WO2023157542A1 - 樹脂組成物 - Google Patents

樹脂組成物 Download PDF

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Publication number
WO2023157542A1
WO2023157542A1 PCT/JP2023/001361 JP2023001361W WO2023157542A1 WO 2023157542 A1 WO2023157542 A1 WO 2023157542A1 JP 2023001361 W JP2023001361 W JP 2023001361W WO 2023157542 A1 WO2023157542 A1 WO 2023157542A1
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Prior art keywords
resin composition
resin
epoxy resin
axis
cured product
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English (en)
French (fr)
Japanese (ja)
Inventor
啓之 阪内
成 佐々木
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Ajinomoto Co Inc
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Ajinomoto Co Inc
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Priority to JP2024501034A priority Critical patent/JPWO2023157542A1/ja
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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
    • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
    • C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K9/00—Use of pretreated ingredients
    • C08K9/04—Ingredients treated with organic substances
    • C08K9/06—Ingredients treated with organic substances with silicon-containing compounds
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L63/00—Compositions of epoxy resins; Compositions of derivatives of epoxy resins
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10W—GENERIC PACKAGES, INTERCONNECTIONS, CONNECTORS OR OTHER CONSTRUCTIONAL DETAILS OF DEVICES COVERED BY CLASS H10
    • H10W72/00—Interconnections or connectors in packages
    • H10W72/071—Connecting or disconnecting

Definitions

  • the present invention relates to resin compositions. Furthermore, it relates to a resin sheet, a semiconductor chip package, and a semiconductor device containing the resin composition.
  • an insulating material that can be used as an insulating layer of a semiconductor chip package for example, one that is formed by curing a resin composition is known (see Patent Document 1, for example).
  • the elastic modulus of the cured product of the resin composition is increased, the flexibility of the cured product of the resin composition is impaired, and the amount of warpage of the cured product may increase.
  • the present invention was invented in view of the above problems, and it is possible to obtain a cured product in which the occurrence of cracks and delamination and the amount of warpage are suppressed even if the semiconductor chip package is enlarged.
  • a resin composition; a resin sheet using the resin composition; a semiconductor chip package; and a semiconductor device was invented in view of the above problems, and it is possible to obtain a cured product in which the occurrence of cracks and delamination and the amount of warpage are suppressed even if the semiconductor chip package is enlarged.
  • the present inventors created an SS curve showing the relationship between the bending strength and strain of the cured product of the resin composition, and the vertical line drawn from the maximum point of the bending strength to the X axis, and the vertical line
  • the epoxy resin and inorganic filler are added so that the toughness value indicated by the area of the triangle exceeds 30 MPa.
  • the present inventors have completed the present invention by discovering that the above problems can be solved by adjusting the amount of carbon per unit surface area of the inorganic filler to a predetermined value or more.
  • the present invention includes the following contents.
  • a resin composition containing (A) an epoxy resin and (B) an inorganic filler The strain (%) of the cured product obtained by thermally curing the resin composition at 150 ° C. for 60 minutes is on the X axis, and the bending strength (MPa) of the cured product by thermally curing the resin composition at 150 ° C. for 60 minutes is on the Y axis.
  • An SS curve was created, and a vertical line extending from the maximum bending strength point to the X-axis, and a triangle having two straight sides from the intersection of the vertical line with the X-axis to the intersection of the X-axis and the Y-axis were created.
  • the toughness value indicated by the area of the triangle ((maximum bending strength (MPa) ⁇ strain (%) at maximum bending strength) / 2) exceeds 30 MPa
  • component (C) contains one or more selected from an amine curing agent, a cyanate ester curing agent, and an acid anhydride curing agent.
  • component (C) contains one or more selected from an amine curing agent, a cyanate ester curing agent, and an acid anhydride curing agent.
  • the resin composition according to any one of [1] to [4] which is for a semiconductor device having a semiconductor chip package with an area of 100 mm 2 or more.
  • a resin sheet comprising a support and a resin composition layer provided on the support and formed of the resin composition according to any one of [1] to [6].
  • a semiconductor chip package comprising a cured product layer formed from the cured product of the resin composition according to any one of [1] to [6], and a semiconductor chip mounted on the cured product layer.
  • a semiconductor device including the semiconductor chip package according to [8].
  • a resin composition capable of obtaining a cured product in which the occurrence of cracks and delamination and the amount of warpage are suppressed even if the semiconductor chip package is enlarged; resin sheets; semiconductor chip packages; and semiconductor devices.
  • FIG. 1 is a graph showing an example of an SS curve for explaining toughness values.
  • the resin composition of the present invention is a resin composition containing (A) an epoxy resin and (B) an inorganic filler, and is a cured product obtained by heat curing the resin composition at 150 ° C. for 60 minutes ( %) as the X axis and the bending strength (MPa) of the cured product obtained by heat curing the resin composition at 150 ° C. for 60 minutes as the Y axis.
  • the area of the triangle ((maximum bending strength (MPa) x maximum bending strength
  • the toughness value represented by (strain (%) at)/2) exceeds 30 MPa
  • the amount of carbon per unit surface area of component (B) is 0.35 mg/m 2 or more.
  • the amount of carbon per unit area of component (B) is adjusted to a predetermined value or more, and the components (A) and (B) are adjusted so that the toughness value is within a predetermined range. It was found that by suppressing the application of excessive stress to the cured product of the resin composition, the occurrence of cracks and delamination was suppressed, and the amount of warpage was also suppressed. The toughness value and carbon amount will be described later.
  • the resin composition of the present invention comprises (A) an epoxy resin, and (B) an inorganic filler in combination with (C) a curing agent, (D) a curing accelerator, (E) a silane coupling agent, and (F) Other additives may be included.
  • A an epoxy resin
  • B an inorganic filler in combination with (C) a curing agent, (D) a curing accelerator, (E) a silane coupling agent, and (F) Other additives may be included.
  • the resin composition contains (A) an epoxy resin as the (A) component.
  • Epoxy resins include, for example, 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, and naphthol novolac type epoxy resin.
  • 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 novolac type epoxy resin , biphenyl type epoxy resin, linear aliphatic epoxy resin, epoxy resin having butadiene structure, alicyclic epoxy resin, heterocyclic epoxy resin, spiro ring-containing epoxy resin, cyclohexanedimethanol type epoxy resin, naphthylene ether type epoxy Examples thereof include resins and trimethylol-type epoxy resins.
  • An epoxy resin may be used individually by 1 type, and may be used in combination of 2 or more type.
  • the epoxy resin preferably contains an epoxy resin having two or more epoxy groups in one molecule.
  • the ratio of the epoxy resin having two or more epoxy groups in one molecule to 100% by mass of the non-volatile components of the epoxy resin is preferably 50% by mass or more. More preferably 60% by mass or more, particularly preferably 70% by mass or more.
  • Epoxy resins are classified into liquid epoxy resins at a temperature of 20°C (hereinafter referred to as “liquid epoxy resins”) and solid epoxy resins at a temperature of 20°C (hereinafter referred to as “solid epoxy resins").
  • the resin composition may contain only a liquid epoxy resin, may contain only a solid epoxy resin, or may contain a combination of a liquid epoxy resin and a solid epoxy resin. , from the viewpoint of significantly obtaining the effects of the present invention, it is preferable that only the liquid epoxy resin is included.
  • the liquid epoxy resin preferably contains a liquid epoxy resin having two or more epoxy groups in one molecule, more preferably a liquid epoxy resin having three or more epoxy groups in one molecule. More preferably, it contains a liquid epoxy resin having 4 or more epoxy groups in the molecule.
  • liquid epoxy resins examples include bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol AF type epoxy resin, naphthalene type epoxy resin, glycidyl ester type epoxy resin, glycidyl amine type epoxy resin, phenol novolac type epoxy resin, and an ester skeleton.
  • liquid epoxy resins include "HP4032", “HP4032D”, and “HP4032SS” (naphthalene-type epoxy resins) manufactured by DIC; 828EL” (bisphenol A type epoxy resin); Mitsubishi Chemical Corporation “jER807”, “1750” (bisphenol F type epoxy resin); Mitsubishi Chemical Corporation “jER152” (phenol novolac type epoxy resin); Mitsubishi Chemical Corporation “JER630", “JER630LSD” (glycidylamine type epoxy resin); Nippon Steel Chemical & Materials “ZX1059” (mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin); Nagase ChemteX Co., Ltd.
  • EX-721 (glycidyl ester type epoxy resin); "Celoxide 2021P” manufactured by Daicel (alicyclic epoxy resin having an ester skeleton); "PB-3600” manufactured by Daicel (epoxy resin having a butadiene structure) Nippon Steel Chemical & Materials "ZX1658", “ZX1658GS” (liquid 1,4-glycidylcyclohexane type epoxy resin); Showa Denko “PETG”, “BATG” (polyvalent glycidyl compound); Sumitomo Chemical "ELM-434VL” (glycidylamine-type epoxy resin) manufactured by Co., Ltd., and the like. These may be used individually by 1 type, and may be used in combination of 2 or more type.
