Resin composition

Abstract

[Problem] To provide a resin composition that has excellent embedment properties, can suppress warping during curing, and can obtain a cured product with excellent mechanical strength. [Solution] A resin composition comprising (A) an epoxy resin, (B) an inorganic filler, (C) a curing agent, and (D) a non-epoxy compound containing a polyether backbone, wherein the polyether backbone included in component (D) is a polyoxyalkylene backbone composed of one or more monomer units selected from ethylene oxide units and propylene oxide units, the content of component (B) is 70 mass% or more when all non-volatile components in the resin composition are 100 mass%, and the content of component (D) is 1 mass% or more and 30 mass% or less when non-volatile components other than component (B) in the resin composition are 100 mass%.

Description

Technology Field

[0001] The present invention relates to a resin composition comprising an epoxy resin. Furthermore, the present invention relates to a cured product, a resin sheet, a circuit board, a semiconductor chip package, and a semiconductor device obtained using the said resin composition. Background Technology

[0002] Recently, the demand for small, high-performance electronic devices such as smartphones and tablet-type devices has been increasing, and accordingly, there is a demand for sealing materials for semiconductor chip packages used in these small electronic devices to become more high-performance. As such sealing materials, those formed by curing a resin composition are known (Patent Document 1).

[0003] In addition, a resin composition comprising an epoxy compound containing a polyether backbone is known to date (Patent Document 2). In addition, a resin composition comprising a non-epoxy compound containing a polyether backbone containing butylene oxide units is known (Patent Document 3). Prior art literature

[0004] Japanese Patent Publication No. JP 2017-008312, International Publication No. 2018 / 221681, Japanese Patent Publication No. JP 2018-168354 The problem to be solved

[0005] For sealants used in semiconductor chip packages, materials with a low coefficient of linear thermal expansion and excellent dimensional stability are required. As a method to keep the coefficient of linear thermal expansion low, a method of high-filling inorganic fillers in the resin composition is known.

[0006] However, when inorganic fillers are heavily filled into resin materials, the mechanical strength is generally reduced because the resin composition tends to become soft, the melt viscosity increases, and voids tend to form easily during landfilling, which tends to reduce landfillability. At the same time, the elastic modulus increases, making it difficult to suppress bending.

[0007] Accordingly, the objective of the present invention is to provide a resin composition that has excellent embedment properties, can suppress warping during curing, and can obtain a cured product with excellent mechanical strength. means of solving the problem

[0008] In order to achieve the objectives of the present invention, the inventors, after careful consideration, discovered that even a resin composition (B) that is highly filled with inorganic filler, can be used to obtain a cured product that has excellent embeddability, can suppress warping during curing, and has excellent mechanical strength by using a resin composition that includes (D) a non-epoxy compound containing a polyether backbone composed of a predetermined monomer unit and satisfies other predetermined conditions.

[0009] That is, the present invention includes the following contents.

[0010] [1] A resin composition comprising (A) an epoxy resin, (B) an inorganic filler, (C) a curing agent, and (D) a non-epoxy compound containing a polyether backbone,

[0011] (D) The polyether backbone included in the component is a polyoxyalkylene backbone composed of one or more monomer units selected from ethylene oxide units and propylene oxide units, and

[0012] (B) The content of the component is 70 mass% or more when all non-volatile components in the resin composition are considered as 100 mass%, and

[0013] (D) A resin composition in which the content of component (D) is 1 mass% or more and 30 mass% or less when the non-volatile component other than component (B) in the resin composition is 100 mass%.

[0014] [2] (D) A resin composition described in [1], wherein the component is one or more compounds selected from the group consisting of polyalkylene glycol and polyoxyalkylene modified silicone.

[0015] [3] A resin composition described in [2] above, wherein the polyalkylene glycol is polyoxyethylene polyoxypropylene glycol.

[0016] [4] (D) A resin composition described in any one of [1] to [3], wherein the number average molecular weight of the components is 500 to 10,000.

[0017] [5] (D) A resin composition described in any one of [1] to [4], wherein the viscosity of the component at 25°C is 3,000 mPa·s or less.

[0018] [6] (B) A resin composition described in any one of [1] to [5], wherein the content of the component is 78 mass% or more when all non-volatile components in the resin composition are 100 mass%.

[0019] [7] (B) A resin composition described in any one of [1] to [6] above, wherein the component is silica.

[0020] [8] (A) A resin composition described in any one of [1] to [7], wherein the component comprises an epoxy resin containing a condensed ring structure.

[0021] [9] A resin composition described in [8] above, wherein the content of the condensed ring structure-containing epoxy resin in component (A) is 50 mass% or more when the total amount of component (A) is 100 mass%.

[0022]

[10] (A) A resin composition described in any one of [1] to [9], wherein the component comprises a glycidylamine-type epoxy resin.

[0023]

[11] (A) A resin composition described in any one of [1] to

[10] , wherein the component comprises a liquid epoxy resin.

[0024]

[12] A resin composition described in

[11] above, wherein the content of liquid epoxy resin in component (A) is 50 mass% or more when the total amount of component (A) is 100 mass%.

[0025]

[13] A resin composition described in any one of [1] to

[12] , wherein the content of component (A) is 40 mass% or more when the non-volatile component other than component (B) in the resin composition is 100 mass%.

[0026]

[14] (C) A resin composition described in any one of [1] to

[13] , wherein the component comprises one or more curing agents selected from the group consisting of acid anhydride curing agents and amine curing agents.

[0027]

[15] A resin composition described in any one of [1] to

[14] for forming an insulating layer of a semiconductor chip package.

[0028]

[16] A resin composition described in any one of [1] to

[14] for forming an insulating layer of a circuit board.

[0029]

[17] A resin composition described in any one of [1] to

[14] for sealing a semiconductor chip of a semiconductor chip package.

[0030]

[18] A cured product of a resin composition described in any one of [1] to

[17] above.

[0031]

[19] A resin sheet having a support and a resin composition layer comprising a resin composition described in any one of [1] to

[17] provided on the support.

[0032]

[20] A circuit board comprising an insulating layer formed by a cured resin composition described in any one of [1] to

[17] above.

[0033]

[21] A semiconductor chip package comprising a circuit board described in

[20] above and a semiconductor chip mounted on the circuit board.

[0034]

[22] A semiconductor chip package comprising a semiconductor chip and a cured resin composition described in any one of [1] to

[17] that seals the semiconductor chip.

[0035]

[23] A semiconductor device having a semiconductor chip package as described in

[21] or

[22] above. Effects of the invention

[0036] According to the present invention, a resin composition can be provided that has excellent embedment properties, can suppress warping during curing, and can obtain a cured product with excellent mechanical strength. Specific details for implementing the invention

[0037] The present invention will be described in detail below based on suitable embodiments thereof. However, the present invention is not limited to the following embodiments and examples, and may be implemented with arbitrary modifications within the scope of the claims of the present invention and their equivalents without departing from the scope of the claims and equivalents thereof.

[0038] <Resin Composition>

[0039] The resin composition of the present invention comprises (A) an epoxy resin, (B) an inorganic filler, (C) a curing agent, and (D) a non-epoxy compound containing a polyether backbone, wherein the polyether backbone included in component (D) is a polyoxyalkylene backbone composed of one or more monomer units selected from ethylene oxide units and propylene oxide units, and the content of component (B) is 70 mass% or more when all non-volatile components in the resin composition are 100 mass%, and the content of component (D) is 1 mass% or more and 30 mass% or less when non-volatile components other than component (B) in the resin composition are 100 mass%.

[0040] This resin composition has excellent embeddability, can suppress warping during curing, and can obtain a cured product with excellent mechanical strength.

[0041] The resin composition of the present invention may additionally include (E) a curing accelerator, (F) other additives, and (G) an organic solvent, in addition to (A) an epoxy resin, (B) an inorganic filler, (C) a curing agent, and (D) a non-epoxy compound containing a polyether backbone. Each component included in the resin composition will be described in detail below.

[0042] <(A) Epoxy Resin>

[0043] The resin composition of the present invention contains (A) an epoxy resin. (A) An epoxy resin means a resin having epoxy groups.

[0044] (A) As an epoxy resin, for example, bixylenol-type epoxy resin, bisphenol A-type epoxy resin, bisphenol F-type epoxy resin, bisphenol S-type epoxy resin, bisphenol AF-type epoxy resin, dicyclopentadiene-type epoxy resin, trisphenol-type epoxy resin, naphthol novolak-type epoxy resin, phenol novolak-type epoxy resin, tert-butyl-catechol-type epoxy resin, naphthalene-type epoxy resin, naphthol-type epoxy resin, anthracene-type epoxy resin, glycidylamine-type epoxy resin, glycidyl ester-type epoxy resin, cresol novolak-type epoxy resin, biphenyl-type epoxy resin, linear aliphatic epoxy resin, epoxy resin having a butadiene structure, alicyclic epoxy resin, heterocyclic epoxy resin, spiro-ring containing epoxy resin, cyclohexane-type epoxy resin, cyclohexanedimethanol-type epoxy resin, naphthylene ether-type epoxy resin, trimethylol-type epoxy resin, tetraphenylethane-type epoxy resin, Examples include isocyanurate-type epoxy resins. (A) One type of epoxy resin may be used alone, or two or more types may be used in combination.

[0045] (A) It is preferable that the epoxy resin include a glycidylamine type epoxy resin to further improve the heat resistance and copper adhesion of the cured product.

[0046] In addition, (A) the epoxy resin preferably comprises an epoxy resin containing a condensed ring structure from the perspective of imparting excellent heat resistance. Examples of condensed rings in the epoxy resin containing a condensed ring structure include, for instance, a naphthalene ring, an anthracene ring, a phenanthrene ring, etc., and are particularly preferably a naphthalene ring. Accordingly, (A) the epoxy resin particularly preferably comprises an epoxy resin containing a naphthalene ring structure. As for the epoxy resin containing a naphthalene ring structure, for example, an epoxy resin having one naphthalene ring structure in one molecule, such as 1,6-bis(glycidyloxy)naphthalene, 1,5-bis(glycidyloxy)naphthalene, or 2,7-bis(glycidyloxy)naphthalene; Examples include epoxy resins having two naphthalene ring structures in one molecule, such as bis[2-(glycidyloxy)-1-naphthyl]methane, bis[2,7-bis(glycidyloxy)-1-naphthyl]methane, and [2,7-bis(glycidyloxy)-1-naphthyl][2-(glycidyloxy)-1-naphthyl]methane; and polymeric epoxy resins having two or three or more naphthalene ring structures in one molecule, such as naphthol novolak-type epoxy resin, naphthol-phenol coaxial novolak-type epoxy resin, naphthol-cresol coaxial novolak-type epoxy resin, naphthol aralkyl-type epoxy resin, naphthalenediol aralkyl-type epoxy resin, and naphthylene ether-type epoxy resin. Among these, an epoxy resin having one naphthalene ring structure in one molecule is preferred. (A) The content of the epoxy resin containing a condensed ring structure in the epoxy resin is not particularly limited, but when the total amount of (A) epoxy resin is 100 mass%, it is preferably 20 mass% or more, more preferably 40 mass% or more, and particularly preferably 50 mass% or more.

[0047] The resin composition preferably comprises (A) an epoxy resin having two or more epoxy groups in one molecule. With respect to 100 mass% of the non-volatile component of (A) the epoxy resin, the ratio of the epoxy resin having two or more epoxy groups in one molecule is preferably 50 mass% or more, more preferably 60 mass% or more, and particularly preferably 70 mass% or more.

[0048] Epoxy resins include epoxy resins that are in a liquid state at a temperature of 20°C (hereinafter referred to as "liquid epoxy resin") and epoxy resins that are in a solid state at a temperature of 20°C (hereinafter referred to as "solid epoxy resin"). The resin composition of the present invention may include only liquid epoxy resin, or only solid epoxy resin, or a combination of liquid epoxy resin and solid epoxy resin, but it is preferable to include only liquid epoxy resin.

[0049] As for the liquid epoxy resin, a liquid epoxy resin having two or more epoxy groups in one molecule is preferred.

[0050] As liquid epoxy resins, bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol AF type epoxy resin, naphthalene type epoxy resin, glycidyl ester type epoxy resin, glycidylamine type epoxy resin, phenol novolak type epoxy resin, alicyclic epoxy resin having an ester backbone, cyclohexane type epoxy resin, cyclohexanedimethanol type epoxy resin, and epoxy resin having a butadiene structure are preferred.

[0051] Specific examples of liquid epoxy resins include “HP4032”, “HP4032D”, and “HP4032SS” (naphthalene-type epoxy resins) manufactured by DIC; “828US”, “828EL”, “jER828EL”, “825”, and “Epicoto828EL” (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 novolak-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; “630”, “630LSD”, and “604” (glycidylamine-type epoxy resins) manufactured by Mitsubishi Chemical Corporation; and “ED-523T” (glycirol-type epoxy resin) manufactured by ADEKA Corporation. "EP-3950L" and "EP-3980S" manufactured by ADEKA (glycidylamine-type epoxy resin); "EP-4088S" manufactured by ADEKA (dicyclopentadiene-type epoxy resin); "ZX1059" manufactured by Shin-Nippon Steel Sumikin Kagaku (mixture of bisphenol A-type epoxy resin and bisphenol F-type epoxy resin); "EX-721" manufactured by Nagase Chemtex (glycidyl ester-type epoxy resin); "Celoxide 2021P" manufactured by Daicel (alicyclic epoxy resin having an ester backbone); "PB-3600" manufactured by Daicel, and "JP-100" and "JP-200" manufactured by Nippon Soda (epoxy resin having a butadiene structure); Examples include "ZX1658" and "ZX1658GS" (liquid 1,4-glycidylcyclohexane type epoxy resin) manufactured by Shin-Nippon Steel Sumikin Kagaku Co., Ltd. These may be used individually or in combination of two or more types.

