific examples of phenol-based curing agents and naphthol-based curing agents 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.; and "SN-170," "SN-180," "SN-190," "SN-475," "SN-485," "SN-495," "SN-495V," "SN-375," and "SN-495V" manufactured by Nippon Steel & Sumikin Chemical Co., Ltd. SN-395; DIC Corporation's "TD-2090," "TD-2090-60M," "LA-7052," "LA-7054," "LA-1356," "LA-3018," "LA-3018-50P," "EXB-9500," "HPC-9500," "KA-1160," "KA-1163," and "KA-1165"; and Gun-ei Chemical Co., Ltd.'s "GDP-6115L," "GDP-6115H," and "ELPC75."

[0061] Examples of active ester curing agents include curing agents having one or more active ester groups per molecule. Among these, preferred active ester curing agents are compounds having two or more highly reactive ester groups per molecule, such as phenol esters, thiophenol esters, N-hydroxyamine esters, and esters of heterocyclic hydroxy compounds. The active ester curing agent 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. In particular, from the viewpoint of improving heat resistance, active ester curing agents obtained from a carboxylic acid compound and a hydroxy compound are preferred, and active ester curing agents obtained from a carboxylic acid compound and a phenol compound and / or a naphthol compound are more preferred.

[0062] 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.

[0063] 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.

[0064] Preferred specific examples of active ester curing agents include active ester compounds containing a dicyclopentadiene-type diphenol structure, active ester compounds containing a naphthalene structure, active ester compounds containing an acetylated product of phenol novolac, and active ester compounds containing a benzoylated product of phenol novolac. Among these, active ester compounds containing a naphthalene structure and active ester compounds containing a dicyclopentadiene-type diphenol structure are more preferred. The "dicyclopentadiene-type diphenol structure" refers to a divalent structure consisting of phenylene-dicyclopentylene-phenylene.

[0065] Commercially available active ester curing agents include active ester compounds containing a dicyclopentadiene-type diphenol structure, such as "EXB9451," "EXB9460," "EXB9460S," "HPC-8000," "HPC-8000H," "HPC-8000-65T," "HPC-8000H-65TM," "EXB-8000L," "EXB-8000L-65TM," and "EXB-8150-65T" (manufactured by DIC Corporation); and active ester compounds containing a naphthalene structure, such as "EXB-8100L-65T," "EXB-8150L-65T," and "EXB9416-70BK" (manufactured by DIC Corporation). IC Co., Ltd.); "DC808" (Mitsubishi Chemical Corporation) as an active ester compound containing an acetylated phenol novolac; "YLH1026" (Mitsubishi Chemical Corporation) as an active ester compound containing a benzoylated phenol novolac; "DC808" (Mitsubishi Chemical Corporation) as an active ester curing agent which is an acetylated phenol novolac; and "YLH1026" (Mitsubishi Chemical Corporation), "YLH1030" (Mitsubishi Chemical Corporation), and "YLH1048" (Mitsubishi Chemical Corporation) as active ester curing agents which are benzoylated phenol novolac.

[0066] Examples of cyanate ester curing agents include bifunctional cyanate 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; polyfunctional cyanate resins derived from phenol novolac, cresol novolac, etc.; and prepolymers in which these cyanate resins are partially converted to triazine. Specific examples of cyanate ester curing agents include "PT30" and "PT60" manufactured by Lonza Japan Co., Ltd. (both are phenol novolac type multifunctional cyanate ester resins); "ULL-950S" (multifunctional cyanate ester resin); "BA230" and "BA230S75" (prepolymers in which part or all of bisphenol A dicyanate has been triazine converted to a trimer); and the like.

[0067] Specific examples of benzoxazine-based curing agents include "HFB2006M" manufactured by Showa Polymer Co., Ltd., and "Pd" and "Fa" manufactured by Shikoku Chemical Industry Co., Ltd.

[0068] Specific examples of carbodiimide curing agents include "V-03", "V-05", and "V-07" manufactured by Nisshinbo Chemical Inc.; and Stavaxol (registered trademark) P manufactured by Rhein Chemie.

[0069] From the viewpoint of significantly obtaining the effects of the present invention, the content of the (C) curing agent is preferably 0.1% by mass or more, more preferably 0.2% by mass or more, and even more preferably 0.3% by mass or more, and is preferably 10% by mass or less, more preferably 8% by mass or less, and even more preferably 7% by mass or less, based on 100% by mass of non-volatile components in the resin composition.

[0070] When the number of epoxy groups in component (A) is taken as 1, the number of active groups in the (C) curing agent is preferably 0.1 or more, more preferably 0.2 or more, even more preferably 0.3 or more, and preferably 2 or less, more preferably 1.8 or less, even more preferably 1.6 or less, and particularly preferably 1.4 or less. Here, "the number of epoxy groups in component (A)" refers to the sum of all values ​​obtained by dividing the mass of the non-volatile components of component (A) present in the resin composition by the epoxy equivalent. Furthermore, "the number of active groups in (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 the active group equivalent. When the number of epoxy groups in component (A) is taken as 1, the desired effects of the present invention can be significantly achieved by having the number of active groups in the (C) curing agent within the above range.

[0071] When the number of epoxy groups in component (A-1) is taken as 1, the number of active groups in (C) curing agent is preferably 0.1 or more, more preferably 0.2 or more, even more preferably 0.3 or more, and preferably 2 or less, more preferably 1.8 or less, even more preferably 1.6 or less, and particularly preferably 1.4 or less. Here, "the number of epoxy groups in component (A-1)" refers to the total value obtained by dividing the mass of the non-volatile components of component (A-1) present in the resin composition by the epoxy equivalent. When the number of epoxy groups in component (A-1) is taken as 1, the desired effects of the present invention can be significantly achieved by having the number of active groups in (C) curing agent within the above range.