  • the solid epoxy resin is preferably a solid epoxy resin having 3 or more epoxy groups per molecule, more preferably an aromatic solid epoxy resin having 3 or more epoxy groups per molecule.
  • Solid epoxy resins include bixylenol-type epoxy resin, naphthalene-type epoxy resin, naphthalene-type tetrafunctional epoxy resin, novolac-type epoxy resin, cresol novolac-type epoxy resin, dicyclopentadiene-type epoxy resin, trisphenol-type epoxy resin, and naphthol. type epoxy resin, biphenyl type epoxy resin, naphthylene ether type epoxy resin, anthracene type epoxy resin, bisphenol A type epoxy resin, bisphenol AF type epoxy resin, tetraphenylethane type epoxy resin, and more preferably novolac type epoxy resin.
  • solid epoxy resins include “HP4032H” (naphthalene-type epoxy resin), “HP-4700”, “HP-4710” (naphthalene-type tetrafunctional epoxy resin), “N-690” ( cresol novolak type epoxy resin), “N-695" (cresol novolak type epoxy resin), “HP-7200”, “HP-7200HH”, “HP-7200H” (dicyclopentadiene type epoxy resin), "EXA-7311 ”, “EXA-7311-G3”, “EXA-7311-G4”, “EXA-7311-G4S”, “HP6000”, “HP6000L” (naphthylene ether type epoxy resin); “EPPN” manufactured by Nippon Kayaku Co., Ltd.
  • ESN475V naphthalene type epoxy resin
  • ESN485" naphthol novolak type epoxy resin
  • resin YX8800
  • anthracene-type epoxy resin 157S70
  • novolac-type epoxy resin PG-100” and "CG-500” manufactured by Osaka Gas Chemicals
  • YX7760 manufactured by Mitsubishi Chemical
  • YL7800 fluorene type epoxy resin
  • jER1010 solid bisphenol A type epoxy resin
  • jER1031S tetraphenylethane type epoxy resin
  • the mass ratio thereof (solid epoxy resin: liquid epoxy resin) is preferably 1:0.01 to 1:50, more preferably 1:0.05 to 1:20, particularly preferably 1:0.1 to 1:10.
  • the amount ratio of the liquid epoxy resin to the solid epoxy resin within this range, 1) when used in the form of a resin sheet, moderate adhesiveness is provided, and 2) when used in the form of a resin sheet. 3) a cured product having sufficient breaking strength can be obtained.
  • the epoxy equivalent of the epoxy resin is preferably 50 g/eq. ⁇ 5000g/eq. , more preferably 50 g/eq. ⁇ 3000g/eq. , more preferably 80 g/eq. ⁇ 2000g/eq. , even more preferably 110 g/eq. ⁇ 1000 g/eq. is. By setting it within this range, a cured product of a resin composition having a sufficient cross-linking density can be obtained.
  • Epoxy equivalent weight is the weight of an epoxy resin containing one equivalent of epoxy groups. This epoxy equivalent can be measured according to JIS K7236.
  • the weight average molecular weight (Mw) of the epoxy resin is preferably 100 to 5000, more preferably 250 to 3000, still more preferably 400 to 1500, from the viewpoint of significantly obtaining the desired effect of the present invention.
  • the weight average molecular weight of the epoxy resin is the polystyrene equivalent weight average molecular weight measured by gel permeation chromatography (GPC).
  • the content of the epoxy resin is preferably 1% by mass or more, more preferably 3%, when the non-volatile component in the resin composition is 100% by mass. It is at least 5% by mass, more preferably at least 5% by mass.
  • the upper limit of the epoxy resin content is preferably 20% by mass or less, more preferably 15% by mass or less, and even more preferably 10% by mass or less, from the viewpoint of significantly obtaining the desired effects of the present invention.
  • the content of each component in the resin composition is a value when the non-volatile component in the resin composition is 100% by mass, unless otherwise specified. It means all non-volatile components in the substance except the solvent.
  • the resin composition contains (B) an inorganic filler as the (B) component.
  • An inorganic compound is used as the material for the inorganic filler.
  • inorganic filler materials include silica, alumina, glass, cordierite, silicon oxide, barium sulfate, barium carbonate, talc, clay, mica powder, zinc oxide, hydrotalcite, boehmite, aluminum hydroxide, Magnesium hydroxide, calcium carbonate, magnesium carbonate, magnesium oxide, boron nitride, aluminum nitride, manganese nitride, aluminum borate, strontium carbonate, strontium titanate, calcium titanate, magnesium titanate, bismuth titanate, titanium oxide, zirconium oxide , barium titanate, barium zirconate titanate, barium zirconate, calcium zirconate, zirconium phosphate, and zirconium tungstate phosphate.
  • silica examples include amorphous silica, fused silica, crystalline silica, synthetic silica, and hollow silica. Moreover, as silica, spherical silica is preferable.
  • the inorganic filler may be used singly or in combination of two or more.
  • inorganic fillers include, for example, "ST7030-20” manufactured by Nippon Steel Chemical &Materials; “MSS-6” and “AC-5V” manufactured by Tatsumori; “ SP60-05”, “SP507-05”; Admatechs “YC100C”, “YA050C”, “YA050C-MJE”, “YA010C”; Denka “UFP-30”, “SFP-130MC”, “FB -7SDC”, “FB-5SDC”, “FB-3SDC”; Tokuyama “Silfil NSS-3N”, “Silfil NSS-4N”, “Silfil NSS-5N”; Admatechs "SC2500SQ", “SO -C4”, “SO-C2”, “SO-C1”, “FE9” and the like.
  • the particle size distribution of the inorganic filler can be measured by a laser diffraction/scattering method based on the Mie scattering theory. Specifically, the particle size distribution of the inorganic filler was created on a volume basis using a laser diffraction scattering particle size distribution measuring device, and 30% particle size (D30), 50% particle size (D50), and 65% particle size. The diameter (D65) can be measured.
  • a measurement sample can be obtained by weighing 100 mg of an inorganic filler and 10 g of methyl ethyl ketone in a vial and dispersing them with ultrasonic waves for 10 minutes.
  • a measurement sample is measured using a laser diffraction particle size distribution measuring device, the wavelengths of the light source used are blue and red, the volume-based particle size distribution of the inorganic filler is measured by the flow cell method, and from the obtained particle size distribution
  • the average particle size can be calculated as the median size.
  • the laser diffraction particle size distribution analyzer include "LA-960" manufactured by Horiba, Ltd., and the like.
  • the 30% particle size (D30) is the particle size when the cumulative amount of the volume accumulated from the smaller particle size side becomes 30% in the particle size distribution curve as a result of measuring the particle size distribution by the above method.
  • the 50% particle size (D50) is the particle size at which the cumulative volume accumulated from the smaller particle size side becomes 50% in the particle size distribution curve as a result of measuring the particle size distribution by the above method.
  • the 65% particle size (D65) is the particle size when the cumulative amount of volume accumulated from the smaller particle size side is 65% in the particle size distribution curve as a result of measuring the particle size distribution by the above method.
  • the average particle size of the inorganic filler means the particle size of the 50% particle size (D50).
  • the 50% particle size (D50) in the particle size distribution is preferably 0.3 ⁇ m or more, more preferably 1 ⁇ m or more, still more preferably 3 ⁇ m or more, and preferably 10 ⁇ m, from the viewpoint of significantly obtaining the desired effect of the present invention. Below, more preferably 8 ⁇ m or less, still more preferably 6 ⁇ m or less.
  • the 30% particle size (D30) in the particle size distribution is 0.1 ⁇ m or more, preferably 0.15 ⁇ m or more, more preferably 0.2 ⁇ m or more, from the viewpoint of significantly obtaining the desired effects of the present invention. .
  • the upper limit is 8 ⁇ m or less, preferably 6 ⁇ m or less, more preferably 4 ⁇ m or less.
  • the 65% particle size (D65) in the particle size distribution is 0.2 ⁇ m or more, preferably 0.3 ⁇ m or more, more preferably 0.4 ⁇ m or more, from the viewpoint of significantly obtaining the desired effects of the present invention.
  • the upper limit is 15 ⁇ m or less, preferably 13 ⁇ m or less, more preferably 11 ⁇ m or less.
  • the specific surface area of the inorganic filler (B) is preferably 1 m 2 /g or more, more preferably 2 m 2 /g or more, and particularly preferably 3 m 2 /g or more. Although there is no particular upper limit, it is preferably 60 m 2 /g or less, 50 m 2 /g or less, or 40 m 2 /g or less.
  • the specific surface area is obtained by adsorbing nitrogen gas on the sample surface using a specific surface area measuring device (Macsorb HM-1210 manufactured by Mountec) according to the BET method and calculating the specific surface area using the BET multipoint method. .
  • the inorganic filler is preferably treated with a surface treatment agent from the viewpoint of suppressing cracks and delamination and obtaining a cured product with a suppressed amount of warpage.