[0052] As for the solid epoxy resin, a solid epoxy resin having three or more epoxy groups in one molecule is preferred, and an aromatic solid epoxy resin having three or more epoxy groups in one molecule is more preferred.

[0053] As for solid epoxy resins, bixylenol-type epoxy resin, naphthalene-type epoxy resin, naphthalene-type tetrafunctional epoxy resin, cresol novolak-type epoxy resin, dicyclopentadiene-type epoxy resin, trisphenol-type epoxy resin, naphthol-type epoxy resin, biphenyl-type epoxy resin, naphtylene ether-type epoxy resin, anthracene-type epoxy resin, bisphenol A-type epoxy resin, bisphenol AF-type epoxy resin, and tetraphenylethane-type epoxy resin are preferred.

[0054] Specific examples of solid-phase epoxy resins include “HP4032H” (naphthalene-type epoxy resin) manufactured by DIC; “HP-4700” and “HP-4710” (naphthalene-type tetrafunctional epoxy resins) manufactured by DIC; “N-690” (cresol novolak-type epoxy resin) manufactured by DIC; “N-695” (cresol novolak-type epoxy resin) manufactured by DIC; “HP-7200”, “HP-7200HH”, and “HP-7200H” (dicyclopentadiene-type epoxy resins) manufactured by DIC; and “EXA-7311”, “EXA-7311-G3”, “EXA-7311-G4”, “EXA-7311-G4S” and “HP6000” (naphtylene ether-type epoxy resins) manufactured by DIC. "EPPN-502H" (trisphenol-type epoxy resin) manufactured by Nippon Kayakusha; "NC7000L" (naphthol novolak-type epoxy resin) manufactured by Nippon Kayakusha; "NC3000H", "NC3000", "NC3000L", "NC3100" (biphenyl-type epoxy resin) manufactured by Nippon Kayakusha; "ESN475V" (naphthol-type epoxy resin) manufactured by Shin-Nippon Steel Sumikin Chemicals; "ESN485" (naphthol novolak-type epoxy resin) manufactured by Shin-Nippon Steel Sumikin Chemicals; "YX4000H", "YX4000", "YL6121" (biphenyl-type epoxy resin) manufactured by Mitsubishi Chemicals; "YX4000HK" (bicylenol-type epoxy resin) manufactured by Mitsubishi Chemicals; Examples include “YX8800” (anthracene-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; “YX7700” (xylene-structure-containing novolak-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; “PG-100” and “CG-500” manufactured by Osaka Gas Chemical Corporation; “YL7760” (bisphenol AF-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; “YL7800” (fluorene-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; “jER1010” (solid-phase 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 as a single type, or two or more types may be used in combination.

[0055] In one embodiment, (A) the epoxy resin is particularly preferably a liquid condensed ring structure-containing epoxy resin, and is particularly preferably a liquid naphthalene ring structure-containing epoxy resin. As for the liquid condensed ring (especially naphthalene ring) structure-containing epoxy resin, examples include those having a condensed ring (especially naphthalene ring) structure among the examples given as liquid epoxy resins.

[0056] (A) The content of liquid epoxy resin in the epoxy resin is not particularly limited, but when the total amount of (A) epoxy resin is 100 mass%, it is preferably 50 mass% or more, 60 mass% or more, more preferably 70 mass% or more, 75 mass% or more, even more preferably 80 mass% or more, 85 mass% or more, even more preferably 90 mass% or more, 95 mass% or more, 98 mass% or more, and particularly preferably 100 mass%.

[0057] (A) The epoxy equivalent of the epoxy resin is preferably 50 g / eq. to 5,000 g / eq., more preferably 50 g / eq. to 2,000 g / eq., even more preferably 80 g / eq. to 1,000 g / eq., and even more preferably 80 g / eq. to 500 g / eq. The epoxy equivalent is the mass of the resin containing 1 equivalent of an epoxy group. This epoxy equivalent can be measured according to JIS K7236.

[0058] (A) The weight average molecular weight (Mw) of the epoxy resin is preferably 100 to 5,000, more preferably 200 to 3,000, and even more preferably 250 to 1,500. The weight average molecular weight of the resin can be measured as a polystyrene equivalent value by gel permeation chromatography (GPC).

[0059] The content of (A) epoxy resin in the resin composition is not particularly limited, but when the non-volatile component other than (B) inorganic filler in the resin composition is 100 mass%, it is preferably 10 mass% or more, more preferably 30 mass% or more, even more preferably 40 mass% or more, and particularly preferably 50 mass% or more. The upper limit of the content of (A) epoxy resin in the resin composition is not particularly limited, but when the non-volatile component other than (B) inorganic filler in the resin composition is 100 mass%, it may be, for example, 98 mass% or less, 95 mass% or less, 90 mass% or less, etc.

[0060] <(B) Weapon Filler>

[0061] The resin composition of the present invention contains (B) an inorganic filler.

[0062] (B) The material of the inorganic filler is not particularly limited, but examples 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 zirconate titanate, barium zirconate, calcium zirconate, zirconium phosphate, and zirconium tungstate phosphate, etc., and silica and alumina are particularly suitable. Examples of silica include amorphous silica, fused silica, crystalline silica, synthetic silica, hollow silica, etc. In addition, spherical silica is preferred as the silica. (B) The inorganic filler may be used as a single type or in combination of two or more types.

[0063] (B) Examples of commercially available inorganic fillers include “UFP-30” manufactured by Denka Kagaku Kogyo Co., Ltd.; “SP60-05” and “SP507-05” manufactured by Shin-Nippon Tetsu Sumikin Materials Co., Ltd.; “YC100C”, “YA050C”, “YA050C-MJE” and “YA010C” manufactured by Adomatex Co., Ltd.; “UFP-30” manufactured by Denka Co., Ltd.; “Silfil NSS-3N”, “Silfil NSS-4N” and “Silfil NSS-5N” manufactured by Tokuyama Co., Ltd.; “SC2500SQ”, “SO-C4”, “SO-C2” and “SO-C1” manufactured by Adomatex Co., Ltd.; “DAW-03” and “FB-105FD” manufactured by Denka Co., Ltd.

[0064] (B) The average particle diameter of the inorganic filler is not particularly limited, but preferably 40 μm or less, more preferably 20 μm or less, even more preferably 10 μm or less, even more preferably 5 μm or less, and particularly preferably 3 μm or less. The lower limit of the average particle diameter of the inorganic filler is not particularly limited, but preferably 0.01 μm or more, more preferably 0.05 μm or more, even more preferably 0.1 μm or more, even more preferably 0.5 μm or more, even more preferably 1 μm or more, and particularly preferably 1.5 μm or more. The average particle diameter of the inorganic filler can be measured by a laser diffraction scattering method based on the Mie scattering theory. Specifically, it can be measured by creating a particle diameter distribution of the inorganic filler on a volume basis using a laser diffraction scattering particle diameter distribution measuring device and taking the central diameter as the average particle diameter. For the measurement sample, 100 mg of inorganic filler and 10 g of methyl ethyl ketone can be weighed into a vial and dispersed by ultrasound for 10 minutes. Using a laser diffraction particle diameter distribution measuring device, the wavelength of the light source used was set to blue and red, and the volume-based particle diameter distribution of the inorganic filler was measured using a flow cell method. From the obtained particle diameter distribution, the average particle diameter was calculated as the median diameter. Examples of laser diffraction particle diameter distribution measuring devices include the “LA-960” manufactured by Horiba Sesakusho Co., Ltd.

[0065] (B) The specific surface area of ​​the inorganic filler is not particularly limited, but preferably 0.01 m² / g or more, 0.1 m² / g or more, 0.5 m² / g or more, more preferably 1 m² / g or more, even more preferably 2 m² / g or more, and particularly preferably 3 m² / g or more. There is no particular limit on the upper limit, but preferably 50 m² / g or less, more preferably 20 m² / g or less, 10 m² / g or less, or 5 m² / g or less. The specific surface area of ​​the inorganic filler can be obtained by using a BET fully automatic specific surface area measuring device (Macsorb HM-1210 manufactured by Mounttec) according to the BET method, adsorbing nitrogen gas onto the surface of the sample, and calculating it using the BET multi-point method.

[0066] (B) In terms of increasing moisture resistance and dispersibility, it is preferable that the inorganic filler be treated with one or more surface treatment agents, such as aminosilane coupling agents, epoxysilane coupling agents, mercaptosilane coupling agents, alkoxysilane compounds, organosilazanes compounds, and titanate coupling agents. As commercially available surface treatment agents, for example, "KBM403" (3-glycidoxypropyltrimethoxysilane) manufactured by Shinetsu Kagaku Kokyo Co., Ltd., "KBM803" (3-mercaptopropyltrimethoxysilane) manufactured by Shinetsu Kagaku Kokyo Co., Ltd., "KBE903" (3-aminopropyltriethoxysilane) manufactured by Shinetsu Kagaku Kokyo Co., Ltd., "KBM573" (N-phenyl-3-aminopropyltrimethoxysilane) manufactured by Shinetsu Kagaku Kokyo Co., Ltd., "SZ-31" (hexamethyldisilazane) manufactured by Shinetsu Kagaku Kokyo Co., Ltd., "KBM103" (phenyltrimethoxysilane) manufactured by Shinetsu Kagaku Kokyo Co., Ltd., "KBM-4803" (long-chain epoxy-type silane coupling agent) manufactured by Shinetsu Kagaku Kokyo Co., Ltd. Examples include “KBM-7103” (3,3,3-trifluoropropyltrimethoxysilane), “KBM503” (3-methacryloxypropyltrimethoxysilane) manufactured by Shin-Etsu Kagaku Kogyo Co., Ltd., and “KBM5783” manufactured by Shin-Etsu Kagaku Kogyo Co., Ltd.

[0067] The degree of surface treatment by the surface treatment agent is preferably within a predetermined range from the perspective of improving the dispersibility of the inorganic filler. Specifically, 100 mass% of the inorganic filler is preferably surface-treated with a surface treatment agent of 0.2 mass% to 5 mass%, preferably surface-treated with 0.2 mass% to 3 mass%, and preferably surface-treated with 0.3 mass% to 2 mass%.

[0068] The degree of surface treatment by a surface treatment agent can be evaluated by the carbon content per unit surface area of ​​the inorganic filler. From the perspective of improving the dispersibility of the inorganic filler, the carbon content per unit surface area of ​​the inorganic filler is preferably 0.02 mg / m² or more, more preferably 0.1 mg / m² or more, and even more preferably 0.2 mg / m² or more. Meanwhile, from the perspective of preventing an increase in the melt viscosity of the resin composition or the melt viscosity in sheet form, it is preferably 1.0 mg / m² or less, more preferably 0.8 mg / m² or less, and even more preferably 0.5 mg / m² or less.

[0069] (B) The carbon content per unit surface area of ​​the inorganic filler can be measured after the inorganic filler is cleaned with a solvent (e.g., methyl ethyl ketone (MEK)) following surface treatment. Specifically, a sufficient amount of MEK is added as a solvent to the inorganic filler surface-treated with a surface treatment agent, and ultrasonically cleaned at 25°C for 5 minutes. After removing the supernatant and drying the solids, the carbon content per unit surface area of ​​the inorganic filler can be measured using a carbon analyzer. As a carbon analyzer, the "EMIA-320V" manufactured by Horiba Sesakusho Co., Ltd. can be used.

[0070] The content of (B) inorganic filler in the resin composition is 70 mass% or more when all non-volatile components in the resin composition are 100 mass%, preferably 72 mass% or more, 73 mass% or more, more preferably 74 mass% or more, 75 mass% or more, even more preferably 76 mass% or more, 77 mass% or more, particularly preferably 78 mass% or more, 79 mass% or more, or 80 mass% or more. The upper limit of the content of (B) inorganic filler in the resin composition is not particularly limited, but when all non-volatile components in the resin composition are 100 mass%, it may be, for example, 98 mass% or less, 95 mass% or less, 90 mass% or less, 85 mass% or less, etc.

[0071] <(C) Curing Agent>

[0072] The resin composition of the present invention contains (C) a curing agent. (C) the curing agent has the function of curing (A) the epoxy resin. The curing agent (C) referred to herein is a component that does not correspond to (D) a non-epoxy compound containing a polyether backbone.

[0073] (C) As for the curing agent, although not specifically limited, examples include phenolic curing agents, naphtholic curing agents, acid anhydride curing agents, amine curing agents, active ester curing agents, benzoxazine curing agents, and cyanate ester curing agents. The curing agent may be used alone or in combination of two or more types.

[0074] In one embodiment, (C) the curing agent preferably comprises one or more curing agents selected from the group consisting of acid anhydride-based curing agents and amine-based curing agents.

