Classifications

• • 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
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B15/00—Layered products comprising a layer of metal
  • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
  • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B15/00—Layered products comprising a layer of metal
  • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
  • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
  • B32B15/092—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin comprising epoxy resins
• • 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
  • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
  • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
  • C08J5/18—Manufacture of films or sheets
• • 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
  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
  • C08K3/20—Oxides; Hydroxides
  • C08K3/22—Oxides; Hydroxides of metals
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
  • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
  • C08L23/04—Homopolymers or copolymers of ethene
  • C08L23/08—Copolymers of ethene
  • C08L23/0846—Copolymers of ethene with unsaturated hydrocarbons containing atoms other than carbon or hydrogen
  • C08L23/0869—Copolymers of ethene with unsaturated hydrocarbons containing atoms other than carbon or hydrogen with unsaturated acids, e.g. [meth]acrylic acid; with unsaturated esters, e.g. [meth]acrylic acid esters
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
  • C08J2363/00—Characterised by the use of epoxy resins; Derivatives of epoxy resins
• • 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
  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
  • C08K3/20—Oxides; Hydroxides
  • C08K3/22—Oxides; Hydroxides of metals
  • C08K2003/2227—Oxides; Hydroxides of metals of aluminium
• • 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
  • C08K2201/00—Specific properties of additives
  • C08K2201/002—Physical properties
  • C08K2201/005—Additives being defined by their particle size in general
• • 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
  • C08K2201/00—Specific properties of additives
  • C08K2201/014—Additives containing two or more different additives of the same subgroup in C08K

Definitions

• the present invention relates to a thermosetting resin composition, a resin sheet, a heat sink, a method for manufacturing a resin sheet, and a method for manufacturing a heat sink.
• the electronic components When a device equipped with many electronic components such as IC chips and transistors is operated, the electronic components generate a lot of heat. If this generated heat cannot be efficiently dissipated, the heat will affect the function of the electronic components and cause the device to malfunction. To prevent this malfunction, the board on which the electronic components are mounted is equipped with a metal plate with high thermal conductivity, sandwiched between an insulating and thermally conductive resin sheet, on the side opposite the side on which the electronic components are mounted. This metal plate allows the heat generated by the electronic components to be efficiently dissipated through the resin sheet.
• Patent Document 1 discloses a metal base substrate that is composed of a metal plate, an insulating adhesive layer laminated thereon, and copper foil that is further laminated on the insulating adhesive layer.
• Patent Document 1 also discloses an adhesive composition that can be used as an insulating adhesive layer, the adhesive composition containing an epoxy resin, a curing agent, a high molecular weight resin that is compatible with the epoxy resin and has a weight average molecular weight of 30,000 or more, a high molecular weight resin that has a glass transition temperature of 0°C or less, has a reactive functional group, and has a weight average molecular weight of 100,000 or more, a curing accelerator, and an inorganic filler with a small particle size.
• Such metal base substrates may have poor heat cycle characteristics. Specifically, when a heat cycle test is performed on a metal base substrate in which electronic components are placed on a circuit formed by etching copper foil, the metal plate that constitutes the metal base substrate expands and contracts repeatedly due to temperature changes. This repeated expansion and contraction generates stress inside the insulating adhesive layer laminated on the metal plate. However, since this insulating adhesive layer cannot relieve this stress, the circuit moves in accordance with the expansion and contraction of the metal plate. As the circuit moves, stress is concentrated in the solder that connects the electronic components and the circuit, and cracks are likely to occur in the solder. For this reason, the heat cycle characteristics of the above-mentioned metal base substrate may be poor. Furthermore, since the particle size of the inorganic filler contained in the insulating adhesive layer is small, resin is likely to be interposed between the fillers, and the thermal conductivity of the insulating adhesive layer is low.
• the present invention has been made in consideration of the above circumstances, and aims to provide a heat sink having excellent heat cycle characteristics, a resin sheet having excellent thermal conductivity, a thermosetting resin composition constituting the resin layer and resin sheet of the heat sink, a method for manufacturing the resin sheet, and a method for manufacturing the heat sink.