  • a surface treatment agent may be used alone, or two or more types may be used in combination. Examples of surface treatment agents include silane coupling agents and alkoxysilane compounds, and silane coupling agents are preferred.
  • a silane coupling agent is a silane compound that has a functional group that contributes to bonding with an inorganic filler and a functional group that contributes to bonding with an organic component such as an epoxy resin.
  • Examples of functional groups that contribute to bonding with inorganic fillers include hydroxy groups and alkoxy groups. These may be contained individually by 1 type, and may be contained in combination of 2 or more types. Among them, an alkoxy group is preferable from the viewpoint of significantly obtaining the effects of the present invention.
  • the alkoxy group may be linear, branched or cyclic.
  • the alkoxy group preferably has 1 to 10 carbon atoms, more preferably 1 to 6 carbon atoms, still more preferably 1 to 4 carbon atoms, and still more preferably 1 or 2 carbon atoms.
  • the silane coupling agent preferably has 1 to 3, more preferably 2 or 3 functional groups that contribute to bonding with the inorganic filler in one molecule.
  • Examples of functional groups that contribute to bonding with organic components include amino groups, epoxy groups, mercapto groups, (meth)acryl groups, vinyl groups, isocyanate groups, imidazolyl groups, ureido groups, sulfide groups, and isocyanurate groups. mentioned. These may be contained individually by 1 type, and may be contained in combination of 2 or more type. Among them, one or more selected from the group consisting of an amino group, an epoxy group, a mercapto group, a (meth)acrylic group, a vinyl group, an isocyanate group and an imidazolyl group is preferred from the viewpoint of significantly obtaining the effects of the present invention. and epoxy groups are more preferred.
  • the silane coupling agent preferably has 1 to 3, more preferably 1 or 2 functional groups that contribute to bonding with an organic component in one molecule.
  • the molecular weight of the silane coupling agent is preferably 100 or more, more preferably 120 or more, still more preferably 140 or more, 160 or more, 180 or more, or 200 or more, from the viewpoint of suppressing volatilization during surface treatment or drying.
  • the upper limit of the molecular weight is preferably 800 or less, more preferably 750 or less, more preferably 700 or less, 650 or less, 600 or less, 550 or less, 500 or less, 450 or less, or 400 or less from the viewpoint of appropriate reactivity. be.
  • the silane coupling agent is a silane compound represented by the following formula (1).
  • X is an amino group, an epoxy group, a mercapto group, a (meth)acrylic group, a vinyl group, an isocyanate group, an imidazolyl group, a ureido group, a sulfide group, and a monovalent containing a functional group selected from the group consisting of an isocyanurate group represents the group of R 1 represents a hydroxy group or an alkoxy group, R 2 represents a hydrogen atom, an alkyl group or an aryl group, m1 and m2 each represent an integer from 1 to 3 with the condition that the sum of m1 and m2 is 4 or less.
  • X's they may be the same or different; when there are a plurality of R 1 's
  • the number of carbon atoms in the monovalent group represented by X is preferably 20 or less, more preferably 14 or less, still more preferably 12 or less, 10 or less, 9 or less, 8 or less, 7 or less, or 6 or less.
  • the lower limit of the number of carbon atoms varies depending on the functional group included in the monovalent group represented by X, but is preferably 1 or more, more preferably 2 or more or 3 or more.
  • the monovalent group represented by X includes an amino group, an epoxy group, a mercapto group, a (meth)acrylic group, a vinyl group, an isocyanate group and an imidazolyl group.
  • a monovalent group containing one or more functional groups selected from the group consisting of is preferred, and a monovalent group containing one or more functional groups selected from an amino group and an epoxy group is more preferred.
  • the monovalent group represented by X include N-(aminoC 1-10 alkyl)-aminoC 1-10 alkyl group, N-(phenyl)-amino C 1-10 alkyl group, N- (C 1-10 alkylidene)-amino C 1-10 alkyl group, (epoxy C 3-10 cycloalkyl) C 1-10 alkyl group, glycidoxy C 1-10 alkyl group, glycidyl C 1-10 alkyl group, mercapto C 1-10 alkyl group, acryloxy C 1-10 alkyl group, methacryloxy C 1-10 alkyl group, vinyl group, styryl group, isocyanate C 1-10 alkyl group, imidazolyl C 1-10 alkyl group, ureido C 1- 10 alkyl group, tri(C 1-10 alkoxy)silyl C 1-10 alkyltetrasulfide C 1-10 alkyl group, and di[tri(C 1-10 alk
  • C p ⁇ q (where p and q are positive integers and satisfies p ⁇ q) means that the number of carbon atoms of the organic group described immediately after this term is from p to q.
  • C 1-6 alkyl denotes an alkyl group having 1 to 6 carbon atoms.
  • the alkoxy group represented by R 1 may be linear, branched or cyclic.
  • the alkoxy group preferably has 1 to 10 carbon atoms, more preferably 1 to 6 carbon atoms, still more preferably 1 to 4 carbon atoms, and still more preferably 1 or 2 carbon atoms.
  • R 1 is preferably an alkoxy group from the viewpoint of efficiently surface-treating the inorganic filler.
  • the alkyl group represented by R2 may be linear, branched or cyclic.
  • the number of carbon atoms in the alkyl group is preferably 1-10, more preferably 1-6, even more preferably 1-4.
  • the number of carbon atoms in the aryl group represented by R 2 is preferably 6-20, more preferably 6-14, still more preferably 6-10.
  • R 2 is preferably an alkyl group.
  • m1 and m2 each represent an integer of 1 to 3, provided that the sum of m1 and m2 is 4 or less.
  • m1 is preferably 1 or 2 and m2 is preferably 2 or 3.
  • silane coupling agents include N-phenyl-3-aminopropyltrimethoxysilane, N-(2-aminoethyl)-3-aminopropylmethyldimethoxysilane, N-(2-aminoethyl)-3 -aminopropyltrimethoxysilane, 3-aminopropyltrimethoxysilane, 3-triethoxysilyl-N-(1,3-dimethyl-butylidene)propylamine, 3-glycidoxypropylmethyldimethoxysilane, 3-glycidoxy Propyltrimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, 3-glycidoxypropyltriethoxysilane, 3-mercaptopropylmethyldimethoxysilane, 3-mercaptopropyltrimethoxysilane, 3-methacryloxypropylmethyldimethoxysilane , 3-methacryloxypropylmethyld
  • Commercially available surface treatment agents may be used. Commercially available surface treatment agents include, for example, Shin-Etsu Chemical Co., Ltd. "KBM1003” (vinyltriethoxysilane), Shin-Etsu Chemical Co., Ltd. "KBM503” (3-methacryloxypropyltriethoxysilane), Shin-Etsu Chemical Co., Ltd. "KBM403” (3-glycidoxypropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd. "KBM803” (3-mercaptopropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.
  • the amount of carbon per unit surface area of component (B) is 0.35 mg/m 2 or more, preferably 0.4 mg/m 2 or more , more preferably 0.41 mg, from the viewpoint of significantly obtaining the effects of the present invention. /m 2 or more, more preferably 0.42 mg/m 2 or more, preferably 1 mg/m 2 or less, more preferably 0.8 mg/m 2 or less, further preferably 0.5 mg/m 2 or less. be.
  • the amount of carbon per unit surface area refers to (B) the total amount of carbon atoms per unit surface area of the component bonded to the surface of the inorganic filler, and (B) the surface of the inorganic filler.
  • the concept of the components that are included also includes the case of components other than the surface treatment agent.
  • the amount of carbon per unit surface area of the inorganic filler is determined by dissolving the inorganic filler (inorganic filler after surface treatment if the inorganic filler is surface-treated with a surface treatment agent) with a solvent (e.g., methyl ethyl ketone (MEK)). It can be measured after washing. Specifically, a sufficient amount of MEK as a solvent is added to 30 g of the inorganic filler (inorganic filler surface-treated with a surface treatment agent when the inorganic filler is surface-treated with a surface treatment agent), and 25 Ultrasonic wash for 5 minutes at °C. Solid-liquid separation is performed by centrifugation, and the supernatant is removed.
  • a solvent e.g., methyl ethyl ketone (MEK)
  • the amount of carbon per unit surface area of the inorganic filler can be measured using a carbon analyzer.
  • a carbon analyzer As the carbon analyzer, "EMIA-321V2" and “EMIA-320V” manufactured by Horiba Ltd. can be used. The details of the measurement of the carbon content can be measured by the method described in Examples below.
  • the content of the inorganic filler is preferably 50% by mass or more, more preferably 60% by mass, when the nonvolatile component in the resin composition is 100% by mass. % or more, more preferably 70 mass % or more or 80 mass % or more.
  • the upper limit is preferably 95% by mass or less, more preferably 93% by mass or less, and even more preferably 90% by mass or less.
  • the resin composition may further contain (C) a curing agent as an optional component in combination with the components (A) to (B) described above.