[0075] As for phenolic curing agents and naphthol-based curing agents, a phenolic curing agent having a novolak structure or a naphthol-based curing agent having a novolak structure is preferred from the perspective of heat resistance and water resistance. In addition, a nitrogen-containing phenolic curing agent or a nitrogen-containing naphthol-based curing agent is preferred from the perspective of adhesion to the substrate, and a triazine-frame-containing phenolic curing agent or a triazine-frame-containing naphthol-based curing agent is more preferred. Among these, a triazine-frame-containing phenol-novolak resin is preferred from the perspective of highly satisfying heat resistance, water resistance, and adhesion. Specific examples of phenolic curing agents and naphthol-based curing agents include, for example, “MEH-7700”, “MEH-7810”, “MEH-7851” manufactured by Meiwa Kasei Co., Ltd., “NHN”, “CBN”, “GPH” manufactured by Nippon Kayaku Co., Ltd., “SN-170”, “SN-180”, “SN-190”, “SN-475”, “SN-485”, “SN-495”, “SN-375”, “SN-395” manufactured by Nittetsu Chemical & Material Co., Ltd., and “LA-7052”, “LA-7054”, “LA-3018”, “LA-3018-50P”, “LA-1356”, “TD2090”, “TD-2090-60M” manufactured by DIC Co., Ltd.

[0076] As for acid anhydride-based curing agents, a curing agent having one or more acid anhydride groups in one molecule may be cited, and a curing agent having two or more acid anhydride groups in one molecule is preferred. Specific examples of acid anhydride-based curing agents 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, benzophenonetetracarboxylic acid dihydride, biphenyltetracarboxylic acid dihydride, naphthalenetetracarboxylic acid dihydride, oxydiphthalic acid dihydride, 3,3'-4,4'-diphenylsulfonetetracarboxylic acid dihydride, Examples of polymeric acid anhydrides include 1,3,3a,4,5,9b-hexahydro-5-(tetrahydro-2,5-dioxo-3-furanyl)-naphtho[1,2-C]furan-1,3-dione, ethylene glycolbis(anhydrotrimellitate), and styrene-maleic acid resin copolymerized with styrene and maleic acid. Examples of commercially available acid anhydride-based curing agents include "HNA-100," "MH-700," "MTA-15," "DDSA," and "OSA" manufactured by Shin Nippon Ricca, "YH-306" and "YH-307" manufactured by Mitsubishi Chemical, and "HN-2200" and "HN-5500" manufactured by Hitachi Kasei.

[0077] As an amine-based curing agent, a curing agent having one or more, preferably two or more, amino groups in one molecule may be cited, for example, aliphatic amines, polyetheramines, alicyclic amines, aromatic amines, etc. Among these, aromatic amines are preferred from the viewpoint of exhibiting the desired effect of the present invention. The amine-based curing agent is preferably a primary amine or a secondary amine, and a primary amine is more preferred. Specific examples of amine-based curing agents include 4,4'-methylenebis(2,6-dimethylaniline), 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, 2,2-bis(3-amino-4-hydroxyphenyl)propane, 3,3-dimethyl-5,5-diethyl-4,4-diphenylmethanediamine, 2,2-bis(4-aminophenyl)propane, 2,2-bis(4-(4-aminophenoxy)phenyl)propane, Examples include 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, bis(4-(3-aminophenoxy)phenyl)sulfone, etc. Commercially available amine-based curing agents may be used, for example, "SEIKACURE-S" manufactured by Seika Co., Ltd., "KAYABOND C-200S", "KAYABOND C-100", "KAYABOND AA", "KAYABOND AB", "KAYABOND AS" manufactured by Nippon Kayaku Co., Ltd., and "Epicure W" manufactured by Mitsubishi Chemical Co., Ltd.

[0078] As for the active ester-based curing agent, there are no particular limitations, but generally, compounds 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, are preferably used. The active ester-based curing agent is preferably 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. Particularly from the perspective of improving heat resistance, an active ester-based curing agent obtained from a carboxylic acid compound and a hydroxy compound is preferred, and an active ester-based curing agent obtained from a carboxylic acid compound and a phenol compound and / or naphthol compound is more preferred. Examples of carboxylic acid compounds include benzoic acid, acetic acid, succinic acid, maleic acid, itaconic acid, phthalic acid, isophthalic acid, terephthalic acid, pyromellitic acid, etc. Examples of phenol compounds or naphthol compounds include hydroquinone, resorcinol, bisphenol A, bisphenol F, bisphenol S, phenolphthalein, 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, phloroglucine, benzenetriol, dicyclopentadiene-type diphenol compounds, phenol novolac, etc. Here, "dicyclopentadiene-type diphenol compound" refers to a diphenol compound obtained by condensing two molecules of phenol with one molecule of dicyclopentadiene.

[0079] Specifically, active ester compounds comprising a dicyclopentadiene-type diphenol structure, active ester compounds comprising a naphthalene structure, active ester compounds comprising an acetylated compound of a phenol novolac, and active ester compounds comprising a benzoylated compound of a phenol novolac are preferred, and among these, active ester compounds comprising a naphthalene structure and active ester compounds comprising a dicyclopentadiene-type diphenol structure are more preferred. "Dicyclopentadiene-type diphenol structure" refers to a divalent structural unit composed of phenylene, dicyclopentylene, and phenylene.

[0080] As commercially available active ester-based curing agents, active ester compounds containing a dicyclopentadiene-type diphenol structure include “EXB9451”, “EXB9460”, “EXB9460S”, “HPC-8000”, “HPC-8000H”, “HPC-8000-65T”, “HPC-8000H-65TM”, “EXB-8000L”, “EXB-8000L-65M”, “EXB-8000L-65TM” (manufactured by DIC); active ester compounds containing a naphthalene structure include “EXB-9416-70BK”, “EXB-8150-65T”, “EXB-8100L-65T”, “EXB-8150L-65T” (manufactured by DIC); Examples of active ester-based curing agents that are acetylated compounds of phenol novolak include “DC808” (manufactured by Mitsubishi Chemical); and examples of active ester-based curing agents that are benzoylated compounds of phenol novolak include “YLH1026” (manufactured by Mitsubishi Chemical), “YLH1030” (manufactured by Mitsubishi Chemical), and “YLH1048” (manufactured by Mitsubishi Chemical).

[0081] Specific examples of benzoxazine-based curing agents include “JBZ-OP100D” and “ODA-BOZ” manufactured by JFE Chemical Co., Ltd.; “HFB2006M” manufactured by Showa Kobunshi Co., Ltd.; and “Pd” and “Fa” manufactured by Shikoku Kasei Kogyo Co., Ltd.

[0082] Examples of cyanate ester-based curing agents include, for instance, bisphenol A dicyanate, polyphenol cyanate (oligo(3-methylene-1,5-phenylene cyanate)), 4,4'-methylenebis(2,6-dimethylphenylcyanate), 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, difunctional cyanate resins, polyfunctional cyanate resins derived from phenol novolac and cresol novolac, and prepolymers in which these cyanate resins are partially triazinated. Specific examples of cyanate ester-based curing agents include “PT30” and “PT60” manufactured by Lonza Japan (both are phenol-novolak type polyfunctional cyanate ester resins), “BA230”, and “BA230S75” (a prepolymer in which part or all of bisphenol A dicyanate is triazinated to become a trimer).

[0083] When the resin composition comprises (A) an epoxy resin and (C) a curing agent, the ratio of (A) the epoxy resin to (C) the curing agent is [number of epoxy groups of (A) epoxy resin]:[number of reactive groups of (C) curing agent], preferably 1:0.2 to 1:2, more preferably 1:0.3 to 1:1.5, and even more preferably 1:0.4 to 1:1.4. Here, the reactive group of (C) the curing agent is, for example, an aromatic hydroxyl group if it is a phenolic curing agent or a naphthol-based curing agent, and an active ester group if it is an active ester-based curing agent, and varies depending on the type of curing agent.

[0084] (C) The reactor equivalent of the curing agent is preferably 50 g / eq. to 3,000 g / eq., more preferably 100 g / eq. to 1,000 g / eq., even more preferably 100 g / eq. to 500 g / eq., and particularly preferably 100 g / eq. to 300 g / eq. The reactor equivalent is the mass of the curing agent per reactor equivalent.

[0085] The content of (C) curing agent in the resin composition is not particularly limited, but when the non-volatile component other than (B) inorganic filler in the resin composition is 100 mass%, it is preferably 80 mass% or less, more preferably 60 mass% or less, even more preferably 50 mass% or less, and particularly preferably 40 mass% or less. The lower limit of the content of (C) curing agent in the resin composition is not particularly limited, but when the non-volatile component other than (B) inorganic filler in the resin composition is 100 mass%, it is, for example, 0.001 mass% or more, 0.01 mass% or more, 0.1 mass% or more, 1 mass% or more, or 2 mass% or more.

[0086] <(D) Non-epoxy compounds containing polyether backbones>

[0087] The resin composition of the present invention contains (D) a non-epoxy compound containing a polyether backbone.

[0088] (D) A non-epoxy compound containing a polyether backbone means a polymer compound having a polyether backbone that does not contain epoxy groups, and the polyether backbone included in (D) a non-epoxy compound containing a polyether backbone is a polyoxyalkylene backbone composed of one or more monomer units selected from ethylene oxide units and propylene oxide units, and does not include a polyether backbone comprising monomer units having 4 or more carbon atoms, such as butylene oxide units and phenylene oxide units. (D) A polyether backbone included in a non-epoxy compound containing a polyether backbone is, particularly preferably, a polyoxyalkylene backbone composed of ethylene oxide units, or a polyoxyalkylene backbone composed of two monomer units, ethylene oxide units and propylene oxide units.

[0089] (D) The average degree of polymerization of monomer units in the polyether backbone included in the polyether backbone-containing non-epoxy compound is preferably 300 or less, more preferably 200 or less, even more preferably 100 or less, and particularly preferably 80 or less.

[0090] In one embodiment, (D) the non-epoxy compound containing a polyether backbone may contain a silicone backbone. The silicone backbone is not particularly limited, but examples include a polydialkyl siloxane backbone such as a polydimethyl siloxane backbone; a polydiaryl siloxane backbone such as a polydiphenyl siloxane backbone; a polyalkylaryl siloxane backbone such as a polymethylphenyl siloxane backbone; a polydialkyl-diaryl siloxane backbone such as a polydimethyl-diphenyl siloxane backbone; a polydialkyl-alkylaryl siloxane backbone such as a polydimethyl-methylphenyl siloxane backbone; a polydiaryl-alkylaryl siloxane backbone such as a polydiphenyl-methylphenyl siloxane backbone; and a polydialkyl siloxane backbone such as a polydiphenyl-methylphenyl siloxane backbone. A polydialkyl siloxane backbone is preferred, and a polydimethyl siloxane backbone is particularly preferred. The (D) component containing the silicone backbone may be a polyoxyalkylene modified silicone, an alkyletherized polyoxyalkylene modified silicone (a polyoxyalkylene modified silicone in which at least a portion of the polyether backbone ends are alkoxy groups), etc. In one embodiment, (D) the non-epoxy compound containing a polyether backbone may contain a hydroxyl group.

[0091] (D) As a non-epoxy compound containing a polyether backbone, for example, a straight-chain polyoxyalkylene glycol (straight-chain polyalkylene glycol) such as polyethylene glycol, polypropylene glycol, polyoxyethylene polyoxypropylene glycol; Polyoxyalkylene glycol (polyalkylene glycol) such as polyoxyethylene glyceryl ether, polyoxypropylene glyceryl ether, polyoxyethylene polyoxypropylene glyceryl ether, polyoxyethylene trimethylolpropane ether, polyoxypropylene trimethylolpropane ether, polyoxyethylene polyoxypropylene trimethylolpropane ether, polyoxyethylene diglyceryl ether, polyoxypropylene diglyceryl ether, polyoxyethylene polyoxypropylene diglyceryl ether, polyoxyethylene pentaerythritol ether, polyoxypropylene pentaerythritol ether, polyoxyethylene polyoxypropylene pentaerythritol ether, polyoxyethylene sorbitol, polyoxypropylene sorbitol, polyoxyethylene polyoxypropylene sorbitol, polyoxyethylene polyoxypropylene sorbitol, etc.; Polyoxyalkylene alkyl ethers such as polyoxyethylene monoalkyl ether, polyoxyethylene dialkyl ether, polyoxypropylene monoalkyl ether, polyoxypropylene dialkyl ether, polyoxyethylene polyoxypropylene monoalkyl ether, polyoxyethylene polyoxypropylene dialkyl ether, etc.; polyoxyalkylene esters such as polyoxyethylene monoester, polyoxyethylene diester, polypropylene glycol monoester, polypropylene glycol diester, polyoxyethylene polyoxypropylene monoester, polyoxyethylene polyoxypropylene diester, etc. (including acetic acid ester, propionic acid ester, butyric acid ester, (meth)acrylic acid ester, etc.);Polyoxyalkylene alkyl ether esters (including acetic acid esters, propionic acid esters, butyric acid esters, (meth)acrylic acid esters, etc.), such as polyoxyethylene monoesters, polyoxyethylene diesters, polyoxypropylene monoesters, polyoxyethylene polyoxypropylene diesters, polyoxyethylene polyoxypropylene monoesters, polyoxyethylene polyoxypropylene diesters, polyoxyethylene alkyl ether esters, polyoxypropylene alkyl ether esters, etc.; polyoxyalkylene alkylamines such as polyoxyethylene alkylamines, polyoxypropylene alkylamines, polyoxyethylene polyoxypropylene alkylamines, etc.; polyoxyalkylene alkylamides such as polyoxyethylene alkylamides, polyoxypropylene alkylamides, polyoxyethylene polyoxypropylene alkylamides, etc.; Examples include polyoxyalkylene modified silicones such as polyoxyethylene dimethicone, polyoxypropylene dimethicone, polyoxyethylene polyoxypropylene dimethicone, polyoxyethylene polydimethylsiloxyalkyl dimethicone, polyoxypropylene polydimethylsiloxyalkyl dimethicone, and polyoxyethylene polyoxypropylene polydimethylsiloxyalkyl dimethicone; alkyl etherified polyoxyalkylene modified silicones such as polyoxyethylene alkyl ether dimethicone, polyoxypropylene alkyl ether dimethicone, polyoxyethylene polyoxypropylene alkyl ether dimethicone, polyoxyethylene alkyl ether polydimethylsiloxyalkyl dimethicone, polyoxypropylene alkyl ether polydimethylsiloxyalkyl dimethicone, and polyoxyethylene polyoxypropylene alkyl ether polydimethylsiloxyalkyl dimethicone (polyoxyalkylene modified silicones in which at least a portion of the polyether backbone ends are alkoxy groups), etc.;

[0092] (D) The polyether-skeleton-containing non-epoxy compound is preferably one or more compounds selected from the group consisting of polyoxyalkylene glycol (polyalkylene glycol) and polyoxyalkylene modified silicone.