• the thermosetting resin composition according to the present invention comprises: Epoxy resin, A curing agent for curing the epoxy resin; an ethylene-acrylic copolymer having a glass transition temperature of ⁇ 30° C. or lower and having a carboxy group in a side chain; A first spherical filler having a thermal conductivity of 20 W/m ⁇ K or more and an average particle size (D50) of 30 ⁇ m or more and 60 ⁇ m or less; A second spherical filler having a thermal conductivity of 20 W/m ⁇ K or more and an average particle diameter (D50) of 1 ⁇ m or more and 10 ⁇ m or less, The total weight ratio of the first spherical filler and the second spherical filler is 84% by weight or more and 90% by weight or less with respect to 100% by weight of the total solid content, The ratio of the first spherical filler to the second spherical filler is 55:45 to 85:15; The content of the
• the first spherical filler may be composed of at least one selected from the group consisting of alumina, boron nitride, aluminum nitride, magnesium oxide, zinc oxide, and silicon nitride.
• the second spherical filler may be composed of at least one selected from the group consisting of alumina, boron nitride, aluminum nitride, magnesium oxide, zinc oxide, and silicon nitride.
• thermosetting resin composition comprises: An ion trapping agent that traps ions is included,
• the content of the ion scavenger may be 40 parts by weight or more and 60 parts by weight or less with respect to 100 parts by weight of the epoxy resin.
• thermosetting resin composition comprises:
• the thermal conductivity after curing may be 2 W/m K or more
• the storage modulus after curing at -30°C may be 7000 MPa or less
• the storage modulus after curing at 25°C may be 10 MPa or more and 100 MPa or less
• the storage modulus after curing at 125°C may be 1 MPa or more and 100 MPa or less.
• the resin sheet according to the present invention is composed of the thermosetting resin composition described in any one of [1] to [5].
• the cured state of the resin sheet may be a semi-cured state.
• the heat sink according to the present invention is A metal plate; A resin layer composed of the thermosetting resin composition according to any one of [1] to [5], The resin layer is formed on at least one surface of the metal plate.
• the cured state of the resin layer may be a semi-cured state.
• a method for producing a resin sheet according to the present invention comprises the steps of: A preparation step of preparing a thermosetting resin composition according to any one of [1] to [5]; forming a resin layer composed of the thermosetting resin composition into a film; and a heating step of heating the film on which the resin layer is formed.
• a method for manufacturing a heat sink according to the present invention comprises: A lamination step of laminating a resin layer of the resin sheet obtained by the method for producing a resin sheet according to [10] onto a metal plate; and a heating and pressing step of heating and pressing the metal plate on which the resin layer is laminated.
• a method for manufacturing a heat sink according to the present invention comprises the steps of: A preparation step of preparing a thermosetting resin composition according to any one of [1] to [5]; A forming step of forming a resin layer composed of the thermosetting resin composition on a metal plate; and a heating step of heating the metal plate on which the resin layer is formed.
• the present invention provides a heat sink having excellent heat cycle characteristics, a resin sheet having excellent thermal conductivity, a thermosetting resin composition constituting the resin layer and resin sheet of the heat sink, a method for manufacturing the resin sheet, and a method for manufacturing the heat sink.
• 1 is a schematic cross-sectional view of a resin sheet according to an embodiment.
• 1 is a schematic cross-sectional view of a heat sink according to an embodiment.
• 1 is a schematic cross-sectional view of a substrate having an electronic component mounted thereon and a heat sink according to an embodiment;
• thermosetting resin composition resin sheet, heat sink, method for manufacturing the resin sheet, and method for manufacturing the heat sink, which are modes for carrying out the present invention (hereinafter referred to as embodiments).
• the following embodiments are examples for explaining the present invention, and are not intended to limit the present invention to the following content.
• the present invention can be practiced with appropriate modifications within the scope of its gist.
• the parts by weight used in the embodiments refer to, for example, the weight of the resin alone excluding volatile components such as organic solvents contained in the resin, and the weight of the non-volatile components.
• the semi-cured state (B stage) refers to a state in which the curing reaction of the thermosetting resin composition has progressed halfway.
• thermosetting resin composition includes an epoxy resin, a curing agent, an ethylene acrylic copolymer having a carboxy group in a side chain, a first spherical filler, and a second spherical filler.
• the thermosetting resin composition of the embodiment is suitably used as a resin composition constituting a resin sheet and a resin composition for a resin layer constituting a heat sink.
• thermosetting resin composition of the embodiment The components contained in the thermosetting resin composition of the embodiment are described below.
• the epoxy resin may be any resin capable of reacting with a curing agent to cure the thermosetting resin composition, and may, for example, have two or more epoxy groups in one molecule and an epoxy equivalent of 100 g/eq or more and 400 g/eq or less.