  • the (C) curing agent as the (C) component does not include those corresponding to the above-mentioned (A) to (B) components.
  • the curing agent is not particularly limited as long as it has a function of curing the (A) epoxy resin.
  • Examples include acid anhydride curing agents, cyanate ester curing agents, amine curing agents, phenol curing agents, Examples include naphthol-based curing agents, active ester-based curing agents, and benzoxazine-based curing agents.
  • the curing agent preferably contains one or more selected from acid anhydride-based curing agents, cyanate ester-based curing agents, and amine-based curing agents, from the viewpoint of significantly obtaining the effects of the present invention.
  • the curing agent may be used singly or in combination of two or more.
  • acid anhydride-based curing agents include curing agents having one or more acid anhydride groups in one molecule.
  • Specific examples of acid anhydride curing agents include phthalic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, methyltetrahydrophthalic anhydride, methylhexahydrophthalic anhydride, methylnadic anhydride, and hydrogenated methylnadic acid.
  • a commercially available product may be used as the acid anhydride curing agent.
  • Commercially available products include “HNA-100” (acid anhydride equivalent: 179 g/eq.) manufactured by Shin Nippon Rika Co., Ltd., and the like.
  • cyanate ester curing agents include bisphenol E cyanate ester, bisphenol A dicyanate, polyphenolcyanate, oligo(3-methylene-1,5-phenylenecyanate), 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- 2, such as 3,5-dimethylphenyl)methane, 1,3-bis(4-cyanatophenyl-1-(methylethylidene))benzene, bis(4-cyanatophenyl)thioether, and bis(4-cyanatophenyl)ether.
  • cyanate ester curing agents include "PT30" and “PT60” (phenol novolac type polyfunctional cyanate ester resins), “ULL-950S” (polyfunctional cyanate ester resins) and "BA230” manufactured by Lonza Japan. , "BA230S75” (a prepolymer in which part or all of bisphenol A dicyanate is triazined to form a trimer), and "LECy” (bisphenol E type cyanate ester) manufactured by Lonza.
  • Amine-based curing agents include curing agents having one or more amino groups in one molecule, such as aliphatic amines, polyether amines, alicyclic amines, and aromatic amines. Among them, aromatic amines are preferred from the viewpoint of achieving the desired effects of the present invention.
  • Amine-based curing agents are preferably primary amines or secondary amines, more preferably primary amines. Specific examples of amine-based curing agents include 4,4′-methylenebis(2,6-dimethylaniline), diphenyldiaminosulfone, 4,4′-diaminodiphenylmethane, 4,4′-diaminodiphenylsulfone, and 3,3′.
  • the phenol-based curing agent and naphthol-based curing agent are preferably a phenol-based curing agent having a novolak structure or a naphthol-based curing agent having a novolac structure.
  • a nitrogen-containing phenolic curing agent or a nitrogen-containing naphthol curing agent is preferable, and a triazine skeleton-containing phenolic curing agent or a triazine skeleton-containing naphthol curing agent is more preferable.
  • a triazine skeleton-containing phenol novolak resin is preferable from the viewpoint of highly satisfying heat resistance, water resistance, and adhesion strength to the conductor layer.
  • These may be used individually by 1 type, and may be used in combination of 2 or more type.
  • phenol-based curing agents and naphthol-based curing agents include “MEH-7700”, “MEH-7810” and “MEH-7851” manufactured by Meiwa Kasei Co., Ltd., “NHN” manufactured by Nippon Kayaku Co., Ltd., “CBN”, “GPH”, Nippon Steel Chemical & Materials “SN170”, “SN180”, “SN190”, “SN475", “SN485", “SN495", “SN-495V”, “SN375”, “ SN395", DIC's "TD-2090”, “LA-7052”, “LA-7054”, “LA-1356”, “LA-3018-50P”, “EXB-9500” and the like.
  • the active ester curing agent is not particularly limited, but in general, one molecule of an ester group with high reaction activity such as phenol esters, thiophenol esters, N-hydroxyamine esters, esters of heterocyclic hydroxy compounds, etc. A compound having two or more in it is preferably used.
  • the active ester compound 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.
  • an active ester compound obtained from a carboxylic acid compound and a hydroxy compound is preferred, and an active ester compound obtained from a carboxylic acid compound and a phenol compound and/or a naphthol compound is more preferred.
  • carboxylic acid compounds include benzoic acid, acetic acid, succinic acid, maleic acid, itaconic acid, phthalic acid, isophthalic acid, terephthalic acid, and pyromellitic acid.
  • phenol compounds or naphthol compounds include hydroquinone, resorcinol, bisphenol A, bisphenol F, bisphenol S, phenolphthalin, methylated bisphenol A, methylated bisphenol F, methylated bisphenol S, phenol, o-cresol, m- cresol, p-cresol, catechol, ⁇ -naphthol, ⁇ -naphthol, 1,5-dihydroxynaphthalene, 1,6-dihydroxynaphthalene, 2,6-dihydroxynaphthalene, dihydroxybenzophenone, trihydroxybenzophenone, tetrahydroxybenzophenone, phloroglucine, Benzenetriol, dicyclopentadiene-type diphenol compound, phenol novolak, and the like.
  • dicyclopentadiene-type diphenol compound refers to a diphenol compound obtained by condensing one molecule of dicyclopentadiene with two molecules of phenol.
  • active ester curing agents include dicyclopentadiene-type active ester compounds, naphthalene-type active ester compounds containing a naphthalene structure, active ester compounds containing acetylated phenol novolacs, and active ester compounds containing benzoylated phenol novolacs.
  • Ester compounds are preferred, and among them, at least one compound selected from dicyclopentadiene-type active ester compounds and naphthalene-type active ester compounds is more preferred.
  • the dicyclopentadiene-type active ester compound an active ester compound containing a dicyclopentadiene-type diphenol structure is preferable.
  • active ester curing agents include "EXB9451”, “EXB9460”, “EXB9460S”, “HPC-8000L-65TM” and “HPC-8000-65T” as active ester compounds containing a dicyclopentadiene type diphenol structure.
  • benzoxazine-based curing agents include “HFB2006M” manufactured by Showa High Polymer Co., Ltd., and “Pd” and “Fa” manufactured by Shikoku Kasei Kogyo Co., Ltd.
  • carbodiimide-based curing agents include commercially available carbodiimide-based curing agents such as Nisshinbo Chemical Co., Ltd. Carbodilite V-03 (carbodiimide group equivalent: 216), V-05 (carbodiimide group equivalent: 262), V -07 (carbodiimide group equivalent: 200); V-09 (carbodiimide group equivalent: 200); stabaxol P manufactured by Rhein Chemie (carbodiimide group equivalent: 302).
  • the ratio of the epoxy resin to the curing agent is [total number of epoxy groups in the epoxy resin]:[total number of active groups in the curing agent], and is preferably in the range of 1:0.01 to 1:5. 1:0.3 to 1:3 is more preferred, and 1:0.5 to 1:2 is even more preferred.
  • the number of epoxy groups in the epoxy resin is the sum of all the values obtained by dividing the mass of the non-volatile component of the epoxy resin present in the resin composition by the epoxy equivalent.
  • the “number of active groups in the curing agent” is the sum of all the values obtained by dividing the mass of the non-volatile component of the curing agent present in the resin composition by the active group equivalent.
  • the content of the curing agent is preferably 1% by mass or more, more preferably 2% by mass or more, and more preferably 100% by mass of non-volatile components in the resin composition. is 3% by mass or more.
  • the upper limit is preferably 20% by mass or less, more preferably 15% by mass or less, and even more preferably 10% by mass or less.
  • the resin composition may further contain (D) a curing accelerator as an optional component in combination with the components (A) to (B) described above.
  • the (D) curing accelerator as the (D) component does not include those corresponding to the above-described components (A) to (C).
  • the curing accelerator functions as a curing catalyst that accelerates the curing of the (A) epoxy resin.
  • (D) As the curing accelerator (A) a compound that accelerates the curing of the epoxy resin can be used.
  • Such (D) curing accelerators include, for example, phosphorus-based curing accelerators, urea-based curing accelerators, guanidine-based curing accelerators, imidazole-based curing accelerators, metal-based curing accelerators, amine-based curing accelerators, and the like. is mentioned.
  • the curing accelerator may be used alone or in combination of two or more.