[0093] In one embodiment, the polyoxyalkylene glycol (polyalkylene glycol) is preferably a straight-chain polyoxyalkylene glycol (straight-chain polyalkylene glycol).

[0094] The average degree of polymerization of monomer units in polyoxyalkylene glycol (polyalkylene glycol) is preferably 300 or less, more preferably 200 or less, even more preferably 100 or less, and particularly preferably 80 or less. The lower limit is preferably 5 or more, more preferably 10 or more, even more preferably 20 or more, and particularly preferably 30 or more.

[0095] Polyoxyalkylene glycol (polyalkylene glycol) is, particularly preferably, polyoxyethylene-polyoxypropylene glycol. Polyoxyethylene-polyoxypropylene glycol includes polyoxyethylene-polyoxypropylene block copolymers, polyoxyethylene-polyoxypropylene-polyoxyethylene block copolymers, polyoxypropylene-polyoxyethylene-polyoxypropylene block copolymers, etc.

[0096] The average degree of polymerization of ethylene oxide units in polyoxyethylene polyoxypropylene glycol is preferably 200 or less, more preferably 100 or less, even more preferably 50 or less, and particularly preferably 30 or less. The lower limit is preferably 3 or more, more preferably 5 or more, even more preferably 10 or more, and particularly preferably 15 or more. The average degree of polymerization of propylene oxide units in polyoxyethylene polyoxypropylene glycol is preferably 200 or less, more preferably 100 or less, even more preferably 50 or less, and particularly preferably 40 or less. The lower limit is preferably 3 or more, more preferably 5 or more, even more preferably 10 or more, and particularly preferably 15 or more.

[0097] In one embodiment, (D) the polyether backbone-containing non-epoxy compound is, chemical formula (1):

[0098] [Chemical Formula (1)]

[0099]

[0100] It is preferable that the compound is represented by, and chemical formula (1'):

[0101] [Chemical formula (1')]

[0102]

[0103] It is particularly desirable that the compound represented by (block copolymer of x1 unit, x2 unit, and x3 unit) be a compound.

[0104] In chemical formula (1), 2 R 1 Each independently represents a hydrogen atom, an alkyl group (preferably having 1 to 6 carbon atoms), an alkenyl group (preferably having 2 to 6 carbon atoms), an alkyl-carbonyl group (preferably having 2 to 7 carbon atoms), or an alkenyl-carbonyl group (preferably having 3 to 7 carbon atoms). Two Rs 1 The atom is, particularly preferably, a hydrogen atom. An alkyl(group) refers to a straight-chain, branched-chain, and / or cyclic monovalent aliphatic saturated hydrocarbon group. Examples of alkyl(groups) include a methyl group, an ethyl group, a propyl group, an isopropyl group, a butyl group, an isobutyl group, a sec-butyl group, a tert-butyl group, a pentyl group, an isopentyl group, a neopentyl group, a sec-pentyl group, a tert-pentyl group, a cyclopentyl group, a cyclohexyl group, etc. An alkenyl(group) refers to a straight-chain, branched-chain, and / or cyclic monovalent aliphatic unsaturated hydrocarbon group having at least one carbon-carbon double bond. Examples of alkenyl(groups) include a vinyl group, a 1-propenyl group, a 2-propenyl group, etc.

[0105] In chemical formula (1), n ​​is independently 2 or 3.

[0106] In chemical formula (1), x represents an integer from 5 to 300. x is preferably an integer from 5 to 200, and particularly preferably an integer from 10 to 100.

[0107] In chemical formula (1'), x1 and x3 are each independently integers from 3 to 200. Preferably, x1 and x3 are each independently integers from 3 to 100.

[0108] In chemical formula (1'), x2 is an integer from 3 to 200. x2 is preferably an integer from 5 to 100.

[0109] In one embodiment, the polyoxyalkylene modified silicone is, for example, a straight-chain or branched-chain dimethylpolysiloxane (dimethicone) having one or more polyoxyalkylene chains, and preferably is polyoxyethylene dimethicone or polyoxyethylene polydimethylsiloxyalkyl dimethicone.

[0110] The average degree of polymerization of monomer units of one polyoxyalkylene chain in polyoxyalkylene modified silicone is preferably 30 or less, more preferably 20 or less, even more preferably 15 or less, and particularly preferably 10 or less. The lower limit is preferably 2 or more.

[0111] In one embodiment, (D) the non-epoxy compound containing a polyether backbone is, formula (2):

[0112] [Chemical Formula (2)]

[0113]

[0114] It is preferable that it be a polyoxyalkylene modified silicone represented by.

[0115] In chemical formula (2), a represents an integer from 2 to 10,000. a is preferably an integer from 2 to 5,000, more preferably an integer from 2 to 1,000, even more preferably an integer from 2 to 500, and particularly preferably an integer from 2 to 200.

[0116] In chemical formula (2), 4 + a R 2 Each independently represents an alkyl group (preferably having 1 to 6 carbon atoms), an aralkyl group (preferably having 7 to 15 carbon atoms), or an aryl group (preferably having 6 to 14 carbon atoms). 4 + a number of R groups 2Each is independently, preferably, an alkyl group (preferably having 1 to 6 carbon atoms), and particularly preferably, a methyl group. An aryl group refers to a monovalent aromatic hydrocarbon group. Examples of aryl groups include a phenyl group, a 1-naphthyl group, a 2-naphthyl group, etc., and preferably a phenyl group. An aralkyl group refers to an alkyl group substituted with one or more aryl groups. Examples of aralkyl groups include a benzyl group, a phenethyl group, a 2-naphthylmethyl group, etc.

[0117] In chemical formula (2), 2 R 3 and a number of R 4 Each independently, an alkyl group (preferably having 1 to 6 carbon atoms), an aralkyl group (preferably having 7 to 15 carbon atoms), an aryl group (preferably having 6 to 14 carbon atoms), chemical formula (X):

[0118] [Chemical formula (X)]

[0119]

[0120] A group represented by, or chemical formula (Y):

[0121] [Chemical Formula (Y)]

[0122]

[0123] It represents the energy indicated by , and also 2 R 3 and a number of R 4 At least one of them is a group represented by the chemical formula (X). Preferably, two Rs 3 Each is independently an alkyl group (preferably having 1 to 6 carbon atoms), an aralkyl group (preferably having 7 to 15 carbon atoms), or an aryl group (preferably having 6 to 14 carbon atoms), and a group of R 4Each is independently an alkyl group (preferably having 1 to 6 carbon atoms), an aralkyl group (preferably having 7 to 15 carbon atoms), an aryl group (preferably having 6 to 14 carbon atoms), a group represented by chemical formula (X), or a group represented by chemical formula (Y), and also a number of R 4 At least one of them is a group represented by the chemical formula (X). More preferably, two Rs 3 Each is independently a methyl group, and a number of R 4 Each is independently a methyl group, a group represented by chemical formula (X), or a group represented by chemical formula (Y), and also a number of R 4 At least one of them is a group represented by the chemical formula (X).

[0124] In chemical formula (2), the group represented by chemical formula (X) is preferably 1 to 20, more preferably 1 to 10, and particularly preferably 1 to 5. In chemical formula (2), the group represented by chemical formula (Y) is preferably 0 to 20, more preferably 0 to 10, and particularly preferably 0 to 5.

[0125] In chemical formulas (X) and (Y), * represents a bond.

[0126] In the chemical formula (X), R 1 and n are respectively R in chemical formula (1) 1 and is the same as the definition of n.

[0127] In the chemical formula (X), X represents a single bond or an alkylene group (preferably having 1 to 6 carbon atoms). An alkylene group refers to a straight-chain, branched-chain, and / or cyclic divalent aliphatic saturated hydrocarbon group. Examples of alkylene groups include a methylene group, an ethylene group, a trimethylene group, a tetramethylene group, a pentamethylene group, a hexamethylene group, etc.

[0128] In the chemical formula (X), y represents an integer from 2 to 300. y is preferably an integer from 2 to 100, more preferably an integer from 2 to 50, and particularly preferably an integer from 2 to 20.

[0129] In the chemical formula (Y), b represents an integer from 1 to 10,000. b is preferably an integer from 1 to 1,000, more preferably an integer from 1 to 500, even more preferably an integer from 1 to 200, and particularly preferably an integer from 1 to 100.

[0130] In the chemical formula (Y), 3 + 2b R 5 Each independently represents an alkyl group (preferably having 1 to 6 carbon atoms), an aralkyl group (preferably having 7 to 15 carbon atoms), or an aryl group (preferably having 6 to 14 carbon atoms). 3 + 2b R groups 5 Each is independently, preferably, an alkyl group (preferably having 1 to 6 carbon atoms), and particularly preferably, a methyl group.

[0131] In the chemical formula (Y), Y represents an alkylene group (preferably having 1 to 6 carbon atoms).

[0132] (D) The number average molecular weight of the non-epoxy compound containing the polyether backbone is preferably 500 to 40,000, more preferably 500 to 20,000, and even more preferably 500 to 10,000. (D) The weight average molecular weight of the non-epoxy compound containing the polyether backbone is preferably 500 to 40,000, more preferably 500 to 20,000, and even more preferably 500 to 10,000. The number average molecular weight and the weight average molecular weight can be measured as polystyrene equivalent values ​​by gel permeation chromatography (GPC).

[0133] (D) The polyether-backed non-epoxy compound is preferably in a liquid state at 25°C. (D) The viscosity of the polyether-backed non-epoxy compound at 25°C is preferably 100,000 mPa·s or less, more preferably 50,000 mPa·s or less, or 30,000 mPa·s or less, even more preferably 10,000 mPa·s or less, or 5,000 mPa·s or less, even more preferably 4,000 mPa·s or less, or 3,000 mPa·s or less, particularly preferably 2,000 mPa·s or less, or 1,500 mPa·s or less. (D) The lower limit of the viscosity of the non-epoxy compound containing a polyether backbone at 25°C is preferably 10 mPa·s or more, more preferably 20 mPa·s or more, even more preferably 30 mPa·s or more, even more preferably 40 mPa·s or more, and particularly preferably 50 mPa·s or more. The viscosity may be the viscosity (mPa·s) obtained by measuring with a Type B viscometer.

[0134] (D) As non-epoxy compounds containing a polyether backbone, for example, “Pronon #102,” “Pronon #104,” “Pronon #201,” “Pronon #202B,” “Pronon #204,” “Pronon #208,” “Unilub 70DP-600B,” and “Unilub 70DP-950B” (polyoxyethylene polyoxypropylene glycol) manufactured by Nichiyu; "Pluronic L-23", "Pluronic L-31", "Pluronic L-44", "Pluronic L-61", "ADEKA Pluronic L-62", "Pluronic L-64", "Pluronic L-71", "Pluronic L-72", "Pluronic L-101", "Pluronic L-121", "Pluronic P-84", "Pluronic P-85", "Pluronic P-103", "Pluronic F-68", "Pluronic F-88", "Pluronic F-108", "Pluronic 25R-1", "Pluronic 25R-2", "Pluronic 17R-2", "Pluronic 17R-3", "Pluronic 17R-4" (polyoxyethylene polyoxypropylene glycol) manufactured by ADEKA; "KF-6011", "KF-6011P", "KF-6012", "KF-6013", "KF-6015", "KF-6016", "KF-6017", "KF-6017P", "KF-6043", "KF-6004", "KF351A", "KF352A", "KF353", "KF354L", "KF355A", "KF615A", "KF945", "KF-640", "KF-642", "KF-643", "KF-644", "KF-6020", "KF-6204", "X22-4515" manufactured by Shin-Etsu Silicon Examples include “KF-6028”, “KF-6028P”, “KF-6038”, “KF-6048”, and “KF-6025” (polyoxyalkylene modified silicone).

[0135] The content of the (D) polyether backbone-containing non-epoxy compound in the resin composition is 1 mass% or more, preferably 2 mass% or more, more preferably 3 mass% or more, even more preferably 4 mass% or more, and particularly preferably 5 mass% or more, when the non-volatile component other than the (B) inorganic filler in the resin composition is 100 mass%. The upper limit of the content of the (D) polyether backbone-containing non-epoxy compound in the resin composition is 30 mass% or less, preferably 27 mass% or less, more preferably 25 mass% or less, even more preferably 23 mass% or less, and particularly preferably 22 mass% or less, when the non-volatile component other than the (B) inorganic filler in the resin composition is 100 mass%.