[0072] When the number of epoxy groups in component (A-2) is taken as 1, the number of active groups in (C) curing agent is preferably 0.1 or more, more preferably 0.2 or more, even more preferably 0.3 or more, and preferably 2 or less, more preferably 1.8 or less, even more preferably 1.6 or less, and particularly preferably 1.4 or less. Here, "the number of epoxy groups in component (A-2)" refers to the total value obtained by dividing the mass of the non-volatile components of component (A-2) present in the resin composition by the epoxy equivalent. When the number of epoxy groups in component (A-2) is taken as 1, the desired effects of the present invention can be significantly achieved by having the number of active groups in (C) curing agent within the above range.

[0073] <(D) Curing accelerator> The resin composition may contain (D) a curing accelerator as an optional component. Examples of the curing accelerator include phosphorus-based curing accelerators, amine-based curing accelerators, imidazole-based curing accelerators, guanidine-based curing accelerators, and metal-based curing accelerators. Amine-based curing accelerators and imidazole-based curing accelerators are preferred, and amine-based curing accelerators are more preferred. The curing accelerators may be used alone or in combination of two or more.

[0074] Examples of phosphorus-based curing accelerators include triphenylphosphine, phosphonium borate compounds, tetraphenylphosphonium tetraphenylborate, n-butylphosphonium tetraphenylborate, tetrabutylphosphonium decanoate, (4-methylphenyl)triphenylphosphonium thiocyanate, tetraphenylphosphonium thiocyanate, and butyltriphenylphosphonium thiocyanate, with triphenylphosphine and tetrabutylphosphonium decanoate being preferred.

[0075] Examples of the amine curing accelerator include trialkylamines such as triethylamine and tributylamine, 4-dimethylaminopyridine, benzyldimethylamine, 2,4,6-tris(dimethylaminomethyl)phenol, and 1,8-diazabicyclo(5,4,0)-undecene, with 4-dimethylaminopyridine and 1,8-diazabicyclo(5,4,0)-undecene being preferred.

[0076] 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, 1-benzyl-2-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, 2-phenyl-4,5-dihydroxymethylimidazole, 2-phenyl-4,5-dihydroxymethylimidazole, Examples of the imidazole compound include imidazole compounds such as 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, and 2-ethyl-4-methylimidazole and 1-benzyl-2-phenylimidazole are preferred.

[0077] As the imidazole-based curing accelerator, commercially available products may be used, for example, "P200-H50" manufactured by Mitsubishi Chemical Corporation.

[0078] Examples of guanidine-based 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, and 7-methyl-1,5,7-triazabicyclo[4.4.0]dec-5-ene. Examples of suitable biguanide include 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. Of these, dicyandiamide and 1,5,7-triazabicyclo[4.4.0]dec-5-ene are preferred.

[0079] 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.

[0080] The content of (D) curing accelerator, when the non-volatile components in the resin composition are taken as 100% by mass, is preferably 0.01% by mass or more, more preferably 0.03% by mass or more, and particularly preferably 0.05% by mass or more, and is preferably 1% by mass or less, more preferably 0.5% by mass or less, and particularly preferably 0.1% by mass or less.

[0081] <(E) Other additives> In addition to the above-mentioned components, the resin composition may further contain other additives as optional components. Examples of such additives include resin additives such as thermoplastic resins; flame retardants; organic fillers; organometallic compounds such as organocopper compounds, organozinc compounds, and organocobalt compounds; thickeners; antifoaming agents; leveling agents; adhesion promoters; colorants; and pigments. These additives may be used alone or in combination of two or more in any ratio. The content of each additive can be determined appropriately by those skilled in the art.

[0082] The above-mentioned resin composition may contain a solvent if necessary, but is preferably a solvent-free resin composition that does not substantially contain a solvent. Even if it does not contain a solvent, the resin composition can be fluidized when molded using a compression molding method, and excellent compression moldability can be achieved. Therefore, this resin composition can be used as a solvent-free resin composition. "Substantially free of solvent" means, for example, that the solvent content is 1% by mass or less based on the entire solvent-free resin composition.

[0083] The method for preparing the resin composition is not particularly limited, and examples thereof include a method in which the ingredients are mixed and dispersed using a rotary mixer or the like, with the addition of a solvent or the like as necessary.

[0084] <Characteristics of resin composition> The resin composition described above can provide a cured layer capable of suppressing warpage. Therefore, by using this resin composition, sealing layers and insulating layers capable of suppressing warpage of circuit boards and semiconductor chip packages can be obtained. For example, a sample substrate is prepared by forming a cured layer of the resin composition on a 12-inch silicon wafer using the method described in the Examples and heating the resin composition at 180°C for 90 minutes. In this case, the amount of warpage measured at 25°C using the method described in the Examples can be typically less than 5 mm, preferably less than 4 mm. The lower limit is not particularly limited, but can be, for example, 0.01 mm or more.

[0085] Furthermore, the resin composition described above can provide a cured product with excellent adhesion. Therefore, by using this resin composition, sealing layers and insulating layers with excellent adhesion can be obtained for circuit boards and semiconductor chip packages. The adhesion strength is preferably 500 kgf / cm. 2 The adhesive strength can be measured according to the method described in the examples below.