  • Phosphorus curing accelerators include, for example, tetrabutylphosphonium bromide, tetrabutylphosphonium chloride, tetrabutylphosphonium acetate, tetrabutylphosphonium decanoate, tetrabutylphosphonium laurate, bis(tetrabutylphosphonium) pyromellitate, tetrabutylphosphonium hydro Aliphatic phosphonium salts such as genhexahydrophthalate, tetrabutylphosphonium 2,6-bis[(2-hydroxy-5-methylphenyl)methyl]-4-methylphenolate, di-tert-butyldimethylphosphonium tetraphenylborate; methyltriphenylphosphonium bromide, ethyltriphenylphosphonium bromide, propyltriphenylphosphonium bromide, butyltriphenylphosphonium bromide, benzyltripheny
  • Urea-based curing accelerators include, for example, 1,1-dimethylurea; 1,1,3-trimethylurea, 3-ethyl-1,1-dimethylurea, 3-cyclohexyl-1,1-dimethylurea, 3- Aliphatic dimethylurea such as 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-dimethyl
  • Guanidine curing accelerators include, 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]dec-5-ene, 7-methyl-1,5,7-triazabicyclo[4.4.0] Dec-5-ene, 1-methylbiguanide, 1-ethylbiguanide, 1-n-butylbiguanide, 1-n-octadecylbiguanide, 1,1-dimethylbiguanide, 1,1-diethylbiguanide, 1-cyclohexylbiguanide, 1 -allylbiguanide, 1-phenylbiguanide, 1-(o-tolyl)biguanide and
  • imidazole curing accelerators examples include 2-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, 1-benzyl-2-methylimidazole, 1-benzyl-2-phenylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2-ethyl-4-methylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-cyanoethyl- 2-phenylimidazolium trimellitate, 2,4-d
  • imidazole curing accelerators include, for example, Shikoku Kasei Co., Ltd. "1B2PZ”, “2E4MZ”, “2MZA-PW”, “2MZ-OK”, “2MA-OK”, “2MA-OK- PW”, “2PHZ”, “2PHZ-PW”, "Cl1Z”, “Cl1Z-CN”, “Cl1Z-CNS”, “C11Z-A”; and "P200-H50” manufactured by Mitsubishi Chemical Corporation.
  • metal-based curing accelerators include organometallic complexes or organometallic salts of metals such as cobalt, copper, zinc, iron, nickel, manganese, and tin.
  • organometallic complexes include organocobalt complexes such as cobalt (II) acetylacetonate and cobalt (III) acetylacetonate, organocopper complexes such as copper (II) acetylacetonate, and 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.
  • organic metal salts include zinc octoate, tin octoate, zinc naphthenate, cobalt naphthenate, tin stearate, and zinc stearate.
  • amine curing accelerators examples include trialkylamines such as triethylamine and tributylamine, 4-dimethylaminopyridine, benzyldimethylamine, 2,4,6-tris(dimethylaminomethyl)phenol, 1,8-diazabicyclo (5,4,0)-undecene and the like.
  • amine-based curing accelerator a commercially available product may be used, such as "MY-25" manufactured by Ajinomoto Fine-Techno Co., Ltd., and the like.
  • the content of the curing accelerator is preferably 0.01% by mass or more, more preferably 0, when the non-volatile component in the resin composition is 100% by mass, from the viewpoint of significantly obtaining the effects of the present invention. 0.03% by mass or more, more preferably 0.05% by mass or more, preferably 1% by mass or less, more preferably 0.5% by mass or less, and even more preferably 0.1% by mass or less.
  • the resin composition may contain (E) a silane coupling agent as an optional component in combination with the components (A) to (B) described above.
  • the (E) silane coupling agent is a silane coupling agent that does not surface-treat the (B) inorganic filler, not the surface-treating agent that surface-treats the (B) inorganic filler.
  • the silane coupling agent may be the same as or different from (B) the surface treating agent for surface treating the inorganic filler.
  • (E) a silane coupling agent may be used individually by 1 type, and may be used in combination of 2 or more type.
  • the silane coupling agent is as described above.
  • the content of the silane coupling agent is preferably 0.01% by mass or more, more preferably 0.01% by mass or more, when the non-volatile component in the resin composition is 100% by mass, from the viewpoint of significantly obtaining the effects of the present invention. is 0.03% by mass or more, more preferably 0.05% by mass or more, preferably 1% by mass or less, more preferably 0.5% by mass or less, and still more preferably 0.1% by mass or less.
  • the resin composition may further contain (F) an optional additive as an optional non-volatile component in combination with the components (A) to (E) described above.
  • Optional additives include, for example, thermoplastic resins; polymerization initiators; organometallic compounds such as organocopper compounds, organozinc compounds, and organocobalt compounds; Colorants such as crystal violet, titanium oxide, 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 bentone and montmorillonite; Antifoaming agents such as silicone antifoaming agents, acrylic antifoaming agents, fluorine antifoaming agents, vinyl resin antifoaming agents; UV absorbers such as benzotriazole UV absorbers; Adhesion improvers such as urea silane Adhesion imparting agents such as tri
  • phosphate ester dispersants such as borate stabilizers, titanate stabilizers, aluminate stabilizers, zirconate stabilizers, isocyanate stabilizers, carboxylic acid stabilizers, and carboxylic anhydride stabilizers photopolymerization initiation aids such as tertiary amines; photosensitizers such as pyrarizones, anthracenes, coumarins, xanthones, and thioxanthones; (F) Any additive may be used alone or in combination of two or more.
  • the resin composition may further contain any solvent as a volatile component.
  • solvents include organic solvents.
  • a solvent may be used individually by 1 type, and may be used in combination of 2 or more types by arbitrary ratios. The smaller the amount of solvent, the better.
  • the amount of the solvent is preferably 3% by mass or less, more preferably 1% by mass or less, still more preferably 0.5% by mass or less, still more preferably 0.1% by mass, based on 100% by mass of the non-volatile components in the resin composition. It is not more than 0.01% by mass, more preferably not more than 0.01% by mass, and is particularly preferably not contained (0% by mass).
  • the resin composition may be in the form of a paste when the amount of the solvent is small in this way.
  • the viscosity of the pasty resin composition at 25° C. is preferably in the range of 20 Pa ⁇ s to 1000 Pa ⁇ s.
  • the resin composition of the present invention is preferably liquid or paste even if the amount of solvent is within the above range.
  • the resin composition is prepared by appropriately mixing the necessary components among the above components, and if necessary, by kneading means such as a three-roll mill, ball mill, bead mill, sand mill, or stirring means such as a super mixer or planetary mixer. It can be prepared by kneading or mixing.
  • the strain (%) of the cured product obtained by thermally curing the resin composition at 150 ° C. for 60 minutes is on the X axis
  • the bending strength (MPa) of the cured product by thermally curing the resin composition at 150 ° C. for 60 minutes is on the Y axis.
  • the "intersection point between the X axis and the Y axis" corresponds to the origin of the XY coordinate system in which the SS curve is created.
  • the area of the triangle ((maximum bending strength (MPa) x strain (%) at maximum bending strength)/2) is referred to as "toughness value”.
  • the resin composition of the present invention has a toughness value exceeding 30 MPa. Therefore, it is possible to form an insulating layer in which the occurrence of cracks and delamination is suppressed.
  • the X axis shows the strain (%) of the cured product obtained by thermally curing the resin composition at 150 ° C. for 60 minutes
  • the Y axis shows the bending of the cured product obtained by thermally curing the resin composition at 150 ° C. for 60 minutes.
  • MPa strength
  • the toughness value is obtained from the perpendicular line A1 drawn from the maximum bending strength point (maximum bending strength) M1 to the X axis, and the intersection point P1 of the perpendicular line A1 with the X axis on the X axis and the Y axis.
  • a triangle having two sides of the straight line B1 to the intersection O with is created, and the area of the triangle is represented by S1. That is, the toughness value of the resin composition having the SS curve ( ⁇ ) is represented by the maximum point M1, the intersection point P1, and the area S1 of a triangle having the intersection point O as vertices.
  • the toughness value is obtained from the perpendicular line A2 drawn from the maximum bending strength point M2 to the X axis, and the intersection point P2 of the perpendicular line A2 with the X axis and the intersection point of the X axis and the Y axis.
  • a triangle having two sides of a straight line B2 to O is created and represented by the area S2 of the triangle. That is, the toughness value of the resin composition having the SS curve ( ⁇ ) is represented by the maximum point M2, the intersection point P2, and the area S2 of a triangle with the intersection point O as the vertices.
  • the toughness value exceeds 30 MPa, preferably 33 MPa or more, more preferably 35 MPa or more, and still more preferably 40 MPa, 41 MPa or more. Although the upper limit is not particularly limited, it is preferably 100 MPa or less, more preferably 90 MPa or less, and still more preferably 80 MPa or less, 70 MPa or less, and 60 MPa or less.
  • the toughness value can be measured by the method described in Examples below.
  • a cured product obtained by thermally curing the resin composition at 180°C for 90 minutes exhibits the characteristic that the amount of warpage is suppressed. Therefore, an insulating layer with a suppressed amount of warpage can be formed.
  • the amount of warpage of the insulating layer having a thickness of 100 ⁇ m is preferably 1500 ⁇ m or less, more preferably 1250 ⁇ m or less, and even more preferably 1000 ⁇ m or less. Although the lower limit is not particularly limited, it may be 0 ⁇ m or more, 1 ⁇ m or more, or the like.
  • the amount of warpage can be measured by the method described in Examples below.