[0136] <(E) Curing Accelerator>

[0137] The resin composition of the present invention may contain (E) a curing accelerator as an optional nonvolatile component. (E) The curing accelerator has the function of promoting the curing of (A) the epoxy resin. The curing accelerator (E) mentioned herein is a component that does not correspond to (D) a non-epoxy compound containing a polyether backbone.

[0138] (E) The curing accelerator preferably comprises at least one selected from the group consisting of 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, and more preferably comprises an imidazole-based curing accelerator.

[0139] As phosphorus-based curing accelerators, for example, aliphatic phosphonium salts such as tetrabutylphosphonium bromide, tetrabutylphosphonium chloride, tetrabutylphosphonium acetate, tetrabutylphosphonium decanoate, tetrabutylphosphonium laurate, bis(tetrabutylphosphonium)pyromellitate, tetrabutylphosphonium hydrogen hexahydrophthalate, tetrabutylphosphonium 2,6-bis[(2-hydroxy-5-methylphenyl)methyl]-4-methylphenorate, and di-tert-butylmethylphosphonium tetraphenylborate; Aromatic phosphonium salts such as methyltriphenylphosphonium bromide, ethyltriphenylphosphonium bromide, propyltriphenylphosphonium bromide, butyltriphenylphosphonium bromide, benzyltriphenylphosphonium chloride, tetraphenylphosphonium bromide, p-tolyltriphenylphosphonium tetra-p-tolylborate, tetraphenylphosphonium tetraphenylborate, tetraphenylphosphonium tetrap-tolylborate, triphenylethylphosphonium tetraphenylborate, tris(3-methylphenyl)ethylphosphonium tetraphenylborate, tris(2-methoxyphenyl)ethylphosphonium tetraphenylborate, (4-methylphenyl)triphenylphosphonium thiocyanate, tetraphenylphosphonium thiocyanate, butyltriphenylphosphonium thiocyanate, etc.; aromatic phosphine-borane complexes such as triphenylphosphine-triphenylborane; Aromatic phosphine-quinone addition products such as triphenylphosphine·p-benzoquinone addition products; aliphatic phosphines such as tributylphosphine, tri-tert-butylphosphine, trioctylphosphine, di-tert-butyl(2-butenyl)phosphine, di-tert-butyl(3-methyl-2-butenyl)phosphine, 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, tris(3,5-dimethylphenyl)phosphine, tris(2,4,6-trimethylphenyl)phosphine, tris(2,6-dimethyl-4-ethoxyphenyl)phosphine, Examples include aromatic phosphines such as 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.

[0140] As urea-based curing accelerators, for example, 1,1-dimethylurea; aliphatic dimethylureas such as 1,1,3-trimethylurea, 3-ethyl-1,1-dimethylurea, 3-cyclohexyl-1,1-dimethylurea, 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, 3-(3,4-dimethylphenyl)-1,1-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, Examples of aromatic dimethylureas include 3-[3-(trifluoromethyl)phenyl]-1,1-dimethylurea, N,N-(1,4-phenylene)bis(N',N'-dimethylurea), N,N-(4-methyl-1,3-phenylene)bis(N',N'-dimethylurea) [toluenebisdimethylurea].

[0141] As guanidine-based curing accelerators, for example, 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]deca-5-ene, 7-methyl-1,5,7-triazabicyclo[4.4.0]deca-5-ene, 1-methylbiguanide, 1-ethylbiguanide, 1-n-butylbiguanide, 1-n-octadecylbiguanide, 1,1-dimethylbiguanide, 1,1-diethylbiguanide, 1-cyclohexylbiguanide, 1-allylbiguanide, Examples include 1-phenylbiguanide, 1-(o-tolylbiguanide, etc.).

[0142] As imidazole-based curing accelerators, for example, 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-undecylimidazolium 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-methyl-5-hydroxymethylimidazole, Examples include imidazole compounds such as 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 and epoxy resins.

[0143] The molecular weight of the imidazole-based curing accelerator is not particularly limited, but in order to improve workability (flowability) and suppress melting residue during heat molding, it is preferably 1,000 or less, more preferably 600 or less, even more preferably 400 or less, and particularly preferably 300 or less.

[0144] Examples of metal-based hardening 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 octylate, tin octylate, zinc naphthenate, cobalt naphthenate, tin stearate, and zinc stearate.

[0145] Examples of amine-based curing accelerators include trialkylamines such as triethylamine and tributylamine, 4-dimethylaminopyridine (DMAP), benzyldimethylamine, 2,4,6-tris(dimethylaminomethyl)phenol, and 1,8-diazabicyclo(5,4,0)-undecene.

[0146] The content of (E) curing accelerator in the resin composition is not particularly limited, but when the non-volatile component other than component (B) in the resin composition is 100 mass%, it is preferably 10 mass% or less, more preferably 5 mass% or less, even more preferably 3 mass% or less, and particularly preferably 1 mass% or less. The lower limit of the content of (E) curing accelerator in the resin composition is not particularly limited, but when the non-volatile component other than component (B) in the resin composition is 100 mass%, it may be, for example, 0 mass% or more, 0.001 mass% or more, 0.01 mass% or more, 0.1 mass% or more, 0.2 mass% or more, 0.3 mass% or more, 0.4 mass% or more, etc.

[0147] <(F) Other Additives>

[0148] The resin composition of the present invention may additionally include any additive as a non-volatile component. Such additives include, for example, organic fillers such as rubber particles, polyamide microparticles, silicone particles; thermoplastic resins such as polycarbonate resin, phenoxy resin, polyvinyl acetal resin, polyolefin resin, polysulfone resin, polyester resin; organometallic compounds such as organocopper compounds, organozinc compounds, and organocobalt compounds; coloring agents such as phthalocyanine blue, phthalocyanine green, iodine green, diazo yellow, crystal violet, titanium oxide, and carbon black; polymerization inhibitors such as hydroquinone, catechol, pyrogallol, and phenothiazine; leveling agents such as silicone-based leveling agents and acrylic polymer-based leveling agents; thickeners such as bentonite and montmorillonite; defoaming agents such as silicone-based defoaming agents, acrylic-based defoaming agents, fluorine-based defoaming agents, and vinyl resin-based defoaming agents; and ultraviolet absorbers such as benzotriazole-based ultraviolet absorbers. Examples include adhesion enhancers such as urea silanes; adhesion promoters such as triazole-based adhesion promoters, tetrazole-based adhesion promoters, and triazine-based adhesion promoters; antioxidants such as hindered phenol-based antioxidants and hindered amine-based antioxidants; fluorescent whitening agents such as stilbene derivatives; surfactants such as fluorine-based surfactants; and flame retardants such as phosphorus-based flame retardants (e.g., phosphate ester compounds, phosphazene compounds, phosphinic acid compounds, red phosphate), nitrogen-based flame retardants (e.g., melamine sulfate), halogen-based flame retardants, and inorganic flame retardants (e.g., antimony trioxide). One type of additive may be used alone, or two or more types may be used in combination in any proportion. (F) The content of other additives can be appropriately set by a person skilled in the art.

[0149] <(G) Organic solvents>

[0150] The resin composition of the present invention may additionally contain any organic solvent as a volatile component in addition to the non-volatile component described above. (G) Known organic solvents may be appropriately used, and the type thereof is not particularly limited. (G) As organic solvents, for example, ketone-based solvents such as acetone, methyl ethyl ketone, methyl isobutyl ketone, cyclohexanone; ester-based solvents such as methyl acetate, ethyl acetate, butyl acetate, isobutyl acetate, isoamyl acetate, methyl propionate, ethyl propionate, γ-butyrolactone; ether-based solvents such as tetrahydropyran, tetrahydrofuran, 1,4-dioxane, diethyl ether, diisopropyl ether, dibutyl ether, diphenyl ether; alcohol-based solvents such as methanol, ethanol, propanol, butanol, ethylene glycol; Ether ester solvents such as 2-ethoxyethyl acetate, propylene glycol monomethyl ether acetate, diethylene glycol monoethyl ether acetate, ethyl diglycol acetate, γ-butyrolactone, methyl methoxypropionate, etc.; ester alcohol solvents such as methyl lactate, ethyl lactate, 2-methyl hydroxyisobutyrate, etc.; ether alcohol solvents such as 2-methoxypropanol, 2-methoxyethanol, 2-ethoxyethanol, propylene glycol monomethyl ether, diethylene glycol monobutyl ether (butylcarbitol), etc.; amide solvents such as N,N-dimethylformamide, N,N-dimethylacetamide, N-methyl-2-pyrrolidone, etc.; sulfoxide solvents such as dimethyl sulfoxide; nitrile solvents such as acetonitrile, propionitrile, etc.; Examples include aliphatic hydrocarbon solvents such as hexane, cyclopentane, cyclohexane, and methylcyclohexane; aromatic hydrocarbon solvents such as benzene, toluene, xylene, ethylbenzene, and trimethylbenzene. (G) The organic solvent may be used as a single type or two or more types may be used in combination in any proportion. In one embodiment, (G) the amount of the organic solvent is preferably as small as possible (for example, when the non-volatile component in the resin composition is 100 mass%, 3 mass% or less, 1 mass% or less, 0.It is particularly desirable not to include 5 mass% or less, 0.1 mass% or less, 0.01 mass% or less).

[0151] <Method for manufacturing a resin composition>

[0152] The resin composition of the present invention may be prepared by adding and mixing (A) an epoxy resin, (B) an inorganic filler, (C) a curing agent, (D) a non-epoxy compound containing a polyether backbone, (E) a curing accelerator as needed, (F) other additives as needed, and (G) an organic solvent as needed, in any order and / or in part or in whole, simultaneously, in any reaction vessel, for example. Additionally, the temperature may be appropriately set during the process of adding and mixing each component, and heating and / or cooling may be performed temporarily or over time. Furthermore, stirring or shaking may be performed during the process of adding and mixing each component. Additionally, the resin composition may be uniformly dispersed by stirring using a stirring device, for example, a mixer, at the time of adding and mixing or thereafter.

[0153] Characteristics of the Resin Composition

[0154] The resin composition of the present invention comprises (A) an epoxy resin, (B) an inorganic filler, (C) a curing agent, and (D) a non-epoxy compound containing a polyether backbone, wherein the polyether backbone included in component (D) is a polyoxyalkylene backbone composed of one or more monomer units selected from ethylene oxide units and propylene oxide units, the content of (B) an inorganic filler is 70 mass% or more when all non-volatile components in the resin composition are 100 mass%, and the content of (D) a non-epoxy compound containing a polyether backbone is 1 mass% or more and 30 mass% or less when non-volatile components other than (B) an inorganic filler in the resin composition are 100 mass%, thereby obtaining a cured product having excellent embeddability, capable of suppressing warping during curing, and having excellent mechanical strength.

[0155] In one embodiment, the resin composition of the present invention has excellent embedding properties, so when the melt viscosity is measured, for example, as in Test Example 5 below, the lowest melt viscosity can be preferably 100 poise or less, more preferably 50 poise or less, even more preferably 20 poise or less, and particularly preferably 10 poise or less.

[0156] In one embodiment, the resin composition of the present invention can suppress warping during curing, so when warping is measured in accordance with JEITA EDX-7311-24, for example, as in Test Example 1 below, the amount of warping can be preferably less than 20 mm, more preferably less than 10 mm, even more preferably less than 5 mm, and particularly preferably less than 3 mm.

[0157] In one embodiment, the resin composition of the present invention can obtain a cured product with excellent mechanical strength, so when the 3-point bending strength of the cured product at 23°C is measured, for example, as in Test Example 3 below, the 3-point bending strength can preferably be greater than 10 MPa, more preferably greater than 30 MPa, even more preferably greater than 40 MPa, and particularly preferably greater than 50 MPa.

[0158] In one embodiment, the elastic modulus of the cured resin composition of the present invention at 25°C, when measured in accordance with JIS K7127 as in Test Example 2 below, can be particularly preferably 25 GPa or less, more preferably 20 GPa or less, even more preferably 17 GPa or less, and particularly preferably 15 GPa or less.

[0159] In one embodiment, when the gelation time of the resin composition of the present invention is measured in accordance with JIS C6521, for example, as in Test Example 4 below, it may preferably be 500 seconds or less, more preferably 400 seconds or less, even more preferably 350 seconds or less, and particularly preferably 300 seconds or less.

[0160] <Uses of Resin Composition>

[0161] The cured product of the resin composition of the present invention is particularly useful for the sealing layer and insulating layer of a semiconductor due to the above-mentioned advantages. Accordingly, this resin composition can be used as a resin composition for semiconductor sealing or insulating layer.

[0162] For example, the resin composition of the present invention can be suitably used as a resin composition for forming an insulating layer of a semiconductor chip package (a resin composition for an insulating layer of a semiconductor chip package) and as a resin composition for forming an insulating layer of a circuit board (including a printed circuit board) (a resin composition for an insulating layer of a circuit board).

[0163] In addition, for example, the resin composition of the present invention can be suitably used as a resin composition for sealing a semiconductor chip of a semiconductor chip package (a resin composition for sealing a semiconductor chip).

[0164] Examples of semiconductor chip packages to which a sealing layer or insulating layer formed from a cured resin composition of the present invention can be applied 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.

[0165] In addition, the resin composition of the present invention may be used as an underfill material, and may also be used as a material for Molding Under Filling (MUF) used after connecting a semiconductor chip to a substrate, for example.