[0086] A cured product using the above-described resin composition exhibits the property of suppressing the occurrence of flow marks after molding. Therefore, by using this resin composition, it is possible to obtain a sealing layer and an insulating layer in which the occurrence of flow marks is suppressed. Specifically, the resin composition was compression molded on a 12-inch silicon wafer using a compression molding device (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) to form a resin composition layer with a thickness of 300 μm, and a sample was formed (the area of ​​the resin composition layer at this time was 14.6 cm × 14.6 × 3.14 = 45.844 cm). 2 ) and observe the appearance of the resin composition layer of the sample. At this time, the area occupied by flow marks is less than 20% of the entire surface of the resin composition layer. The occurrence of flow marks after molding can be evaluated by measurement according to the method described in the examples below.

[0087] Furthermore, a cured product using the above-described resin composition exhibits the characteristic of suppressing the occurrence of resin surface unevenness after post-cure. Therefore, by using this resin composition, it is possible to obtain a sealing layer and an insulating layer in which the occurrence of resin surface unevenness after post-cure is suppressed. Specifically, the resin composition is compression-molded onto a 12-inch silicon wafer using a compression molding device (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) to form a 300 μm-thick resin composition layer on the 12-inch silicon wafer (the area of ​​the resin composition layer at this time is 14.6 cm × 14.6 × 3.14 = 45.844 cm). 2 The resin composition layer is then heated at 180°C for 90 minutes to heat-cure the resin composition layer, and the appearance of the cured layer is observed. At this time, the surface of the cured layer is usually uniform and free of color unevenness.

[0088] The resin composition may be liquid or solid, but is preferably liquid during molding. For example, a resin composition that is liquid at room temperature (e.g., 20°C) may be compressed at room temperature without any special temperature adjustment, or may be heated to an appropriate temperature and then compressed. Alternatively, a resin composition that is liquid at room temperature may be filled into a cartridge, discharged from the cartridge, and then compressed.

[0089] Furthermore, resin compositions that are solid at room temperature can usually be made liquid by adjusting the temperature to a higher temperature (e.g., 130°C), and can be molded by compression molding with appropriate temperature adjustment, such as heating. The resin composition can usually be made liquid at an appropriate temperature even without a solvent, and can be used, for example, as a liquid encapsulant. Here, "liquid" refers to a composition whose viscosity, measured using the following measurement method, is less than 1500 Pa·s. Using a RE80 viscometer (manufactured by Toki Sangyo Co., Ltd.), 0.2 to 0.3 ml of the resin composition to be measured is measured using a syringe. During measurement, the temperature of the measurement chamber of the viscometer is controlled at 25.0°C using an external circulation type thermostatic bath. The rotor rotation speed is set to 1 rpm, and the viscosity is measured after 120 seconds.

[0090] Because the resin composition has the above-described properties, it can be suitably used as a resin composition for encapsulating electronic devices such as organic electroluminescence devices and semiconductors. In particular, it can be suitably used as a resin composition for encapsulating semiconductors (semiconductor encapsulation resin composition), preferably as a resin composition for encapsulating semiconductor chips (semiconductor chip encapsulation resin composition). Furthermore, the resin composition can be used as a resin composition for insulating layers other than encapsulation. For example, the resin composition can be suitably used as a resin composition for forming an insulating layer of a semiconductor chip package (semiconductor chip package insulating layer resin composition) and a resin composition for forming an insulating layer of a circuit board (including a printed wiring board) (circuit board insulating layer resin composition).

[0091] Examples of semiconductor chip packages include FC-CSP, MIS-BGA package, ETS-BGA package, fan-out type WLP (Wafer Level Package), fan-in type WLP, fan-out type PLP (Panel Level Package), and fan-in type PLP.

[0092] The resin composition may also be used as an underfill material, for example, as a material for MUF (Molding Under Filling) that is used after connecting a semiconductor chip to a substrate.

[0093] Furthermore, the resin composition can be used in a wide range of applications where resin compositions are used, such as sheet-like laminate materials such as resin sheets and prepregs, solder resists, die bonding materials, hole-filling resins, and component-embedding resins.

[0094] [Resin sheet] The resin sheet of the present invention has a support and a resin composition layer provided on the support. The resin composition layer is a layer containing the resin composition of the present invention and is usually formed from the resin composition.

[0095] From the viewpoint of thinning, the thickness of the resin composition layer is preferably 600 μm or less, more preferably 550 μm or less, and even more preferably 500 μm or less, 400 μm or less, 350 μm or less, 300 μm or less, or 200 μm or less. The lower limit of the thickness of the resin composition layer is not particularly limited and can be, for example, 1 μm or more, 5 μm or more, 10 μm or more, etc.

[0096] Examples of the support include films made of plastic materials, metal foils, and release papers, with films made of plastic materials and metal foils being preferred.

[0097] When a film made 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"); acrylic polymers such as polymethyl methacrylate (hereinafter sometimes abbreviated as "PMMA"); cyclic polyolefins; triacetyl cellulose (hereinafter sometimes abbreviated as "TAC"); polyether sulfide (hereinafter sometimes abbreviated as "PES"); polyether ketone; polyimide; etc. Among these, polyethylene terephthalate and polyethylene naphthalate are preferred, and inexpensive polyethylene terephthalate is particularly preferred.

[0098] When a metal foil is used as the support, examples of the metal foil include copper foil and aluminum foil. Of these, copper foil is preferred. The copper foil may be a foil made of a single metal, copper, or a foil made of an alloy of copper and another metal (e.g., tin, chromium, silver, magnesium, nickel, zirconium, silicon, titanium, etc.).

[0099] The surface of the support that is to be bonded to the resin composition layer may be subjected to a matte treatment, a corona treatment, an antistatic treatment or the like.