  • a cured product obtained by thermally curing the resin composition at 180°C for 90 minutes exhibits the characteristic that the amount of warpage is suppressed. Therefore, an insulating layer with a suppressed amount of warpage can be formed.
  • the amount of warpage of the insulating layer having a thickness of 300 ⁇ m is preferably 5000 ⁇ m or less, more preferably 4500 ⁇ m or less, and even more preferably 4000 ⁇ m or less. Although the lower limit is not particularly limited, it may be 0 ⁇ m or more, 1 ⁇ m or more, or the like.
  • the amount of warpage can be measured by the method described in Examples below.
  • a cured product obtained by thermally curing the resin composition at 180°C for 90 minutes exhibits a high storage modulus at 245°C. Therefore, it is possible to form an insulating layer in which the occurrence of cracks is suppressed.
  • the storage modulus is preferably 0.5 GPa or more, more preferably 0.8 GPa or more, and still more preferably 1 GPa or more. Although the upper limit is not particularly limited, it may be 10 GPa or less, 5 GPa or less, or the like.
  • the storage modulus can be measured by the method described in Examples below.
  • a cured product obtained by thermally curing the resin composition at 150°C for 60 minutes has excellent toughness value and storage elastic modulus, so it exhibits the property of suppressing the occurrence of cracks and delamination. Therefore, it is possible to form an insulating layer in which the occurrence of cracks and delamination is suppressed.
  • the resin composition is compression-molded to a thickness of 400 ⁇ m, and mold underfill is applied to the chip component. Thereafter, the resin composition is heat-cured at 150° C. for 60 minutes to obtain a cured product.
  • a thermal cycle test of the cured product did not cause delamination with the chip component or cracks in the cured product. The details can be measured by the method described in Examples below.
  • the resin composition of the present invention is a resin composition for a semiconductor device having a semiconductor chip package having an area of 100 mm 2 or more (a resin composition used for a semiconductor device including a semiconductor chip package having a substrate having an area of 100 mm 2 or more). ) can be suitably used as.
  • the resin composition of the present invention includes a resin composition for a semiconductor device including a semiconductor chip package having a protruding electrode such as a copper post (a resin composition used for a semiconductor device including a semiconductor chip package having a protruding electrode), a protruding electrode, and a protruding electrode.
  • a resin composition for a semiconductor device including a semiconductor package including a step of polishing (a resin composition used for a semiconductor device including a semiconductor package including a step of polishing a protruding electrode) can be used in a wide range of applications.
  • the resin sheet of the present invention includes a support and a resin composition layer formed of the resin composition of the present invention provided on the support.
  • the thickness of the resin composition layer is preferably 100 ⁇ m or less, more It is preferably 70 ⁇ m or less, more preferably 55 ⁇ m or less. Although the lower limit of the thickness of the resin composition layer is not particularly limited, it can be usually 5 ⁇ m or more, 10 ⁇ m or more, or the like.
  • the support examples include a film made of a plastic material, a metal foil, and a release paper, and a film made of a plastic material and a metal foil are preferable.
  • plastic material examples include polyethylene terephthalate (hereinafter sometimes abbreviated as "PET”) and polyethylene naphthalate (hereinafter sometimes abbreviated as “PEN”).
  • PET polyethylene terephthalate
  • PEN polyethylene naphthalate
  • PC polycarbonate
  • acrylic such as polymethyl methacrylate (PMMA)
  • PMMA polymethyl methacrylate
  • TAC triacetyl cellulose
  • PES polyether sulfide
  • polyether ketones polyimides, and the like.
  • polyethylene terephthalate and polyethylene naphthalate are preferable, and inexpensive polyethylene terephthalate is particularly preferable.
  • examples of the metal foil include copper foil and aluminum foil, with copper foil being preferred.
  • a foil made of a single metal of copper may be used, and a foil made of an alloy of copper and other metals (for example, tin, chromium, silver, magnesium, nickel, zirconium, silicon, titanium, etc.) may be used. may be used.
  • the support may be subjected to matte treatment, corona treatment, or antistatic treatment on the surface to be bonded to the resin composition layer.
  • a support with a release layer having a release layer on the surface to be bonded to the resin composition layer may be used.
  • the release agent used in the release layer of the release layer-attached support includes, for example, one or more release agents selected from the group consisting of alkyd resins, polyolefin resins, urethane resins, and silicone resins.
  • a commercially available product may be used, for example, "SK-1", “ AL-5", “AL-7”, Toray's "Lumirror T60", Teijin's "Purex”, and Unitika's "Unipeel”.
  • the thickness of the support is not particularly limited, but is preferably in the range of 5 ⁇ m to 75 ⁇ m, more preferably in the range of 10 ⁇ m to 60 ⁇ m.
  • the thickness of the release layer-attached support as a whole is preferably within the above range.
  • the resin sheet may further contain other layers as necessary.
  • Such other layers include, for example, a protective film conforming to the support provided on the surface of the resin composition layer not bonded to the support (that is, the surface opposite to the support). be done.
  • the thickness of the protective film is not particularly limited, it is, for example, 1 ⁇ m to 40 ⁇ m.
  • a resin varnish is prepared by dissolving a resin composition in an organic solvent, the resin varnish is applied onto a support using a die coater or the like, and dried to form a resin composition layer. It can be manufactured by
  • organic solvents examples include ketones such as acetone, methyl ethyl ketone (MEK) and cyclohexanone; acetic acid esters such as ethyl acetate, butyl acetate, cellosolve acetate, propylene glycol monomethyl ether acetate and carbitol acetate; cellosolve and butyl carbitol; carbitols; aromatic hydrocarbons such as toluene and xylene; amide solvents such as dimethylformamide, dimethylacetamide (DMAc) and N-methylpyrrolidone.
  • An organic solvent may be used individually by 1 type, and may be used in combination of 2 or more type.
  • Drying may be carried out by known methods such as heating and blowing hot air.
  • the drying conditions are not particularly limited, but the resin composition layer is dried so that the content of the organic solvent is 10% by mass or less, preferably 5% by mass or less. Although it varies depending on the boiling point of the organic solvent in the resin varnish, for example, when using a resin varnish containing 30% by mass to 60% by mass of the organic solvent, drying at 50 ° C. to 150 ° C. for 3 minutes to 10 minutes
  • the resin composition layer can be formed.
  • the resin sheet can be rolled up and stored.
  • the resin sheet has a protective film, it can be used by peeling off the protective film.
  • the semiconductor chip package of the present invention includes a cured product layer formed from a cured product of the resin composition of the present invention, and a semiconductor chip mounted on the cured product layer.
  • the cured material layer can be an insulating layer or a sealing layer.
  • This semiconductor chip package can be manufactured, for example, by a manufacturing method including the following steps (1) to (2). Moreover, it is preferable that the steps (1) to (2) are included in this order. (1) A step of forming a resin composition layer on a substrate. (2) A step of thermosetting the resin composition layer to form an insulating layer.
  • the method for manufacturing a semiconductor chip package preferably includes step (3) after step (2). (3) polishing the insulating layer;
  • a resin composition layer is formed on a substrate.
  • the resin composition layer may be the same as the resin composition layer of the resin sheet.
  • the resin composition layer can be formed by laminating resin sheets such that the resin composition layer of the resin sheet is bonded to the substrate.
  • Materials for the substrate include, for example, glass epoxy substrates, metal substrates, polyester substrates, polyimide substrates, BT resin substrates, thermosetting polyphenylene ether substrates, and the like.
  • a substrate with metal posts having a plurality of projecting electrodes such as metal posts is preferable.
  • the substrate with metal posts preferably has a large area so that a plurality of semiconductor chips can be arranged on the metal posts.
  • the area of the substrate with metal posts is the same as that of the semiconductor chip package, preferably 100 mm 2 or more, more preferably 150 mm 2 or more, and even more preferably 200 mm 2 or more.
  • the upper limit is not particularly limited, it may be 1000 mm 2 or less.
  • a substrate with metal posts is produced by, for example, a step of laminating a dry film on a base material, and a step of forming a pattern by exposing and developing the dry film under predetermined conditions using a photomask to obtain a patterned dry film.
  • the metal posts can be formed by a plating method such as electroplating using the developed patterned dry film as a plating mask, and the step of peeling off the patterned dry film.
  • a photosensitive dry film made of a photoresist composition can be used.
  • a dry film made of a resin such as a novolak resin or an acrylic resin can be used.
  • the conditions for laminating the substrate and the dry film may be the same as the conditions for laminating the substrate and the resin sheet, which will be described later. Stripping of the dry film can be carried out using, for example, an alkaline stripping solution such as sodium hydroxide solution.
  • the height of the metal post is preferably 1 ⁇ m or more, more preferably 5 ⁇ m or more, and still more preferably 10 ⁇ m or more, 15 ⁇ m or more, 20 ⁇ m or more, or 25 ⁇ m or more, from the viewpoint of obtaining the effects of the present invention remarkably.
  • the upper limit is not particularly limited, it may be 100 ⁇ m or less, 50 ⁇ m or less, or the like.