[0166] In addition, the resin composition of the present invention can be used in a wide range of applications where resin compositions are used, such as sheet-like laminated materials like resin sheets and prepregs, liquid materials like resin inks for solder resists, die bonding materials, hole-filling resins, and component-filling resins.

[0167] Suzy Sheet

[0168] The resin sheet of the present invention comprises a support and a resin composition layer provided on the support. The resin composition layer is a layer comprising the resin composition of the present invention, and is typically formed of a resin composition.

[0169] The thickness of the resin composition layer is preferably 600 μm or less, more preferably 500 μm or less, from the perspective of thinning. The lower limit of the thickness of the resin composition layer may be preferably 1 μm or more, 5 μm or more, more preferably 10 μm or more, even more preferably 50 μm or more, and particularly preferably 100 μm or more.

[0170] In addition, the thickness of the cured product obtained by curing the resin composition layer is preferably 600 μm or less, more preferably 500 μm or less. The lower limit of the thickness of the cured product is preferably 1 μm or more, 5 μm or more, more preferably 10 μm or more, even more preferably 50 μm or more, and particularly preferably 100 μm or more.

[0171] Examples of supports include films made of plastic materials, metal foils, and release papers, and films made of plastic materials and metal foils are preferred.

[0172] When a film made of a plastic material is used as a support, the plastic material may include, for example, polyesters such as polyethylene terephthalate (hereinafter abbreviated as "PET") and polyethylene naphthalate (hereinafter abbreviated as "PEN"); polycarbonate (hereinafter abbreviated as "PC"); acrylic polymers such as polymethyl methacrylate (hereinafter abbreviated as "PMMA"); cyclic polyolefins; triacetylcellulose (hereinafter abbreviated as "TAC"); polyether sulfide (hereinafter abbreviated as "PES"); polyether ketones; polyimides, etc. Among these, polyethylene terephthalate and polyethylene naphthalate are preferred, and inexpensive polyethylene terephthalate is particularly preferred.

[0173] When using a metal foil as a support, examples of metal foils include copper foil and aluminum foil. Among these, copper foil is preferred. As for the copper foil, a foil made of copper may be used, or a foil made of an alloy of copper and other metals (e.g., tin, chromium, silver, magnesium, nickel, zirconium, silicon, titanium, etc.) may be used.

[0174] The support may have a surface bonded to the resin composition layer treated with matting, corona treatment, antistatic treatment, etc.

[0175] In addition, as a support, a support with a release layer attached having a release layer on the surface bonded to the resin composition layer may be used. As a release agent used in the release layer of the support with a release layer attached, for example, one or more release agents selected from the group consisting of alkyd resin, polyolefin resin, urethane resin, and silicone resin may be used. As commercially available release agents, for example, alkyd resin-based release agents such as "SK-1," "AL-5," and "AL-7" manufactured by Lintec Co., Ltd. may be used. In addition, as a support with a release layer attached, for example, "Lumira T60" manufactured by Tore Co., Ltd.; "Purex" manufactured by Teijin Co., Ltd.; and "Unifil" manufactured by Unichika Co., Ltd. may be used.

[0176] The thickness of the support is preferably in the range of 5㎛ to 75㎛, and more preferably in the range of 10㎛ to 60㎛. Meanwhile, when using a support with a release layer attached, it is preferable that the total thickness of the support with the release layer attached is within the above range.

[0177] A resin sheet can be manufactured, for example, by applying a resin composition onto a support using a coating device such as a die coater. Additionally, if necessary, a resin varnish may be prepared by dissolving the resin composition in an organic solvent, and the resin sheet may be manufactured by applying this resin varnish. By using an organic solvent, the viscosity can be adjusted to improve the applicability. When a resin composition or resin varnish containing an organic solvent is used, the resin composition or resin varnish is typically dried after application to form a resin composition layer.

[0178] Drying may be carried out by known methods such as heating or hot air spraying. The drying conditions are such that the content of the organic solvent in the resin composition layer is typically 10 mass% or less, preferably 5 mass% or less. Although it varies depending on the boiling point of the organic solvent in the resin composition or resin varnish, for example, when using a resin composition or resin varnish containing 30 mass% to 60 mass% of an organic solvent, the resin composition layer can be formed by drying at 50°C to 150°C for 3 to 10 minutes.

[0179] The resin sheet may include any layer other than the support and the resin composition layer, if necessary. For example, in the resin sheet, a protective film equivalent to the support may be provided on the side of the resin composition layer that is not bonded to the support (i.e., the side opposite to the support). The thickness of the protective film is, for example, 1 μm to 40 μm. The protective film can prevent the adhesion of dust, etc., or scratches on the surface of the resin composition layer. When the resin sheet has a protective film, the resin sheet becomes usable by peeling off the protective film. In addition, the resin sheet can be stored by winding it into a roll shape.

[0180] A resin sheet can be suitably used to form an insulating layer in the manufacture of a semiconductor chip package (a resin sheet for insulating a semiconductor chip package). For example, the resin sheet can be used to form an insulating layer of a circuit board (a resin sheet for insulating a circuit board). Examples of packages using such a substrate include FC-CSP, MIS-BGA packages, and ETS-BGA packages.

[0181] In addition, the resin sheet can be suitably used to seal semiconductor chips (resin sheet for semiconductor chip sealing). Examples of applicable semiconductor chip packages include, for instance, fan-out type WLP, fan-in type WLP, fan-out type PLP, fan-in type PLP, etc.

[0182] In addition, the resin sheet may be used as a material for the MUF used after connecting the semiconductor chip to the substrate.

[0183] In addition, resin sheets can be used in a wide range of other applications requiring high insulation reliability. For example, resin sheets can be suitably used to form an insulating layer on circuit boards, such as printed circuit boards.

[0184] Circuit board

[0185] The circuit board of the present invention comprises an insulating layer formed by a cured product of the resin composition of the present invention. The circuit board can be manufactured, for example, by a manufacturing method comprising the following process (1) and process (2).

[0186] (1) A process of forming a resin composition layer on a substrate.

[0187] (2) A process of forming an insulating layer by heat-curing a resin composition layer.

[0188] In process (1), a substrate is prepared. Examples of substrates include glass epoxy substrates, metal substrates (stainless steel or cold-rolled steel sheets (SPCC), etc.), polyester substrates, polyimide substrates, BT resin substrates, thermosetting polyphenylene ether substrates, etc. Additionally, the substrate may have a metal layer, such as a copper foil, on its surface as part of the above substrate. For example, a substrate having a peelable first metal layer and a second metal layer on both surfaces may be used. When such a substrate is used, a conductor layer, which functions as a wiring layer capable of functioning as a circuit wiring, is typically formed on the surface of the second metal layer opposite to the first metal layer. Examples of substrates having such a metal layer include the carrier copper foil attached ultra-thin copper foil "Micro Thin" manufactured by Mitsui Kinzoku Kogyo Co., Ltd.

[0189] In addition, a conductive layer may be formed on one or both surfaces of the substrate. In the following description, a member comprising the substrate and the conductive layer formed on the surface of the substrate may appropriately be referred to as a "substrate with a wiring layer attached." As a conductive material included in the conductive layer, for example, a material comprising 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 may be used. As a conductive material, a single metal may be used or an alloy may be used. As an alloy, for example, an alloy of two or more metals selected from the above group (for example, nickel-chromium alloy, copper-nickel alloy, and copper-titanium alloy) may be used. Among these, chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, or copper as single metals, from the perspective of the versatility of forming the conductive layer, cost, and ease of patterning; As an alloy, nickel-chromium alloy, copper-nickel alloy, and copper-titanium alloy are preferred. Among these, chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, or copper are preferred; and nickel-chromium alloy is more preferred, and copper is particularly preferred.

[0190] The conductor layer may be patterned, for example, to function as 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㎛ or less (i.e., pitch is 40㎛ or less), more preferably 10 / 10㎛ or less, even more preferably 5 / 5㎛ or less, even more preferably 1 / 1㎛ or less, and particularly preferably 0.5 / 0.5㎛ or more. The pitch does not need to be uniform throughout the entire conductor layer. The minimum pitch of the conductor layer may be, for example, 40㎛ or less, 36㎛ or less, or 30㎛ or less.

[0191] 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.

[0192] A conductive layer can be formed by a method comprising, for example, a process of laminating a dry film (photosensitive resist film) onto a substrate; a process of obtaining a patterned dry film by forming a pattern through exposure and development of the dry film under predetermined conditions using a photomask; a process of forming a conductive layer by a plating method, such as electroplating, using the developed patterned dry film as a plating mask; and a process of peeling off the patterned dry film. As the dry film, a photosensitive dry film composed of a photoresist composition may be used, and for example, a dry film formed from a resin such as novolak resin or acrylic resin may be used. The lamination conditions of the substrate and the dry film may be the same as the lamination conditions of the substrate and the resin sheet described later. The peeling of the dry film may be carried out using an alkaline peeling solution, such as a sodium hydroxide solution.

[0193] After preparing the substrate, a resin composition layer is formed on the substrate. If a conductive layer is formed on the surface of the substrate, it is preferable to form the resin composition layer such that the conductive layer is embedded in the resin composition layer.

[0194] The formation of the resin composition layer is performed, for example, by laminating a resin sheet and a substrate. This lamination can be performed, for example, by heat-pressing the resin sheet onto the substrate from the support side to bond the resin composition layer to the substrate. As for the member that heat-presses the resin sheet onto the substrate (hereinafter referred to as the "heat-pressing member"), examples include a heated metal plate (such as a SUS hard plate) or a metal roll (such as a SUS roll). Furthermore, rather than pressing the heat-pressing member directly onto the resin sheet, it is preferable to press by interposing an elastic material, such as heat-resistant rubber, so that the resin sheet sufficiently follows the surface irregularities of the substrate.

[0195] Lamination of the substrate and the resin sheet may be carried out, for example, by a vacuum lamination method. In the vacuum lamination method, the heat pressing temperature is preferably in the range of 60°C to 160°C, more preferably in the range of 80°C to 140°C. The heat pressing pressure is preferably in the range of 0.098 MPa to 1.77 MPa, more preferably in the range of 0.29 MPa to 1.47 MPa. The heat pressing time is preferably in the range of 20 seconds to 400 seconds, more preferably in the range of 30 seconds to 300 seconds. Lamination is preferably carried out under reduced pressure conditions with a pressure of 13 hPa or less.

[0196] After lamination, the laminated resin sheets may be smoothed by pressing a heat-pressing member from the support side under atmospheric pressure, for example. The pressing conditions for the smoothing treatment may be the same as the heat-pressing conditions for the lamination. Meanwhile, lamination and the smoothing treatment may be performed continuously using a vacuum laminator.

[0197] In addition, the resin composition layer may be formed, for example, by a compression molding method. The molding conditions may be the same as those for the method of forming the resin composition layer in the process of forming the sealing layer of a semiconductor chip package described later.

[0198] After forming a resin composition layer on a substrate, the resin composition layer is heat-cured to form an insulating layer. Although the heat-curing conditions of the resin composition layer vary depending on the type of resin composition, the curing temperature is typically 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).

[0199] Before heat-curing the resin composition layer, a preheating treatment may be performed on the resin composition layer by heating it at a temperature lower than the curing temperature. For example, prior to heat-curing the resin composition layer, the resin composition layer may be preheated for at least 5 minutes (preferably 5 minutes to 150 minutes, more preferably 15 minutes to 120 minutes) at a temperature typically 50°C or higher and less than 120°C (preferably 60°C or higher and 110°C or lower, more preferably 70°C or higher and 100°C or lower).

[0200] In accordance with the above, a circuit board having an insulating layer can be manufactured. Furthermore, the method for manufacturing the circuit board may additionally include any additional process.

[0201] For example, when a circuit board is manufactured using a resin sheet, the method for manufacturing the circuit board may include a process of peeling off a support of the resin sheet. The support may be peeled off before the thermal curing of the resin composition layer, or peeled off after the thermal curing of the resin composition layer.

[0202] The method for manufacturing a circuit board may include, for example, a process of polishing the surface of an insulating layer after forming the insulating layer. The polishing method is not particularly limited. For example, the surface of the insulating layer may be polished using a flat polishing plate.

[0203] The method for manufacturing a circuit board may include, for example, a process (3) for inter-layer connection of conductor layers, and, for example, a process for drilling in an insulating layer. This allows holes such as via holes and through holes to be formed in the insulating layer. Methods for forming via holes include, for example, laser irradiation, etching, and mechanical drilling. The dimensions and shape of the via holes may be appropriately determined according to the design of the circuit board. Additionally, the process (3) may perform inter-layer connection by polishing or grinding the insulating layer.

[0204] After forming the via hole, it is desirable to perform a process to remove the smear within the via hole. This process is sometimes referred to as a desmear process. For example, if the formation of a conductor layer on an insulating layer is performed by a plating process, a wet desmear treatment may be performed on the via hole. In addition, if the formation of a conductor layer on an insulating layer is performed by a sputtering process, a dry desmear process, such as a plasma treatment process, may be performed. Furthermore, a shaping treatment may be performed on the insulating layer through the desmear process.

[0205] In addition, before forming a conductor layer on the insulating layer, a tamping treatment may be performed on the insulating layer. Through such tamping treatment, the surface of the insulating layer, including the via hole, is typically tamped. As for the tamping treatment, either a dry or wet tamping treatment may be performed. Examples of dry tamping treatment include plasma treatment. In addition, examples of wet tamping treatment include a method of performing swelling treatment with a swelling liquid, tamping treatment with an oxidizing agent, and neutralization treatment with a neutralizing liquid in this order.