[0100] The support may also be a support with a release layer, which has a release layer on the surface that bonds to 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 resins, polyolefin resins, urethane resins, and silicone resins. Commercially available release agents include alkyd resin-based release agents such as "SK-1," "AL-5," and "AL-7" manufactured by Lintec Corporation. Examples of support with a release layer include "Lumirror T60" manufactured by Toray Industries, Inc.; "Purex" manufactured by Teijin Limited; and "Uni-Peel" manufactured by Unitika Limited.

[0101] The thickness of the support is preferably in the range of 5 μm to 75 μm, more preferably in the range of 10 μm to 60 μm. When a support with a release layer is used, it is preferable that the total thickness of the support with a release layer is in the above range.

[0102] The resin sheet can be produced, for example, by applying the resin composition to a support using a coating device such as a die coater. Alternatively, if necessary, the resin composition may be dissolved in an organic solvent to prepare a resin varnish, and the resin sheet may be produced by applying the resin varnish. The use of a solvent can adjust the viscosity and improve the coatability. When a resin varnish is used, the resin varnish is usually dried after application to form a resin composition layer.

[0103] Examples of organic solvents include ketone solvents such as acetone, methyl ethyl ketone, and cyclohexanone; acetate ester solvents such as ethyl acetate, butyl acetate, cellosolve acetate, propylene glycol monomethyl ether acetate, and carbitol acetate; carbitol solvents such as cellosolve and butyl carbitol; aromatic hydrocarbon solvents such as toluene and xylene; and amide solvents such as dimethylformamide, dimethylacetamide (DMAc), and N-methylpyrrolidone. One type of organic solvent may be used alone, or two or more types may be used in combination at any ratio.

[0104] Drying may be carried out by known methods such as heating or hot air blowing. Drying conditions are such that the content of organic solvent in the resin composition layer is generally 10% by mass or less, preferably 5% by mass or less. Although this varies depending on the boiling point of the organic solvent in the resin varnish, for example, when a resin varnish containing 30% by mass to 60% by mass of organic solvent is used, the resin composition layer can be formed by drying at 50°C to 150°C for 3 to 10 minutes.

[0105] The resin sheet may include any layer other than the support and the resin composition layer, as needed. For example, in the resin sheet, a protective film similar to that of the support may be provided on the surface of the resin composition layer not bonded to the support (i.e., the surface opposite to the support). The thickness of the protective film is, for example, 1 μm to 40 μm. The protective film can prevent adhesion of dust and the like to the surface of the resin composition layer and scratches. When the resin sheet has a protective film, the resin sheet can be used by peeling off the protective film. The resin sheet can also be stored by being wound into a roll.

[0106] [Circuit board] The circuit board used in the present invention can be produced, for example, by a production method including the following steps (1) and (2). The cured product of the resin composition described above can be used as a sealing layer for semiconductor chips and the like on a circuit board, as described below. The cured product of the resin composition may also be used to form an insulating layer included in the circuit board. However, the insulating layer may be formed from a material other than the cured product of the resin composition described above. (1) A step of forming a resin composition layer on a substrate. (2) A step of thermally curing the resin composition layer to form an insulating layer.

[0107] In step (1), a substrate is prepared. Examples of the substrate include glass epoxy substrates, metal substrates (such as stainless steel and cold-rolled steel sheet (SPCC)), polyester substrates, polyimide substrates, BT resin substrates, and thermosetting polyphenylene ether substrates. The substrate may also have a metal layer such as copper foil on its surface as part of the substrate. For example, a substrate having a peelable first metal layer and a peelable second metal layer on both surfaces may be used. When using such a substrate, a conductor layer serving as a wiring layer capable of functioning as circuit wiring is typically formed on the surface of the second metal layer opposite the first metal layer. An example of a substrate having such a metal layer is "Micro Thin," an ultra-thin copper foil with a carrier foil manufactured by Mitsui Mining & Smelting Co., Ltd.

[0108] A conductor layer may be formed on one or both surfaces of the substrate. In the following description, a member including a substrate and a conductor layer formed on the substrate surface may be referred to as a "substrate with wiring layer" where appropriate. Examples of conductor materials included in the conductor layer include materials containing 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 material may be a single metal or an alloy. Examples of alloys include alloys of two or more metals selected from the above group (e.g., nickel-chromium alloys, copper-nickel alloys, and copper-titanium alloys). Among these, from the viewpoints of versatility, cost, and ease of patterning in the formation of the conductor layer, single metals such as chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, or copper are preferred; and alloys such as nickel-chromium alloys, copper-nickel alloys, and copper-titanium alloys are preferred. Among these, the single metals chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, and copper; and nickel-chromium alloys; are more preferred, and the single metal copper is particularly preferred.

[0109] The conductor layer may be patterned to function as, for example, a wiring layer. In this case, the line (circuit width) / space (width between circuits) ratio of the conductor layer is not particularly limited, but is preferably 20 / 20 μm or less (i.e., a pitch of 40 μm or less), more preferably 10 / 10 μm or less, even more preferably 5 / 5 μm or less, even more preferably 1 / 1 μm or less, and particularly preferably 0.5 / 0.5 μm or more. The pitch does not need to be uniform throughout the conductor layer. The minimum pitch of the conductor layer may be, for example, 40 μm or less, 36 μm or less, or 30 μm or less.

[0110] The thickness of the conductor layer depends on the design of the circuit board, but is preferably 3 μm to 35 μm, more preferably 5 μm to 30 μm, even more preferably 10 μm to 20 μm, and particularly preferably 15 μm to 20 μm.