• epoxy resins examples include bisphenol A type epoxy resins, bisphenol F type epoxy resins, bisphenol S type epoxy resins, novolac type epoxy resins, amine type epoxy resins, biphenyl type epoxy resins, alicyclic epoxy resins, phenol novolac type epoxy resins, cresol novolac type epoxy resins, naphthalene ring-containing epoxy resins, dicyclopentadiene type epoxy resins, etc.
• epoxy resins from the viewpoint of improving the dielectric breakdown voltage characteristics, for example, novolac type epoxy resins, phenol novolac type epoxy resins, cresol novolac type epoxy resins, and bisphenol A type epoxy resins are preferred.
• the epoxy resin may be used alone or in combination with two or more kinds of epoxy resins.
• the epoxy resin may be dissolved in an organic solvent in advance to facilitate mixing with other materials contained in the thermosetting resin composition.
• the curing agent may be any agent capable of curing the epoxy resin, and examples thereof include diaminodiphenylmethane (DDM), diaminodiphenylsulfone (DDS), diaminodiphenylether (DDE), hexamethylenediamine, dicyandiamide, phenol novolac type phenolic resin, phenol novolac type cyanate ester resin, etc. From the viewpoint of ease of control of the curing reaction, the curing agent is preferably dicyandiamide or diaminodiphenylsulfone.
• the curing agent may be used alone or in combination of two or more types.
• the content of the curing agent may be any amount that can cure the thermosetting resin composition, and is preferably 1 part by weight or more and 40 parts by weight or less, and more preferably 5 parts by weight or more and 40 parts by weight or less, per 100 parts by weight of the epoxy resin. This can improve the breakdown voltage characteristics and heat resistance of the cured thermosetting resin composition. It can also improve the heat cycle characteristics of the resin sheet and heat sink made from this resin composition.
• the equivalent weight of the curing agent should be sufficient to cure the thermosetting resin composition, and is preferably 0.1 to 0.8 equivalents relative to 1 equivalent of epoxy groups contained in the epoxy resin, more preferably 0.1 to 0.6 equivalents, and even more preferably 0.2 to 0.4 equivalents. This makes it possible to improve the breakdown voltage characteristics and heat resistance of the cured thermosetting resin composition. It also makes it possible to improve the heat cycle characteristics of a heat sink using this resin composition.
• ethylene acrylic copolymers having a carboxy group in the side chain examples include (meth)acrylic acid ester copolymers having an ethylene structure in the main chain and a carboxy group in the side chain.
• the glass transition temperature of the ethylene acrylic copolymer having a carboxy group in the side chain is ⁇ 30° C. or lower, preferably ⁇ 35° C. or lower, and more preferably ⁇ 40° C. or lower, from the viewpoint of alleviating stress generated during heat cycles.
• the (meth)acrylic acid ester copolymer means an acrylic acid ester copolymer or a methacrylic acid ester copolymer.
• the glass transition temperature can be measured by differential scanning calorimetry (DSC).
• a (meth)acrylic acid ester copolymer having a carboxy group in the side chain is composed of, for example, two or more types of monomers.
• the monomers that compose this copolymer include a (meth)acrylic acid ester monomer, a carboxy group-containing monomer, and an anhydride of a carboxy group-containing monomer.
• a (meth)acrylic acid ester monomer means an acrylic acid ester monomer or a methacrylic acid ester monomer.
• Ethylene acrylic copolymers having carboxy groups in the side chains can have an ethylene structure introduced into the main chain of the copolymer by polymerizing the above-mentioned monomers.
• introduction method include Ziegler-Natta catalyst polymerization method, metallocene catalyst polymerization method, Versipol catalyst polymerization method, and free radical polymerization method.
• Examples of (meth)acrylic acid ester monomers include (meth)acrylic acid alkyl esters such as methyl (meth)acrylate, ethyl (meth)acrylate, n-butyl (meth)acrylate, and 2-ethylhexyl (meth)acrylate; (meth)acrylic acid hydroxyalkyl esters such as hydroxyethyl (meth)acrylate; (meth)acrylic acid N,N-dimethylaminoalkyl (meth)acrylates such as N,N-dimethylaminomethyl (meth)acrylate; and epoxy group-containing (meth)acrylic acid esters such as glycidyl (meth)acrylate.
• methyl (meth)acrylate means methyl acrylate or methyl methacrylate.
• (meth)acrylic acid means acrylic acid or methacrylic acid. The same applies below.
• carboxyl group-containing monomers examples include (meth)acrylic acid, fumaric acid, and maleic acid.