[0206] After forming via holes, a conductor layer may be formed on the insulating layer. By forming a conductor layer at the location where the via holes are formed, the newly formed conductor layer and the conductor layer on the surface of the substrate become conductive, thereby performing interlayer connection. Methods for forming the conductor layer include, for example, plating, sputtering, and deposition, among which plating is preferred. In a suitable embodiment, a conductor layer having a desired wiring pattern is formed by plating on the surface of the insulating layer using an appropriate method such as a semi-additive method or a full-additive method. Additionally, if the support in the resin sheet is a metal foil, a conductor layer having a desired wiring pattern can be formed by a subtractive method. The material of the conductor layer to be 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 types of materials.

[0207] Here, an example of an embodiment for forming a conductor layer on an insulating layer is described in detail. A plating seed layer is formed on the surface of the insulating layer by electroless plating. Afterward, a mask pattern is formed on the formed plating seed layer to expose a portion of the plating seed layer corresponding to a desired wiring pattern. After forming an electroplated layer by electroplating on the exposed plating seed layer, the mask pattern is removed. Subsequently, the unnecessary plating seed layer is removed by a process such as etching to form a conductor layer having a desired wiring pattern. Meanwhile, when forming the conductor layer, the dry film used for forming the mask pattern is the same as the dry film above.

[0208] The method for manufacturing a circuit board may include a process (4) for removing a substrate. By removing the substrate, a circuit board having an insulating layer and a conductor layer embedded in the insulating layer can be obtained. The process (4) can be performed, for example, when a substrate having a peelable metal layer is used.

[0209] Semiconductor Chip Package

[0210] A semiconductor chip package according to a first embodiment of the present invention includes the circuit board described above and a semiconductor chip mounted on the circuit board. This semiconductor chip package can be manufactured by bonding the semiconductor chip to the circuit board.

[0211] The bonding conditions between the circuit board and the semiconductor chip may adopt any condition that allows the terminal electrodes of the semiconductor chip and the circuit wiring of the circuit board to be conductively connected. For example, conditions used in flip-chip mounting of semiconductor chips may be adopted. Additionally, for example, an insulating adhesive may be interposed between the semiconductor chip and the circuit board for bonding.

[0212] An example of a bonding method is a method of pressing a semiconductor chip onto a circuit board. As for the pressing conditions, the pressing temperature is 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 the pressing time is typically in the range of 1 second to 60 seconds (preferably in the range of 5 seconds to 30 seconds).

[0213] In addition, another example of a bonding method is a method of bonding a semiconductor chip to a circuit board by reflowing it. The reflow conditions may be in the range of 120°C to 300°C.

[0214] After bonding the semiconductor chip to the circuit board, the semiconductor chip may be filled with a mold underfill material. As the mold underfill material, the resin composition described above may be used, and the resin sheet described above may also be used.

[0215] A semiconductor chip package according to a second embodiment of the present invention comprises a semiconductor chip and a cured product of the resin composition that seals the semiconductor chip. In such a semiconductor chip package, the cured product of the resin composition typically functions as a sealing layer. An example of a semiconductor chip package according to the second embodiment is a fan-out type WLP.

[0216] The method for manufacturing such a semiconductor chip package is,

[0217] (A) A process of laminating a fixed film onto a substrate,

[0218] (B) A process of temporarily fixing a semiconductor chip onto a temporary fixing film,

[0219] (C) A process of forming a sealing layer on a semiconductor chip,

[0220] (D) A process for peeling off the substrate and the fixed film from the semiconductor chip,

[0221] (E) A process of forming a redistribution forming layer as an insulating layer on the surface of the semiconductor chip from which the substrate and temporary fixing film have been peeled off,

[0222] (F) A process of forming a redistribution layer as a conductor layer on a redistribution forming layer, and

[0223] (G) Includes a process of forming a solder resist layer on the redistribution layer.

[0224] In addition, the method for manufacturing the above semiconductor chip package is,

[0225] (H) The process may include dicing multiple semiconductor chip packages into individual semiconductor chip packages and reorganizing them.

[0226] (Process (A))

[0227] Process (A) is a process of laminating a temporary fixing film onto a substrate. The lamination conditions of the substrate and the temporary fixing film may be the same as the lamination conditions of the substrate and the resin sheet in the method of manufacturing a circuit board.

[0228] Examples of substrates include, for instance, 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 and heat-cured; and substrates made of bismaleimide triazine resins such as BT resin.

[0229] Any material that can be peeled off from the semiconductor chip and can also temporarily fix the semiconductor chip can be used as the temporary fixing film. Examples of commercially available products include "Reva Alpha" manufactured by Nitto Denko Co., Ltd.

[0230] (Process (B))

[0231] Process (B) is a process of temporarily fixing a semiconductor chip onto a temporary fixing film. The temporary fixing of the semiconductor chip can be performed using a device such as a flip-chip bonder or a die bonder, for example. The layout and number of semiconductor chips can be appropriately set according to the shape and size of the temporary fixing film and the production of the intended semiconductor chip package. For example, the semiconductor chips may be temporarily fixed by aligning them in a matrix shape of multiple rows and multiple columns.

[0232] (Process (C))

[0233] Process (C) is a process of forming a sealing layer on a semiconductor chip. The sealing layer is formed by a cured product of the resin composition described above. The sealing layer is typically formed by a method comprising a process of forming a resin composition layer on a semiconductor chip and a process of heat-curing the resin composition layer to form a sealing layer.

[0234] It is preferable to form the resin composition layer by compression molding. In compression molding, a semiconductor chip and a resin composition are typically placed in a mold, and pressure and, if necessary, heat are applied to the resin composition within the mold to form a resin composition layer covering the semiconductor chip.

[0235] The specific operation of the compression molding method may be performed as follows, for example. An upper mold and a lower mold are prepared as compression molding dies. Additionally, a resin composition is applied to a semiconductor chip that has been temporarily fixed on a temporary fixing film as described above. The semiconductor chip coated with the resin composition is attached to the lower mold together with the substrate and the temporary fixing film. Subsequently, the upper and lower molds are joined together, and heat and pressure are applied to the resin composition to perform compression molding.

[0236] In addition, the specific operation of the compression molding method may be performed as follows, for example. An upper mold and a lower mold are prepared as compression molding molds. A resin composition is placed on the lower mold. Additionally, a semiconductor chip is attached to the upper mold along with a substrate and a temporary fixing film. Then, the upper and lower molds are joined so that the resin composition placed on the lower mold comes into contact with the semiconductor chip attached to the upper mold, and compression molding is performed by applying heat and pressure.

[0237] Molding conditions vary depending on the composition of the resin composition, and appropriate conditions may be adopted to achieve good sealing. For example, the temperature of the mold during molding is preferably 70°C or higher, more preferably 80°C or higher, particularly preferably 90°C or higher, preferably 200°C or lower, more preferably 170°C or lower, and particularly preferably 150°C or lower. In addition, the pressure applied during molding is preferably 1 MPa or higher, more preferably 3 MPa or higher, and particularly preferably 5 MPa or higher, preferably 50 MPa or lower, more preferably 30 MPa or lower, and particularly preferably 20 MPa or lower. The curing time is preferably 1 minute or more, more preferably 2 minutes or more, and particularly preferably 3 minutes or more, preferably 60 minutes or less, more preferably 30 minutes or less, and particularly preferably 20 minutes or less. Typically, after the formation of the resin composition layer, the mold is removed. The removal of the mold may be performed before or after the thermal curing of the resin composition layer.

[0238] The formation of the resin composition layer may be performed by laminating a resin sheet and a semiconductor chip. For example, a resin composition layer can be formed on a semiconductor chip by heat-pressing the resin composition layer of the resin sheet and the semiconductor chip. The lamination of the resin sheet and the semiconductor chip can typically be performed by using a semiconductor chip instead of a substrate, in the same manner as the lamination of a resin sheet and a substrate in a method for manufacturing a circuit board.

[0239] After forming a resin composition layer on a semiconductor chip, the resin composition layer is heat-cured to obtain a sealing layer covering the semiconductor chip. In this way, the semiconductor chip is sealed by the cured resin composition. The heat-curing conditions of the resin composition layer may be the same as those for the heat-curing conditions of the resin composition layer in the method for manufacturing a circuit board. Additionally, before heat-curing the resin composition layer, a preheating treatment may be performed on the resin composition layer by heating it at a temperature lower than the curing temperature. The conditions for this preheating treatment may be the same as those for the preheating treatment in the method for manufacturing a circuit board.

[0240] ( Process (D))

[0241] Process (D) is a process for peeling off a substrate and a temporary fixing film from a semiconductor chip. It is preferable to employ a peeling method suitable for the material of the temporary fixing film. As a peeling method, for example, a method of peeling off by heating, foaming, or expanding the temporary fixing film may be cited. In addition, as a peeling method, for example, a method of peeling off by irradiating ultraviolet light onto the temporary fixing film through the substrate and reducing the adhesive strength of the temporary fixing film may be cited.

[0242] In a method for peeling off a temporary fixing film by heating, foaming, or expanding it, the heating conditions are typically 100°C to 250°C for 1 second to 90 seconds or 5 minutes to 15 minutes. In addition, in a method for peeling off a temporary fixing film by reducing its adhesive strength by irradiating it with ultraviolet rays, the amount of ultraviolet irradiation is typically 10 mJ / ㎠ to 1,000 mJ / ㎠.

[0243] (Process (E))

[0244] Process (E) is a process of forming a redistribution forming layer as an insulating layer on the surface where the substrate and the temporary fixing film of the semiconductor chip have been peeled off.

[0245] Any material having insulating properties may be used as the material for the redistribution forming layer. Among these, photosensitive resins and thermosetting resins are preferred from the perspective of ease of manufacturing the semiconductor chip package. In addition, the resin composition of the present invention may be used as such a thermosetting resin.

[0246] After forming the redistribution forming layer, via holes may be formed in the redistribution forming layer to interlayer connect the semiconductor chip and the redistribution layer.

[0247] In a method for forming via holes when the material of the redistribution forming layer is a photosensitive resin, typically, an active energy line is irradiated onto the surface of the redistribution forming layer through a mask pattern to photocur the redistribution forming layer in the irradiated portion. Examples of active energy lines include ultraviolet rays, visible light, electron beams, X-rays, etc., and ultraviolet rays are particularly preferred. The amount and duration of ultraviolet irradiation can be appropriately set according to the photosensitive resin. Examples of exposure methods include a contact exposure method in which a mask pattern is placed in close contact with the redistribution forming layer for exposure, and a non-contact exposure method in which a parallel light beam is used for exposure without placing a mask pattern in close contact with the redistribution forming layer.

[0248] After photocuring the redistribution forming layer, the redistribution forming layer is developed, and unexposed areas are removed to form via holes. Development may be performed using either wet development or dry development. Examples of development methods include the dip method, paddle method, spray method, brushing method, and scraping method, and the paddle method is suitable from the perspective of resolution.

[0249] When the material of the redistribution forming layer is a thermosetting resin, methods for forming via holes include, for example, laser irradiation, etching, and mechanical drilling. Among these, laser irradiation is preferred. Laser irradiation can be performed using a suitable laser processing machine that uses a light source such as a carbon dioxide laser, a UV-YAG laser, or an excimer laser.

[0250] The shape of the via hole is not particularly limited, but is generally circular (approximately circular). The top diameter of the via hole is preferably 50 μm or less, more preferably 30 μm or less, and even more preferably 20 μm or less. Here, the top diameter of the via hole refers to the diameter of the opening of the via hole on the surface of the redistribution forming layer.

[0251] (Process (F))

[0252] Process (F) is a process of forming a redistribution layer as a conductor layer on a redistribution forming layer. The method of forming the redistribution layer on the redistribution forming layer may be the same as the method of forming a conductor layer on an insulating layer in a method of manufacturing a circuit board. In addition, processes (E) and (F) may be repeated, and the redistribution layer and the redistribution forming layer may be built up alternately.

[0253] (Process (G))

[0254] Process (G) is a process of forming a solder resist layer on a redistribution layer. Any material having insulating properties may be used as the material of the solder resist layer. Among these, photosensitive resins and thermosetting resins are preferred from the perspective of ease of manufacturing a semiconductor chip package. In addition, the resin composition of the present invention may be used as the thermosetting resin.

[0255] In addition, in process (G), bumping processing to form bumps may be performed as needed. Bumping processing can be performed by methods such as solder balls or solder plating. In addition, the formation of via holes in the bumping process can be performed in the same way as in process (E).

[0256] ( Process (H))

[0257] The method for manufacturing a semiconductor chip package may include a process (H) in addition to processes (A) to (G). Process (H) is a process of dicing a plurality of semiconductor chip packages into individual semiconductor chip packages to form a single semiconductor chip package. The method of dicing the semiconductor chip packages into individual semiconductor chip packages is not particularly limited.

[0258] Semiconductor Device

[0259] A semiconductor device is provided with a semiconductor chip package. Examples of semiconductor devices include various semiconductor devices provided for electrical products (e.g., computers, mobile phones, smartphones, tablet devices, wearable devices, digital cameras, medical devices, and televisions, etc.) and vehicles (e.g., motorcycles, automobiles, electric trains, ships, and aircraft, etc.).

[0260] [Example]

[0261] The present invention will be explained in detail below through examples. The present invention is not limited to these examples. Furthermore, in the following, "parts" and "%" indicating amounts refer to "parts by mass" and "% by mass," respectively, unless otherwise specified.