  • the width of the metal post is preferably 1 ⁇ m or more, more preferably 5 ⁇ m or more, and still more preferably 8 ⁇ m or more, 10 ⁇ m or more, 20 ⁇ m or more, 30 ⁇ m or more, 40 ⁇ m or more, or 50 ⁇ m, from the viewpoint of significantly obtaining the effects of the present invention. 100 ⁇ m or more, 150 ⁇ m or more, or 200 ⁇ m or more. Although the upper limit is not particularly limited, it may be 1000 ⁇ m or less, 500 ⁇ m or less, or the like.
  • the metal posts preferably contain one or more metals selected from the group consisting of gold, platinum, palladium, silver, copper, aluminum, cobalt, chromium, zinc, nickel, titanium, tungsten, iron, tin and indium.
  • the metal post may be a single metal layer or an alloy layer.
  • the alloy layer may be, for example, an alloy of two or more metals selected from the above group (for example, a nickel-chromium alloy, a copper-chromium alloy, a nickel alloys and copper-titanium alloys).
  • single metal layers of chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver or copper, nickel-chromium alloys, copper- Nickel alloys and copper/titanium alloy alloy layers are preferred, and single metal layers of chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver or copper, or nickel/chromium alloy alloy layers are more preferred, and copper single metal layers are preferred.
  • Metal layers (copper posts) are more preferred.
  • a resin composition layer is formed on the base material.
  • the resin composition layer is preferably formed so that the metal posts are embedded in the resin composition layer.
  • the formation of the resin composition layer can be performed by compression molding.
  • an upper mold and a lower mold are prepared as molds.
  • a substrate is coated with a liquid or paste resin composition.
  • the substrate coated with the resin composition is attached to the lower mold. After that, the upper mold and the lower mold are clamped, and heat and pressure are applied to the resin composition for compression molding.
  • the specific operation of the compression molding method may be, for example, as follows.
  • An upper mold and a lower mold are prepared as molds for compression molding.
  • a resin composition is placed on the lower mold.
  • the substrate is attached to the upper mold.
  • the upper mold and the lower mold are clamped so that the resin composition placed on the lower mold is in contact with the substrate attached to the upper mold, and heat and pressure are applied to perform compression molding.
  • the molding conditions in the compression molding method differ depending on the composition of the resin composition.
  • the temperature of the mold during molding is preferably a temperature at which the resin composition can exhibit excellent compression moldability. It is 200° C. or lower, more preferably 170° C. or lower, and still more preferably 150° C. or lower.
  • the pressure applied during molding is preferably 1 MPa or higher, more preferably 3 MPa or higher, still more preferably 5 MPa or higher, and preferably 50 MPa or lower, more preferably 30 MPa or lower, and still more preferably 20 MPa or lower.
  • the curing time is preferably 1 minute or longer, more preferably 2 minutes or longer, particularly preferably 5 minutes or longer, and preferably 60 minutes or shorter, more preferably 30 minutes or shorter, and particularly preferably 20 minutes or shorter.
  • the mold is usually removed. The mold may be removed before or after heat curing of the resin composition layer.
  • the resin composition layer it may be performed by laminating a resin sheet and a substrate.
  • This lamination can be performed, for example, by bonding the resin composition layer to the substrate by thermocompression bonding the resin sheet to the substrate from the support side.
  • the member for thermocompression bonding the resin sheet to the substrate include heated metal plates (such as SUS end plates) and metal rolls (such as SUS rolls). be done.
  • thermocompression member instead of pressing the thermocompression member directly onto the resin sheet, it is preferable to press the resin sheet through an elastic material such as heat-resistant rubber so that the resin sheet can sufficiently follow the uneven surface of the substrate.
  • the resin composition layer may be formed by applying a resin composition to the substrate instead of the resin sheet, and the resin composition of the present invention may be included. It may be carried out by laminating the prepreg with the base material.
  • the lamination of the base material and the resin sheet may be carried out, for example, by a vacuum lamination method.
  • the thermocompression bonding temperature is preferably in the range of 60°C to 160°C, more preferably 80°C to 140°C.
  • the thermocompression pressure is preferably in the range of 0.098 MPa to 1.77 MPa, more preferably 0.29 MPa to 1.47 MPa.
  • the thermocompression bonding time is preferably in the range of 20 seconds to 400 seconds, more preferably 30 seconds to 300 seconds.
  • Lamination is preferably carried out under reduced pressure conditions of 13 hPa or less.
  • the laminated resin sheets may be smoothed under normal pressure (atmospheric pressure), for example, by pressing a thermocompression member from the support side. Pressing conditions for the smoothing treatment may be the same as the thermocompression bonding conditions for the lamination described above. Lamination and smoothing may be performed continuously using a vacuum laminator.
  • the support may be removed after step (1) and before step (2), or after step (2) and before step (3).
  • the resin composition layer may be formed by directly applying the resin composition onto the surface of the substrate.
  • the resin composition to be applied is as described above.
  • the insulating layer is formed by thermosetting the resin composition layer.
  • the thermosetting conditions for the resin composition layer vary depending on the type of resin composition, but the curing temperature is usually in the range of 120°C to 240°C (preferably in the range of 150°C to 220°C, more preferably in the range of 170°C to 200°C). range), and the curing time is in the range of 5 minutes to 120 minutes (preferably 10 minutes to 100 minutes, more preferably 15 minutes to 90 minutes).
  • the resin composition layer Before thermally curing the resin composition layer, the resin composition layer may be subjected to a preliminary heating treatment of heating at a temperature lower than the curing temperature.
  • the resin composition layer prior to thermosetting the resin composition layer, the resin composition layer is usually heated at a temperature of 50 ° C. or higher and lower than 120 ° C. (preferably 60 ° C. or higher and 110 ° C. or lower, more preferably 70 ° C. or higher and 100 ° C. or lower). may be preheated for usually 5 minutes or more (preferably 5 minutes to 150 minutes, more preferably 15 minutes to 120 minutes).
  • step (3) the insulating layer is polished to expose the surface of the metal post to the main surface of the insulating layer, and if necessary, the metal post is also polished until the height of the metal post is within a predetermined range. do. Since the insulating layer is made of the resin composition of the present invention, separation between the insulating layer and the metal post can be suppressed.
  • a method for polishing the insulating layer a method capable of polishing the insulating layer can be used. Examples of such polishing methods include CMP (chemical mechanical polishing), buffing, and belt polishing. Examples of commercially available buffing devices include "NT-700IM" manufactured by Ishii Hokumon Co., Ltd., and the like. Polishing conditions may be carried out according to methods known to those skilled in the art.
  • the arithmetic mean roughness (Ra) of the polished surface of the insulating layer is preferably 1000 nm or less, more preferably 900 nm or less, and even more preferably 800 nm or less from the viewpoint of improving adhesion.
  • the lower limit is not particularly limited, it may be 1 ⁇ m or more, 10 ⁇ m or more, or the like.
  • the surface roughness (Ra) can be measured using, for example, a non-contact surface roughness meter.
  • the method for manufacturing a semiconductor chip package further comprises: (4) A step of bonding the semiconductor chip onto the substrate. (5) forming a sealing layer on the semiconductor chip; may contain Steps (4) and (5) are preferably performed in this order.
  • a method of forming the semiconductor chip on the metal post of the base material can be adopted.
  • the method of forming the semiconductor chip on the metal posts may be carried out according to methods known to those skilled in the art used in the manufacture of semiconductor chip packages.
  • the sealing layer is usually formed from a cured composition that is used to form the sealing layer or insulating layer of printed wiring boards.
  • the encapsulation layer is usually formed by a method comprising the steps of forming a layer containing the composition on the semiconductor chip and thermally curing the layer containing the composition to form the encapsulation layer.
  • a method of forming a layer containing a composition on a semiconductor chip is usually carried out using a sealing resin sheet having a support and a layer containing the composition. Specifically, the layer containing the composition of the sealing resin sheet and the semiconductor chip are laminated to form the layer containing the composition on the semiconductor chip.
  • the conditions for laminating the semiconductor chip and the sealing resin sheet are the same as those for laminating the base material and the resin sheet in step (1).
  • thermosetting conditions for the layer containing the composition are the same as the thermosetting conditions for the resin composition layer in step (2).
  • step (5) a step of polishing the sealing layer may be performed as necessary. Polishing of the sealing layer can be performed under the same conditions as in step (3).
  • a semiconductor device of the present invention includes the printed wiring board of the present invention.
  • the semiconductor device of the present invention can be manufactured using the printed wiring board of the present invention.
  • semiconductor devices examples include various semiconductor devices used in electrical products (such as computers, mobile phones, digital cameras, televisions, etc.) and vehicles (such as motorcycles, automobiles, trains, ships, aircraft, etc.).
  • the semiconductor device of the present invention can be manufactured by mounting components (semiconductor chips) on conductive portions of a printed wiring board.