[0111] The conductor layer can be formed, for example, by a method including the steps of laminating a dry film (photosensitive resist film) on a substrate, exposing and developing the dry film under predetermined conditions using a photomask to form a pattern to obtain a patterned dry film, forming a conductor layer by a plating method such as electrolytic plating using the developed patterned dry film as a plating mask, and peeling off the patterned dry film. The dry film can be a photosensitive dry film made of a photoresist composition, and can be, for example, a dry film made of a resin such as a novolac resin or an acrylic resin. The lamination conditions for the substrate and dry film can be the same as the lamination conditions for the substrate and resin sheet described below. The dry film can be peeled off using, for example, an alkaline stripping solution such as a sodium hydroxide solution.

[0112] After preparing the substrate, a resin composition layer is formed on the substrate. When a conductor layer is formed on the surface of the substrate, the resin composition layer is preferably formed so that the conductor layer is embedded in the resin composition layer.

[0113] The resin composition layer is formed, for example, by laminating a resin sheet and a substrate. This lamination can be performed, for example, by thermocompression bonding the resin sheet to the substrate from the support side, thereby laminating the resin composition layer to the substrate. Examples of a member for thermocompression bonding the resin sheet to the substrate (hereinafter sometimes referred to as a "thermocompression bonding member") include a heated metal plate (such as a SUS panel) or a metal roll (such as a SUS roll). Note that, rather than pressing the thermocompression bonding member directly onto the resin sheet, it is preferable to press it via an elastic material such as heat-resistant rubber so that the resin sheet can sufficiently conform to the surface irregularities of the substrate.

[0114] The substrate and the resin sheet may be laminated, for example, by a vacuum lamination method. In the vacuum lamination method, the thermocompression temperature is preferably in the range of 60°C to 160°C, more preferably 80°C to 140°C. The thermocompression pressure is preferably in the range of 0.098MPa to 1.77MPa, more preferably 0.29MPa to 1.47MPa. The thermocompression time is preferably in the range of 20 seconds to 400 seconds, more preferably 30 seconds to 300 seconds. The lamination is preferably carried out under reduced pressure conditions of 13hPa or less.

[0115] After lamination, the laminated resin sheets may be smoothed under normal pressure (atmospheric pressure), for example, by pressing the support side with a thermocompression member. The pressing conditions for the smoothing treatment may be the same as the thermocompression conditions for lamination. Note that lamination and smoothing may be performed consecutively using a vacuum laminator.

[0116] The resin composition layer may be formed from the resin sheet or resin composition of the present invention. When the resin composition layer is formed from the resin composition, the resin composition layer may be formed, for example, by a compression molding method. Alternatively, the resin composition layer may be formed by filling a cartridge with the resin composition and discharging the resin composition from the cartridge. The molding conditions may be similar to those of the method for forming the resin composition layer in the step of forming the encapsulating layer of the semiconductor chip package described below.

[0117] After forming the resin composition layer on the substrate, the resin composition layer is thermally cured to form an insulating layer. The thermal curing conditions for the resin composition layer vary depending on the type of resin composition, but the curing temperature is usually in the range of 120°C to 240°C (preferably in the range of 150°C to 220°C, more preferably in the range of 170°C to 200°C), and the curing time is in the range of 5 minutes to 120 minutes (preferably in the range of 10 minutes to 100 minutes, more preferably in the range of 15 minutes to 90 minutes).

[0118] Before the resin composition layer is thermally cured, the resin composition layer may be subjected to a preheating treatment in which the resin composition layer is heated at a temperature lower than the curing temperature. For example, prior to thermally curing the resin composition layer, the resin composition layer may be preheated at a temperature of typically 50°C or higher and lower than 120°C (preferably 60°C or higher and 110°C or lower, more preferably 70°C or higher and 100°C or lower) for typically 5 minutes or longer (preferably 5 to 150 minutes, more preferably 15 to 120 minutes).

[0119] In this manner, a circuit board having an insulating layer can be manufactured. The method for manufacturing a circuit board may further include any optional steps. For example, when a circuit board is manufactured using a resin sheet, the manufacturing method of the circuit board may include a step of peeling off the support of the resin sheet. The support may be peeled off before or after the resin composition layer is thermally cured.

[0120] The method for manufacturing a circuit board may include, for example, a step of polishing the surface of the insulating layer after forming the insulating layer. The polishing method is not particularly limited. For example, the surface of the insulating layer can be polished using a surface grinder.

[0121] The manufacturing method of a circuit board may include, for example, a step of connecting conductor layers to each other, i.e., a step of drilling holes in an insulating layer. This allows holes such as via holes and through holes to be formed in the insulating layer. Examples of methods for forming via holes include laser irradiation, etching, and mechanical drilling. The dimensions and shape of the via holes may be determined appropriately depending on the design of the circuit board. Note that the step of connecting conductor layers to each other may also involve polishing or grinding the insulating layer to achieve the interlayer connection.

[0122] After the via holes are formed, it is preferable to carry out a step of removing smears from the via holes. This step is sometimes called a desmear step. For example, when a conductor layer is formed on an insulating layer by a plating step, a wet desmear treatment may be carried out on the via holes. When a conductor layer is formed on an insulating layer by a sputtering step, a dry desmear step such as a plasma treatment step may be carried out. Furthermore, the insulating layer may be roughened by the desmear step.

[0123] Furthermore, before forming a conductor layer on the insulating layer, the insulating layer may be subjected to a roughening treatment. This roughening treatment typically roughens the surface of the insulating layer, including the interior of the via holes. The roughening treatment may be either a dry or wet roughening treatment. An example of a dry roughening treatment is plasma treatment. An example of a wet roughening treatment is a method in which a swelling treatment using a swelling liquid, a roughening treatment using an oxidizing agent, and a neutralization treatment using a neutralizing liquid are performed in this order.