[0262] <Example 1>

[0263] A resin composition was prepared by uniformly dispersing 0.5 parts of an amine curing agent ("SEIKACURE-S" manufactured by Seika Co., 7 parts of a glycidylamine-type epoxy resin ("630" manufactured by Mitsubishi Chemical Co., epoxy equivalent of about 95 g / eq.), 8 parts of a naphthalene-type epoxy resin ("HP-4032D" manufactured by DIC Co., epoxy equivalent of about 143 g / eq.), 0.1 parts of an imidazole-based curing accelerator ("2E4-MZ" manufactured by Shikoku Kasei Kogyo Co., 2 parts of polyoxyethylene polyoxypropylene glycol ("L-44" manufactured by ADEKA Co.), and 70 parts of an inorganic filler (spherical silica treated with KBM573 (N-phenyl-3-aminopropyltrimethoxysilane, manufactured by Shin-Etsu Kagaku Kogyo Co., 3.6 m² / g, average particle diameter 1.8 μm, specific surface area 3.6 m² / g) using a mixer.

[0264] <Example 2>

[0265] A resin composition was prepared in the same manner as in Example 1, except that 2 parts of polyoxyethylene polyoxypropylene glycol (L-64 manufactured by ADEKA) were used instead of 2 parts of polyoxyethylene polyoxypropylene glycol (L-44 manufactured by ADEKA).

[0266] <Example 3>

[0267] A resin composition was prepared in the same manner as in Example 1, except that 4 parts of polyoxyethylene polyoxypropylene glycol (L-64 manufactured by ADEKA) were used instead of 2 parts of polyoxyethylene polyoxypropylene glycol (L-44 manufactured by ADEKA).

[0268] <Example 4>

[0269] 7 parts of acid anhydride curing agent (Shin-Nippon Ricca "MH-700", acid anhydride equivalent 163 g / eq.), 5 parts of glycidylamine-type epoxy resin (Mitsubishi Chemical "630", epoxy equivalent approx. 95 g / eq.), 6 parts of naphthalene-type epoxy resin (DIC "HP-4032D", epoxy equivalent approx. 143 g / eq.), 0.1 parts of imidazole-based curing accelerator (Shikoku Kasei Kogyo "2MA-OK-PW"), 3 parts of polyoxyalkylene-modified silicone (Shin-Etsu Kagaku Kogyo "KF-6028"), inorganic filler (average particle diameter 1.8 µm, specific surface area 3.6 m² / g, KBM573 (N-phenyl-3-aminopropyltrimethoxysilane, Shin-Etsu Kagaku Kogyo Co. A resin composition was prepared by uniformly dispersing 85 parts of spherical silica treated with a mixer.

[0270] <Example 5>

[0271] A resin composition was prepared in the same manner as in Example 4, except that three parts of polyoxyalkylene modified silicone (Shin-Etsu Kagaku Kogyo Co., Ltd. “KF-6015”) were used instead of three parts of polyoxyalkylene modified silicone (Shin-Etsu Kagaku Kogyo Co., Ltd. “KF-6028”).

[0272] <Example 6>

[0273] A resin composition was prepared in the same manner as in Example 4, except that one part of polyoxyalkylene modified silicone ("KF-6015" manufactured by Shin-Etsu Kagaku Kogyo Co., Ltd.) was used instead of three parts of polyoxyalkylene modified silicone ("KF-6028" manufactured by Shin-Etsu Kagaku Kogyo Co., Ltd.).

[0274] <Comparative Example 1>

[0275] A resin composition was prepared in the same manner as in Example 1, except that polyoxyethylene polyoxypropylene glycol ("L-44" manufactured by ADEKA) was not used.

[0276] <Comparative Example 2>

[0277] A resin composition was prepared in the same manner as in Example 1, except that the amount of polyoxyethylene polyoxypropylene glycol ("L-44" manufactured by ADEKA) was changed from 2 parts to 7 parts.

[0278] <Comparative Example 3>

[0279] A resin composition was prepared in the same manner as in Example 4, except that polyoxyalkylene modified silicone (Shin-Etsu Kagaku Kogyo Co., Ltd. “KF-6028”) was not used.

[0280] <Comparative Example 4>

[0281] A resin composition was prepared in the same manner as in Example 4, except that the amount of polyoxyalkylene modified silicone (Shin-Etsu Kagaku Kogyo Co., Ltd. “KF-6028”) used was changed from 3 parts to 8 parts.

[0282] <Comparative Example 5>

[0283] A resin composition was prepared in the same manner as Comparative Example 4, except that 8 parts of the polyoxyalkylene modified silicone (Shin-Etsu Kagaku Kogyo Co., Ltd. “KF-6028”) of Comparative Example 4 were replaced with 8 parts of an amphiphilic polyether block copolymer (Dow Chemical Co., Ltd. “Fortegra 100”, a polyether compound containing a polybutylene oxide block).

[0284] <Test Example 1: Evaluation of Flexure>

[0285] On a 12-inch silicon wafer, the resin composition prepared in the examples and comparative examples was compression molded using a compression mold device (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 min) to form a resin composition layer with a thickness of 300 μm. Subsequently, the resin composition layer was heat-cured by heating at 180°C for 90 minutes. Thus, a sample substrate comprising a silicon wafer and a cured layer of the resin composition was obtained. The amount of warping at 25°C was measured for the sample substrate using a shadow moiré measuring device ("ThermoireAXP" manufactured by Akorometrix). The measurement was performed in accordance with JEITA EDX-7311-24, a standard of the Electronic and Information Technology Industries Association. Specifically, a virtual plane calculated by the least squares method of the entire data of the substrate surface of the measurement area was set as the reference plane, and the difference between the minimum and maximum values ​​in the vertical direction from the reference plane was calculated as the amount of warping and evaluated according to the following criteria.

[0286] "○": Bending amount less than 3mm

[0287] 「×」: Bending amount is 3mm or more

[0288] <Test Example 2: Measurement of Elastic Modulus (GPa)>

[0289] On a SUS plate with a release treatment applied to its surface, the resin composition prepared in the examples and comparative examples was compression molded using a compression mold 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 SUS plate was peeled off, and the resin composition layer was heat-cured by heating at 180°C for 90 minutes to obtain a cured layer of the resin composition. This cured layer was cut into a dumbbell shape (No. 1) to obtain a test specimen. The tensile strength of the test specimen was measured using an Orientec tensile testing machine "RTC-1250A," and the elastic modulus (GPa) at 25°C was determined. The measurement was performed in accordance with JIS K7127. This operation was performed three times, and the average value is shown in the table.

[0290] <Test Example 3: Evaluation of 3-Point Bending Strength>

[0291] The resin composition prepared in the examples and comparative examples was compression molded using a release-treated SUS plate-shaped compression mold device (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 min) to form a resin composition layer with a thickness of 300 μm. Afterward, the resin composition was peeled off from the SUS plate and heat-cured under conditions of 150°C for 60 minutes to obtain a test specimen for measuring three-point bending strength. The three-point bending strength (MPa) at 23°C was determined using the tensile testing machine "RTC-1250A" manufactured by Orientec Co., Ltd. The test was performed five times, and the average value was used. A three-point bending strength of 50 MPa or less was marked as "×", and a value greater than 50 MPa was marked as "○".

[0292] <Test Example 4: Measurement of Gel Time (Gelization Time) (Sec)>

[0293] For the resin compositions prepared in the examples and comparative examples, the gel time (gelation time) was measured in accordance with JIS C6521. Specifically, first, the time (in seconds) at which the resin compositions of the examples and comparative examples could not be pulled at 130°C was measured using a hot plate gelation tester (GT-D: manufactured by Nissin Kagaku Co., Ltd.). More specifically, about 0.5g of the sample (resin composition) was placed on the hot plate gelation tester. Taking the point at which the temperature reached 130°C (130°C gel time) as the starting point, contact circular motion was repeated with a spatula with a tip width of 5mm over the resin composition so that the resin composition entered within a diameter range of 25mm on the hot plate (1 rotation per second). The resin composition was lifted vertically 30 mm from the hot plate, and the point at which the thread-like structure broke was set as the endpoint. The time from the starting point to the endpoint was considered as the time until gelation, and measurements were taken. Additionally, the spatula was not lifted while the viscosity of the resin was low, and when the viscosity increased, it was lifted vertically about 30 mm from the hot plate from time to time, and this up-and-down motion was repeated until the thread-like structure broke. The measurement was repeated twice, and the average value was used as the result.

[0294] <Test Example 5: Evaluation of Minimum Melt Viscosity>

[0295] The melt viscosity of the resin compositions prepared in the examples and comparative examples was measured using a dynamic viscoelasticity measuring device ("Rheosol-G3000" manufactured by UBM). This measurement was performed on a 1g sample taken from the resin composition using a flat plate with a diameter of 18mm. The measurement conditions were set as follows: starting temperature from 60℃ to 200℃, heating rate of 5℃ / min, measurement temperature interval of 2.5℃, and vibration of 1Hz / deg. The minimum melt viscosity was determined from the measured values ​​of the obtained melt viscosity. A minimum melt viscosity of 10 poise or less was designated as "○", a minimum melt viscosity greater than 10 poise and 100 poise or less as "△", and a minimum melt viscosity greater than 100 poise as "×".

[0296] The non-volatile components of the resin compositions of the examples and comparative examples and the amount used thereof, as well as the measurement and evaluation results of the test examples, are shown in Table 1 below.

[0297]

[0298] From the above results, it was found that when the resin composition used comprises (A) an epoxy resin, (B) an inorganic filler, (C) a curing agent, and (D) a non-epoxy compound containing a polyether backbone, the polyether backbone included in component (D) is a polyoxyalkylene backbone composed of one or more monomer units selected from ethylene oxide units and propylene oxide units, the content of (B) the inorganic filler is 70 mass% or more when all non-volatile components in the resin composition are 100 mass%, and the content of (D) the non-epoxy compound containing a polyether backbone is 1 mass% or more and 30 mass% or less when non-volatile components other than (B) the inorganic filler in the resin composition are 100 mass%, it is possible to obtain a cured product having excellent embeddability, suppressing warping during curing, and excellent mechanical strength.

Claims

Claim 1 A resin composition comprising (A) an epoxy resin, (B) an inorganic filler, (C) a curing agent, and (D) a non-epoxy compound containing a polyether backbone, wherein the polyether backbone included in component (D) is a polyoxyalkylene backbone composed of one or more monomer units selected from ethylene oxide units and propylene oxide units, (B) is 70 mass% or more when all nonvolatile components in the resin composition are 100 mass%, (D) is one or more compounds selected from the group consisting of polyalkylene glycol and polyoxyalkylene modified silicone, and the polyalkylene glycol is polyoxyethylenepolyoxypropylene glycol, and (D) is 1 mass% or more and 30 mass% or less when all nonvolatile components other than component (B) in the resin composition are 100 mass%. Claim 2 A resin composition according to claim 1, wherein (D) the number average molecular weight of the component is 500 to 10,000. Claim 3 A resin composition according to claim 1, wherein the viscosity of component (D) at 25°C is 3,000 mPa·s or less. Claim 4 A resin composition according to claim 1, wherein the content of component (B) is 78 mass% or more when all non-volatile components in the resin composition are 100 mass%. Claim 5 A resin composition according to claim 1, wherein (B) the component is silica. Claim 6 A resin composition according to claim 1, wherein (A) a component comprises a condensed ring structure-containing epoxy resin. Claim 7 A resin composition according to claim 6, wherein the content of the condensed ring structure-containing epoxy resin in component (A) is 50 mass% or more when the total amount of component (A) is 100 mass%. Claim 8 A resin composition according to claim 1, wherein (A) the component comprises a glycidylamine-type epoxy resin. Claim 9 A resin composition according to claim 1, wherein (A) a component comprises a liquid epoxy resin. Claim 10 A resin composition according to claim 9, wherein the content of liquid epoxy resin in component (A) is 50 mass% or more when the total amount of component (A) is 100 mass%. Claim 11 A resin composition according to claim 1, wherein the content of component (A) is 40 mass% or more when the non-volatile component other than component (B) in the resin composition is 100 mass%. Claim 12 A resin composition according to claim 1, wherein component (C) comprises one or more curing agents selected from the group consisting of acid anhydride-based curing agents and amine-based curing agents. Claim 13 A resin composition for forming an insulating layer of a semiconductor chip package, according to claim 1. Claim 14 A resin composition for forming an insulating layer of a circuit board in claim 1. Claim 15 A resin composition for sealing a semiconductor chip of a semiconductor chip package, in accordance with claim 1. Claim 16 A cured product of a resin composition described in any one of claims 1 to 15. Claim 17 A resin sheet having a support and a resin composition layer comprising a resin composition described in any one of claims 1 to 15 provided on the support. Claim 18 A circuit board comprising an insulating layer formed by a cured product of a resin composition described in any one of claims 1 to 15. Claim 19 A semiconductor chip package comprising a circuit board described in claim 18 and a semiconductor chip mounted on said circuit board. Claim 20 A semiconductor device having a semiconductor chip package as described in paragraph 19. Claim 21 A semiconductor chip package comprising a semiconductor chip and a cured product of a resin composition described in any one of claims 1 to 15 for sealing the semiconductor chip. Claim 22 A semiconductor device having a semiconductor chip package as described in paragraph 20. Claim 23 delete Claim 24 delete

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