• anhydrides of carboxyl group-containing monomers include anhydrides of (meth)acrylic acid, maleic acid, etc.
• the weight average molecular weight of the ethylene acrylic copolymer having a carboxy group in the side chain is, for example, 100,000 to 400,000, preferably 150,000 to 300,000, from the viewpoint of preventing stress from being generated in the resin layer of the heat sink.
• the weight average molecular weight can be measured by gel permeation chromatography (GPC) using standard polystyrene with an average molecular weight of about 500 to about 1,000,000.
• the content of the ethylene acrylic copolymer having a carboxy group in the side chain is from 700 parts by weight to 1,000 parts by weight, and preferably from 700 parts by weight to 900 parts by weight, per 100 parts by weight of epoxy resin, from the viewpoint of preventing stress from occurring in the resin layer of the heat sink and from the viewpoint of thermal conductivity.
• the content of the carboxyl group is preferably, for example, 3 mgKOH/g or more and 30 mgKOH/g or less, and more preferably 10 mgKOH/g or more and 30 mgKOH/g or less.
• the content of the carboxyl group can be measured by a titration method using a 0.1 N potassium hydroxide aqueous solution.
• the average particle diameter (D50) of the first spherical filler is 30 ⁇ m or more and 60 ⁇ m or less.
• the average particle diameter (D50) of 30 ⁇ m or more and 60 ⁇ m or less the first spherical filler is less likely to protrude from the surface of the resin layer. This improves the smoothness of the surface of the resin layer.
• a network between the first spherical fillers is easily formed, and the thermal conductivity of the resin layer is improved.
• the thermal conductivity of the first spherical filler is 20 W/m ⁇ K or more from the viewpoint of improving the thermal conductivity of the resin layer of the heat sink.
• the first spherical filler may be any filler having excellent insulating properties and thermal conductivity, and is composed of at least one type selected from the group consisting of alumina, boron nitride, aluminum nitride, magnesium oxide, zinc oxide, and silicon nitride, with alumina being more preferable.
• the average particle size (D50) refers to the particle size when the particles are counted from the smallest particle size in the volume-based particle size distribution and the cumulative total reaches 50% of the total volume.
• the particle size can be measured by dynamic light scattering.
• the average particle size (D50) of the second spherical filler is 1 ⁇ m or more and 10 ⁇ m or less, more preferably 1 ⁇ m or more and 5 ⁇ m or less.
• the second spherical filler having such an average particle size (D50) is filled so as to fill the gap between one first spherical filler and another first spherical filler. This contributes to improving the thermal conductivity of the resin layer described later.
• the thermal conductivity of the second spherical filler is 20 W / m ⁇ K or more from the viewpoint of improving the thermal conductivity of the resin layer composed of the thermosetting resin composition.
• the second spherical filler may be a filler having excellent insulating properties and thermal conductivity, and is composed of at least one selected from the group consisting of alumina, boron nitride, aluminum nitride, magnesium oxide, zinc oxide, and silicon nitride, and alumina is more preferable.
• the total weight ratio of the first spherical filler and the second spherical filler described above is 84% by weight or more and 90% by weight or less, preferably 85% by weight or more and 90% by weight or less, and more preferably 85% by weight or more and 89% by weight or less, based on 100% by weight of the total solid content contained in the thermosetting resin composition, from the viewpoint of improving thermal conductivity, heat cycle characteristics, and dielectric breakdown voltage characteristics.
• the ratio of the first spherical filler and the second spherical filler is 55:45 to 85:15, preferably 55:45 to 65:35, from the viewpoint of not generating stress in the resin layer of the heat sink.
• the resin layer composed of a thermosetting resin composition containing the above-mentioned materials and having the above-mentioned ratios and other configurations has the following effects.
• the resin layer formed from the thermosetting resin composition in which the above-mentioned materials are uniformly mixed is composed by filling the second spherical filler so as to fill the gaps between one first spherical filler and another first spherical filler. By filling the spherical filler without any gaps, a dense network of spherical fillers is formed within the resin layer. As a result, the resin layer composed of the thermosetting resin composition of this embodiment has excellent thermal conductivity.
• thermosetting resin composition of this embodiment contains an ethylene acrylic copolymer having a glass transition temperature of -30°C or less and the above-mentioned spherical filler, the generation of stress can be reduced.
• a heat sink having a resin layer composed of such a thermosetting resin composition has excellent heat cycle properties because the generation of stress can be reduced in the resin layer even when temperature changes occur.