[0124] After the via holes are formed, a conductor layer is formed on the insulating layer. By forming a conductor layer at the position where the via holes are formed, the newly formed conductor layer and the conductor layer on the surface of the substrate are electrically connected to each other, resulting in interlayer connection. Examples of methods for forming the conductor layer include plating, sputtering, and vapor deposition, with plating being preferred. In a preferred embodiment, the surface of the insulating layer is plated using an appropriate method such as a semi-additive method or a full-additive method to form a conductor layer having a desired wiring pattern. Furthermore, when the support in the resin sheet is a metal foil, a conductor layer having a desired wiring pattern can be formed using a subtractive method. The material of the conductor layer formed may be a single metal or an alloy. Furthermore, this conductor layer may have a single-layer structure or a multi-layer structure including two or more layers of different materials.

[0125] Here, an example of an embodiment in which a conductor layer is formed on an insulating layer will be described in detail. A plating seed layer is formed on the surface of the insulating layer by electroless plating. Next, a mask pattern is formed on the formed plating seed layer, exposing a portion of the plating seed layer corresponding to the desired wiring pattern. After an electrolytic plating layer is formed on the exposed plating seed layer by electrolytic plating, the mask pattern is removed. Thereafter, unnecessary plating seed layer is removed by a process such as etching, thereby forming a conductor layer having the desired wiring pattern. Note that when forming the conductor layer, the dry film used to form the mask pattern is the same as the dry film described above.

[0126] The method for manufacturing a circuit board may include a step of removing the substrate. By removing the substrate, a circuit board having an insulating layer and a conductor layer embedded in the insulating layer is obtained. This step of removing the substrate can be performed, for example, when a substrate having a peelable metal layer is used.

[0127] [Semiconductor chip package] The semiconductor chip package according to the first embodiment of the present invention includes the circuit board described above and a semiconductor chip mounted on the circuit board, and can be manufactured by bonding the semiconductor chip to the circuit board.

[0128] The bonding conditions for the circuit 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 circuit board. For example, the conditions used in flip-chip mounting of semiconductor chips can be used. Furthermore, for example, the semiconductor chip and the circuit board can be bonded via an insulating adhesive.

[0129] An example of a bonding method is a method in which a semiconductor chip is pressure-bonded to a circuit board. Pressure-bonding conditions are a pressure-bonding temperature typically in the range of 120°C to 240°C (preferably 130°C to 200°C, more preferably 140°C to 180°C), and a pressure-bonding time typically in the range of 1 second to 60 seconds (preferably 5 seconds to 30 seconds).

[0130] Another example of a bonding method is to bond the semiconductor chip to the circuit board by reflow. The reflow conditions may be in the range of 120°C to 300°C.

[0131] After bonding the semiconductor chip to the circuit board, the semiconductor chip may be filled with a mold underfill material, which may be the resin composition described above or the resin sheet described above.

[0132] The semiconductor chip package according to the second embodiment of the present invention includes a semiconductor chip and a cured product of the resin composition that encapsulates the semiconductor chip. In such a semiconductor chip package, the cured product of the resin composition typically functions as an encapsulation layer. An example of the semiconductor chip package according to the second embodiment is a fan-out type WLP.

[0133] The manufacturing method of such a semiconductor chip package as a fan-out type WLP is as follows: (A) a step of laminating a temporary fixing film on a substrate; (B) a step of temporarily fixing a semiconductor chip on a temporary fixing film; (C) a step of laminating a resin composition layer of the resin sheet of the present invention on a semiconductor chip, or applying the resin composition of the present invention on a semiconductor chip and thermally curing the composition to form an encapsulating layer; (D) peeling the substrate and the temporary fixing film from the semiconductor chip; (E) a step of forming a rewiring formation layer (insulating layer) on the surface from which the base material and the temporary fixing film of the semiconductor chip have been peeled off; (F) forming a conductor layer (rewiring layer) on the rewiring formation layer (insulating layer); and (G) forming a solder resist layer on the conductor layer. The method for manufacturing a semiconductor chip package may also include (H) dicing the plurality of semiconductor chip packages into individual semiconductor chip packages.

[0134] For details of the method for manufacturing such a semiconductor chip package, please refer to paragraphs 0066 to 0081 of International Publication No. 2016 / 035577, the contents of which are incorporated herein by reference.

[0135] A semiconductor chip package according to a third embodiment of the present invention is, for example, a semiconductor chip package according to the second embodiment, in which the rewiring formation layer or the solder resist layer is formed from a cured product of the resin composition of the present invention.

[0136] [Semiconductor Devices] Examples of semiconductor devices on which the above-mentioned semiconductor chip package is mounted 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]

[0137] 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, "parts" and "%" representing amounts mean "parts by mass" and "% by mass", respectively, unless otherwise specified. Furthermore, the operations described below were carried out in an environment of normal temperature and pressure, unless otherwise specified.

[0138] (Preparation of Silica A) Average particle size 7μm, specific surface area 3.4m 2 / g of spherical silica was surface-treated with KBM-573 (manufactured by Shin-Etsu Chemical Co., Ltd.) to obtain spherical silica A.