  • a “conducting part” is a “part where an electric signal is transmitted on a printed wiring board", and the place may be a surface or an embedded part.
  • the semiconductor chip is not particularly limited as long as it is an electric circuit element made of a semiconductor.
  • the method of mounting the semiconductor chip when manufacturing the semiconductor device of the present invention is not particularly limited as long as the semiconductor chip functions effectively.
  • Examples include a mounting method using a buildup layer (BBUL), a mounting method using an anisotropic conductive film (ACF), and a mounting method using a non-conductive film (NCF).
  • BBUL buildup layer
  • ACF anisotropic conductive film
  • NCF non-conductive film
  • BBUL a mounting method using a build-up layer without bumps
  • Naphthalene type epoxy resin manufactured by DIC “HP4032D", epoxy equivalent 140 g / eq. 10 parts, inorganic filler 1 90 parts, acid anhydride curing agent (Shin Nippon Rika Co., Ltd., "HNA-100", acid anhydride Equivalent weight 179 g / eq.) 10 parts, curing accelerator (manufactured by Shikoku Kasei Co., Ltd., "1B2PZ”) 0.1 part, and silane coupling agent (manufactured by Shin-Etsu Chemical Co., Ltd., "KBM-403”) 0.1 part was blended and uniformly dispersed in a mixer to obtain a resin composition.
  • acid anhydride curing agent Shin Nippon Rika Co., Ltd., "HNA-100", acid anhydride Equivalent weight 179 g / eq.
  • curing accelerator manufactured by Shikoku Kasei Co., Ltd., "1B2PZ
  • silane coupling agent manufactured by Shin
  • Example 2 In Example 1, 1) Change the amount of naphthalene type epoxy resin ("HP4032D” manufactured by DIC, epoxy equivalent 140 g/eq.) from 10 parts to 5 parts, 2) Using 5 parts of glycidylamine type epoxy resin ("JER630LSD” manufactured by Mitsubishi Chemical Corporation, epoxy equivalent 95 g / eq.), 3) Inorganic filler 1 90 parts was changed to inorganic filler 2 90 parts. A resin composition was obtained in the same manner as in Example 1 except for the above matters.
  • HP4032D manufactured by DIC, epoxy equivalent 140 g/eq.
  • Example 3 In Example 2, 1) 5 parts of naphthalene type epoxy resin ("HP4032D” manufactured by DIC, epoxy equivalent 140 g/eq.) is changed to 5 parts of polyvalent glycidyl compound ("PETG” manufactured by Showa Denko KK, epoxy equivalent 92 g/eq.), 2) Inorganic filler 2 90 parts was changed to inorganic filler 1 90 parts. A resin composition was obtained in the same manner as in Example 2 except for the above matters.
  • Epoxy resin mixture (mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin, "ZX-1059” manufactured by Nippon Steel Chemical & Materials Co., Ltd., epoxy equivalent 170 g / eq.) 3 parts, glycidylamine type epoxy resin (Mitsubishi Chemical Co., Ltd. "JER630LSD” manufactured by Showa Denko Co., Ltd., epoxy equivalent 95 g / eq.) 5 parts, polyvalent glycidyl compound (manufactured by Showa Denko "BATG”, epoxy equivalent 119 g / eq.) 2 parts, inorganic filler 2 90 parts, amine curing agent ( Nippon Kayaku Co., Ltd.
  • Example 5 Naphthalene type epoxy resin (manufactured by DIC “HP4032D”, epoxy equivalent 140 g / eq.) 5 parts, glycidylamine type epoxy resin (manufactured by Mitsubishi Chemical Corporation “JER630LSD”, epoxy equivalent 95 g / eq.) 4 parts, glycidylamine type epoxy Resin ("ELM-434VL” manufactured by Sumitomo Chemical Co., Ltd.) 1 part, inorganic filler 1 90 parts, cyanate curing agent (manufactured by Lonza, bisphenol E type cyanate ester "LECy”) 3 parts, curing accelerator (Shikoku Kasei Co., Ltd.
  • Example 6 In Example 1, 90 parts of inorganic filler 1 was changed to 110 parts of inorganic filler 3. A resin composition was obtained in the same manner as in Example 1 except for the above matters.
  • Example 1 ⁇ Comparative Example 1> In Example 1, 1) Using 3 parts of a polyvalent glycidyl compound (“PETG” manufactured by Showa Denko Co., Ltd., epoxy equivalent 92 g / eq.), 2) Inorganic filler 1 90 parts was changed to inorganic filler 4 90 parts. A resin composition was obtained in the same manner as in Example 1 except for the above matters.
  • PETG polyvalent glycidyl compound manufactured by Showa Denko Co., Ltd., epoxy equivalent 92 g / eq.
  • Example 4 Change the amount of glycidylamine type epoxy resin ("JER630LSD” manufactured by Mitsubishi Chemical Corporation, epoxy equivalent 95 g / eq.) from 5 parts to 10 parts, 2) The amount of epoxy resin mixture (mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin, "ZX1059” manufactured by Nippon Steel Chemical & Material, epoxy equivalent 170 g / eq.) was changed from 3 parts to 5 parts, 3) Without using 2 parts of a polyvalent glycidyl compound (“BATG” manufactured by Showa Denko Co., Ltd., epoxy equivalent 119 g / eq.), 4) 90 parts of inorganic filler 2 is changed to 90 parts of inorganic filler 3, 5) The amount of amine-based curing agent (“Kayahard AA” manufactured by Nippon Kayaku Co., Ltd.) was changed from 3 parts to 5 parts. A resin composition was obtained in the same manner as in Example 4 except for the above matters.
  • the cured product was cut into a test piece having a width of 7 mm and a length of 40 mm, and subjected to dynamic mechanical analysis in tensile mode using a dynamic mechanical analyzer DMS-6100 (manufactured by Seiko Instruments Inc.). After mounting the test piece on the apparatus, measurement was performed under the measurement conditions of a frequency of 1 Hz and a heating rate of 5° C./min. The value of storage modulus (E') GPa at 245°C in this measurement was read.
  • the resin compositions prepared in Examples and Comparative Examples were used to form a resin composition layer having a thickness of 1 mm by means of a compression molding apparatus on a SUS plate which had been subjected to mold release treatment. After that, the resin composition layer was peeled off from the SUS plate and thermally cured at 150° C. for 60 minutes. The thermoset resin composition layer was cut into a width of 10 mm, a length of 40 mm and a thickness of 1 mm to obtain a test piece for measuring three-point bending strength. A three-point bending test was performed at 245° C.
  • Chip parts with copper bumps on a 12-inch silicon wafer with a thickness of 775 ⁇ m (chip size 10 mm ⁇ 10 mm, chip thickness 300 ⁇ m, copper bump size diameter 20 ⁇ m, height 30 ⁇ m, copper bump pitch 40 ⁇ m, WALTS-TEG FBW40A-0001JY manufactured by Waltz) was mounted on a silicon wafer with adhesive on the four corners with copper bumps in contact.
  • the resin compositions prepared in Examples and Comparative Examples were compression-molded using a compression molding apparatus (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) so that the resin thickness was 400 ⁇ m.
  • a mold underfill (MUF) was performed on the part.
  • a thermal cycle test ( ⁇ 55° C. to 125° C., 500 cycles) was performed and evaluated according to the following criteria. ⁇ : No delamination with the chip component or resin crack occurred after the test. x: Chip component and delamination or resin crack occurred after the test.
  • the measurement was performed in accordance with JEITA EDX-7311-24 of the Japan Electronics and Information Technology Industries Association standard. Specifically, a virtual plane calculated by the method of least squares of all data of the substrate surface in the measurement area was used as a reference plane, and the difference between the minimum value and the maximum value in the direction perpendicular to the reference plane was obtained as the amount of warpage.

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  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
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  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Structures Or Materials For Encapsulating Or Coating Semiconductor Devices Or Solid State Devices (AREA)
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JP2017048400A (ja) * 2016-11-29 2017-03-09 味の素株式会社 樹脂組成物
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JP2021161206A (ja) * 2020-03-31 2021-10-11 味の素株式会社 樹脂組成物、樹脂ペースト、硬化物、樹脂シート、プリント配線板、半導体チップパッケージ及び半導体装置

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Publication number Priority date Publication date Assignee Title
JP2006036916A (ja) * 2004-07-27 2006-02-09 Admatechs Co Ltd スラリー組成物、ワニス組成物、およびそれを用いた絶縁フィルム、プリプレグ
JP2006052357A (ja) * 2004-08-16 2006-02-23 Denki Kagaku Kogyo Kk 充填材及びその製造方法
JP2007262126A (ja) * 2006-03-27 2007-10-11 Toray Ind Inc フレキシブル印刷回路用接着剤組成物およびそれを用いたカバーレイフィルム、銅張り積層板、接着剤シート、リードフレーム固定テープ
JP2011089038A (ja) * 2009-10-22 2011-05-06 Ajinomoto Co Inc 樹脂組成物
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