• the first and second spherical fillers do not need to be perfect spheres, but may be fillers with a shape with minimal surface irregularities that allow stress generated inside the resin layer to escape.
• Spherical fillers also include fillers composed of polyhedrons with 12 or more sides, for example.
• the materials of the first and second spherical fillers may be the same or different.
• the thermosetting resin composition of the embodiment may contain an ion trapping agent that traps ions generated in the thermosetting resin composition.
• an ion trapping agent that traps ions generated in the thermosetting resin composition.
• the content of the ion trapping agent contained in the thermosetting resin composition is 40 parts by weight or more and 60 parts by weight or less with respect to 100 parts by weight of the epoxy resin.
• thermosetting resin composition of the embodiment may further contain other additives.
• other additives include imidazole-based curing accelerators such as 2-methylimidazole, 2-undecylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, and N-benzyl-2-methylimidazole; Lewis acid complex-based curing accelerators such as boron trifluoride monoethylamine and boron trifluoride diethylamine; curing accelerators such as polyamines and melamine resins, dispersants, softeners, heat aging inhibitors, and silane coupling agents.
• imidazole-based curing accelerators such as 2-methylimidazole, 2-undecylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, and N-benzyl-2-methylimidazole
• Lewis acid complex-based curing accelerators such as boron trifluoride monoethy
• thermosetting resin composition of the embodiment can be obtained by mixing the above-mentioned materials.
• thermosetting resin composition has excellent thermal conductivity, with a thermal conductivity of 2 W/m ⁇ K or more after curing.
• the thermosetting resin composition has a storage modulus of 7000 MPa or less at -30°C after curing, a storage modulus of 10 MPa or more and 100 MPa or less at 25°C after curing, and a storage modulus of 1 MPa or more and 100 MPa or less at 125°C after curing.
• a heat sink comprising a resin layer made of such a thermosetting resin composition and a metal plate has excellent heat cycle properties in a heat cycle test in which the heat sink is alternately and repeatedly exposed to two temperature atmospheres: a low temperature atmosphere of -20°C to -40°C, and a high temperature atmosphere of 100°C to 175°C.
• the conditions for curing the thermosetting resin composition are, for example, 160°C to 200°C for at least 1 hour.
• the thermal conductivity of the thermosetting resin composition can be measured by the laser flash method using an LFA (Laser Flash Analyzer) device.
• the storage modulus of the thermosetting resin composition can be measured by a dynamic viscoelasticity measurement method.
• a resin sheet 10 according to an embodiment is made of the thermosetting resin composition according to the embodiment and has a sheet-like shape.
• the cured state of the resin sheet 10 is a semi-cured state.
• the thickness of the resin sheet 10 is sufficient if it has adhesive properties and has excellent thermal conductivity and heat cycle characteristics when used as the resin layer of a heat sink, and is, for example, 80 ⁇ m or more and 500 ⁇ m or less.
• the resin sheet 10 is produced, for example, by the following procedure.
• a thermosetting resin composition is prepared by adding and mixing predetermined amounts of epoxy resin, a curing agent, an ethylene acrylic copolymer, a first spherical filler, and a second spherical filler into a container.
• the thermosetting resin composition is applied to a separate film, for example, using an application device, and heated. After cooling, a separate film is obtained in which a resin layer composed of the thermosetting resin composition is formed, i.e., the resin sheet 10.
• the separate film is peeled off.
• the cured state of the resin sheet 10 is a semi-cured state.
• the curing conditions are, for example, 100°C to 250°C, and 5 seconds to 30 minutes, and can be adjusted according to the thickness of the resin sheet 10.
• the thickness of the separate film used in producing the resin sheet 10 may be any thickness that is easy to handle, for example, 25 ⁇ m to 100 ⁇ m.
• the thickness of the separate film is determined according to the thickness of the resin layer.
• materials for the separate film include polyethylene, polypropylene, polyimide, polyamide, polyethylene naphthalate, and polyethylene terephthalate.
• the surface of the separate film may be subjected to a release treatment.
• treatment agents for the release treatment include silicone-based treatment agents and fluorine-based treatment agents.
• the resin sheet 10 may have a different configuration.
• An example of the resin sheet 10 having a different configuration is a double-sided resin sheet in which a resin layer is formed on both sides of a film from the viewpoint of increasing the rigidity and the electrical insulation reliability.
• Examples of the material of this film from the viewpoint of increasing the heat resistance and the rigidity of the resin sheet include polyimide, polyamide, and polyethylene naphthalate.
• the resin sheet according to the embodiment has been described above.