[0139] Example 1 Five parts of a liquid epoxy resin ("ZX1059" manufactured by Nippon Steel & Sumikin Chemical Co., Ltd., a 1:1 mixture (by mass) of bisphenol A epoxy resin and bisphenol F epoxy resin, epoxy equivalent: 169 g / eq.), seven parts of a glycidylamine epoxy resin ("630" manufactured by Mitsubishi Chemical Corporation, epoxy equivalent: 95 g / eq.), two parts of a fluorene skeleton-containing epoxy resin ("EG-280" manufactured by Osaka Gas Chemicals Co., Ltd., epoxy equivalent: 460 g / eq.), eight parts of an acid anhydride curing agent ("MH-700" manufactured by New Japan Chemical Co., Ltd., 4-methylhexahydrophthalic anhydride / hexahydrophthalic anhydride = 70 / 30), 140 parts of silica A, and 0.1 parts of a curing accelerator ("1B2PZ" manufactured by Shikoku Chemicals Corporation) were uniformly dispersed using a mixer to obtain resin composition 1.

[0140] <Example 2> In Example 1, 2 parts of a fluorene skeleton-containing epoxy resin ("EG-280" manufactured by Osaka Gas Chemicals Co., Ltd., epoxy equivalent weight 460 g / eq.) was replaced with 2 parts of a liquid alkyleneoxy skeleton- and butadiene skeleton-containing epoxy resin ("EX-991L" manufactured by Nagase ChemteX Corporation, epoxy equivalent weight 450 g / eq.). Resin composition 2 was obtained in the same manner as in Example 1, except for the above-mentioned changes.

[0141] Example 3 In Example 1, 2 parts of a fluorene skeleton-containing epoxy resin ("EG-280" manufactured by Osaka Gas Chemicals Co., Ltd., epoxy equivalent weight 460 g / eq.) was replaced with 2 parts of a liquid alkyleneoxy skeleton-containing epoxy resin ("SR-PTMG" manufactured by Sakamoto Yakuhin Kogyo Co., Ltd., epoxy equivalent weight 420 g / eq.). Resin composition 3 was obtained in the same manner as in Example 1, except for the above-mentioned changes.

[0142] Example 4 In Example 1, 2 parts of the fluorene skeleton-containing epoxy resin ("EG-280" manufactured by Osaka Gas Chemicals Co., Ltd., epoxy equivalent weight 460 g / eq.) was replaced with 2 parts of a liquid siloxane skeleton-containing epoxy resin ("KF-105" manufactured by Shin-Etsu Chemical Co., Ltd., epoxy equivalent weight 490 g / eq.). Resin composition 4 was obtained in the same manner as in Example 1, except for the above-mentioned changes.

[0143] <Example 5> In Example 1, 2 parts of a fluorene skeleton-containing epoxy resin ("EG-280" manufactured by Osaka Gas Chemicals Co., Ltd., epoxy equivalent weight 460 g / eq.) was replaced with 2 parts of a bisphenol A skeleton-containing liquid epoxy resin ("EXA-4816" manufactured by DIC Corporation, epoxy equivalent weight 403 g / eq.). Resin composition 5 was obtained in the same manner as in Example 1 except for the above-mentioned changes.

[0144] Example 6 In Example 1, the amount of the fluorene skeleton-containing epoxy resin ("EG-280" manufactured by Osaka Gas Chemicals Co., Ltd., epoxy equivalent weight 460 g / eq.) was changed from 2 parts to 1 part. Resin composition 6 was obtained in the same manner as in Example 1 except for the above-mentioned changes.

[0145] <Comparative Example 1> In Example 1, 2 parts of a fluorene skeleton-containing epoxy resin ("EG-280" manufactured by Osaka Gas Chemicals Co., Ltd., epoxy equivalent weight 460 g / eq.) was replaced with 2 parts of a liquid epoxy resin ("SR-14BJ" manufactured by Sakamoto Yakuhin Kogyo Co., Ltd., epoxy equivalent weight 102 g / eq.). Resin composition 7 was obtained in the same manner as in Example 1 except for the above-mentioned points.

[0146] <Comparative Example 2> In Example 1, 2 parts of a fluorene skeleton-containing epoxy resin ("EG-280" manufactured by Osaka Gas Chemicals Co., Ltd., epoxy equivalent weight 460 g / eq.) was replaced with 2 parts of a liquid epoxy resin ("SR-16BJ" manufactured by Sakamoto Yakuhin Kogyo Co., Ltd., epoxy equivalent weight 120 g / eq.). Except for the above, the same procedure as in Example 1 was repeated to obtain a resin composition 8.

[0147] <Comparative Example 3> In Example 1, 2 parts of a fluorene skeleton-containing epoxy resin ("EG-280" manufactured by Osaka Gas Chemicals Co., Ltd., epoxy equivalent weight 460 g / eq.) was replaced with 2 parts of a liquid epoxy resin ("X-22-163B" manufactured by Shin-Etsu Chemical Co., Ltd., epoxy equivalent weight 1800 g / eq.). Except for the above, the same procedure as in Example 1 was repeated to obtain a resin composition 9.

[0148] <Comparative Example 4> In Example 4, the amount of liquid epoxy resin ("KF-105" manufactured by Shin-Etsu Chemical Co., Ltd., epoxy equivalent 490 g / eq.) was changed from 2 parts to 5 parts. Resin composition 10 was obtained in the same manner as in Example 4 except for the above-mentioned changes.

[0149] <Comparative Example 5> The amount of silica A in Example 2 was changed from 140 parts to 55 parts. Resin composition 11 was obtained in the same manner as in Example 2 except for the above-mentioned points.

[0150] <Warp evaluation> Each resin composition produced in the Examples and Comparative Examples was compression molded onto a 12-inch silicon wafer using a compression molding machine (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) to form a 300 μm-thick resin composition layer. The wafer was then heated at 180°C for 90 minutes to thermally cure the resin composition layer. This resulted in a sample substrate comprising a silicon wafer and a cured resin composition layer. The amount of warpage of the sample substrate at 25°C was measured using a shadow moiré measurement device ("Thermoire AXP" manufactured by Akorometrix). The measurement was performed in accordance with JEITA EDX-7311-24, a standard of the Japan Electronics and Information Technology Industries Association. Specifically, a virtual plane calculated using the least-squares method for all data on the substrate surface in the measurement area was used as the reference plane. The difference between the minimum and maximum values ​​in the perpendicular direction from this reference plane was determined as the amount of warpage, and the amount of warpage was evaluated according to the following criteria. ○: Warpage is less than 4 mm △: Warpage is 4mm or more and less than 5mm ×: Warpage is 5mm or more

[0151] <Adhesion strength evaluation> The resin compositions prepared in the Examples and Comparative Examples were compression molded onto a 12-inch silicon wafer using a compression molding machine (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) to form a 300 μm-thick resin composition layer. The wafer was then heated at 180°C for 90 minutes to thermally cure the resin composition layer. This resulted in a sample substrate comprising a silicon wafer and a cured resin composition layer. Subsequently, a high-temperature, high-humidity environmental test (HAST) was performed at 130°C and 85% RH for 96 hours. The cured layer after HAST was polished using #180 sandpaper until it reached a thickness of 50 μm. The polished sample was cut into a 1 cm square test piece, and a 2.7 mm diameter stud pin with adhesive was placed perpendicular to the cured layer. The wafer was then heated at 150°C for 60 minutes to produce a test piece in which the stud pin and the cured layer were bonded. The obtained test pieces with stud pins were subjected to a vertical tensile test at a test speed of 0.1 kg / sec using a vertical tensile testing machine "ROMULUS" manufactured by QUAD GROUP Co., Ltd. Measurements were carried out on five test pieces, and the average value was calculated and evaluated according to the following criteria. ○: Adhesion strength is 500kgf / cm 2 Exceeds. ×:500kgf / cm 2 less than.

[0152] <Evaluation of flow marks after molding> The resin compositions prepared in the Examples and Comparative Examples were compression molded onto a 12-inch silicon wafer using a compression molding device (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) to form a resin composition layer with a thickness of 300 μm (the area of ​​the resin composition layer at this time was 14.6 cm × 14.6 × 3.14 = 45.844 cm). 2 The appearance of the resin composition layer was observed. When the area of ​​the flow marks occupied less than 20% of the entire surface of the resin composition layer, it was evaluated as "Good", and when it occupied more than 20% it was evaluated as "Poor".

[0153] <Evaluation of resin surface unevenness after post-cure> The resin compositions prepared in the Examples and Comparative Examples were compression molded onto a 12-inch silicon wafer using a compression molding machine (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) to form a resin composition layer with a thickness of 300 μm (the area of ​​the resin composition layer at this time was 14.6 cm × 14.6 × 3.14 = 45.844 cm). 2 The resin composition layer was then heat-cured by heating at 180°C for 90 minutes, and the appearance of the cured layer was observed. A cured layer with a uniform surface and no color unevenness was rated "Good", and a cured layer with an uneven surface due to color unevenness caused by separation of the resin or the like was rated "Poor".

[0154] [Table 1] In the table, the content of the component (A-1) and the content of the component (B) represent the content when the total amount of nonvolatile components in the resin composition is taken as 100% by mass.

[0155] In Examples 1 to 6, it was confirmed that even when component (D) was not contained, the same results as in the above Examples were obtained, although to a different extent.

Claims

1. (A-1) an epoxy resin having an epoxy equivalent of more than 400 g / eq. and not more than 1000 g / eq.; (B) an inorganic filler, and (C) a curing agent, The resin composition is liquid at 20°C, The amount of the solvent relative to the entire resin composition is 1% by mass or less, The component (A-1) contains one or more skeletons selected from the group consisting of a fluorene skeleton, a butadiene skeleton, an isoprene skeleton, an alkyleneoxy skeleton, and a bisphenol skeleton, The content of the component (A-1) is 0.2% by mass or more and less than 3% by mass, when the total amount of nonvolatile components in the resin composition is 100% by mass, The content of the (B) component is 75% by mass or more when the total amount of nonvolatile components in the resin composition is 100% by mass, A resin composition, wherein A1 is the content of the component (A-1) when the total nonvolatile components in the resin composition is taken as 100 mass%, and B1 is the content of the component (B) when the total nonvolatile components in the resin composition is taken as 100 mass%, and A1 / B1 is 0.001 or more and 2 / 140 or less.

2. The resin composition according to claim 1, further comprising (A-2) an epoxy resin having an epoxy equivalent of 400 g / eq. or less, or an epoxy resin having an epoxy equivalent of more than 1500 g / eq.

3. A resin composition described in claim 1 or 2, wherein the resin composition is liquid.

4. A resin composition described in any one of claims 1 to 3, wherein component (C) includes an acid anhydride-based curing agent.

5. A resin composition described in any one of claims 1 to 4, wherein component (B) is silica.

6. A resin composition described in any one of claims 1 to 5, which is a resin composition for sealing or insulation.

7. A circuit board comprising an insulating layer formed from a cured product of the resin composition described in any one of claims 1 to 6.

8. A semiconductor chip package comprising the circuit board described in claim 7 and a semiconductor chip mounted on the circuit board.

9. A semiconductor chip package comprising a semiconductor chip and a cured product of the resin composition described in any one of claims 1 to 6 that encapsulates the semiconductor chip.

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