• the heat sink 20 of the embodiment includes a metal plate 21 and a resin layer 23 made of the thermosetting resin composition of the embodiment.
• the resin layer 23 is formed on at least one surface of the metal plate 21.
• the resin layer 23 is in a semi-cured state.
• the electronic component 40 is mounted on the substrate 30 via a circuit 31 formed on the substrate 30.
• the substrate 30 is provided on the surface of the resin layer 23 opposite to the surface on which the metal plate 21 is formed.
• the thickness of the resin layer 23 should be sufficient to maintain insulation between the substrate 30 and the metal plate 21, and is, for example, 80 ⁇ m or more and 500 ⁇ m or less, and preferably 100 ⁇ m or more and 200 ⁇ m or less.
• the metal plate 21 is preferably made of a metal with high thermal conductivity as long as it can efficiently dissipate heat generated by the electronic components 40 mounted on the substrate 30.
• metals with high thermal conductivity include copper, aluminum, and stainless steel. Among these, copper and aluminum are preferred because they are easy to process and have high thermal conductivity.
• the thickness of the metal plate 21 may be any thickness that is easy to process, and is, for example, 9 ⁇ m to 10 mm, and preferably 500 ⁇ m to 2 mm. Note that the metal plate 21 also includes metal foil.
• the metal plate 21 may have a plurality of fins 22 on the surface opposite to the surface on which the resin layer 23 is formed.
• the metal plate 21 having a plurality of fins 22 is also called a heat sink.
• the thickness of the metal plate 21 on which the multiple fins 22 are provided is, for example, 0.3 mm or more and 50 mm or less.
• the fins 22 are formed, for example, from a plate or a rod.
• the height of the fins 22 is, for example, 1 mm or more and 100 mm or less.
• the thickness of the plate-shaped fin is, for example, 0.2 mm or more and 9 mm or less, and is preferably thinner than the thickness of the metal plate 21.
• the plate-shaped fin is preferably smaller than the metal plate 21.
• the cross-sectional shape of the rod-shaped fin in a direction perpendicular to the longitudinal direction of the fin is, for example, square or circular.
• the entire surface of the fin 22 may be covered with the thermosetting resin composition of the embodiment, or only a portion of the surface of the fin 22 may be covered with the thermosetting resin composition of the embodiment.
• the heat sink 20 is produced, for example, by the following procedure.
• a metal plate 21 and a resin sheet 10 as the resin layer 23 are prepared.
• the separate film is peeled off from the resin surface of the resin sheet 10.
• the resin sheet 10 is laminated on the metal plate 21 so that the resin sheet 10 and the metal plate 21 are in contact with each other.
• the metal plate 21 on which the resin sheet 10 is laminated is heated and pressurized under conditions of, for example, 0.3 MPa to 10 MPa, 100°C to 250°C, and 5 seconds to 30 minutes.
• the heat sink 20 is obtained.
• the heating and pressurizing conditions can be adjusted according to the thickness of the resin layer 23.
• thermosetting resin composition is prepared by adding and mixing a predetermined amount of epoxy resin, a curing agent, an ethylene acrylic copolymer, a first spherical filler, and a second spherical filler into a container.
• a metal plate 21 is also prepared.
• the thermosetting resin composition is applied to the metal plate 21 using, for example, an application device, and heated.
• the metal plate 21 on which the resin layer 23 is formed, that is, the heat sink 20, is obtained.
• the heating conditions are, for example, 100° C. or higher and 250° C. or lower, and 5 seconds or higher and 30 minutes or lower. The heating conditions can be adjusted according to the thickness of the resin layer 23.
• the heat sink according to the embodiment has been described above.
• an organic solvent may be used when preparing the thermosetting resin composition of the embodiment.
• organic solvents include alcohols such as methanol and ethanol; glycols such as ethylene glycol and propylene glycol; glycol monoalkyl ethers such as ethylene glycol monomethyl ether and ethylene glycol monoethyl ether; glycol dialkyl ethers such as ethylene glycol dimethyl ether and ethylene glycol diethyl ether; alkyl esters such as methyl acetate, ethyl acetate, propyl acetate, and methyl acetoacetate; ketones such as acetone, methyl ethyl ketone, methyl isobutyl ketone, and cyclohexanone; aromatic hydrocarbons such as benzene, toluene, xylene, and ethylbenzene; aliphatic hydrocarbons such as hexane, cyclohexane, and octane
• an example of an apparatus used to form the resin layer 23 of the resin sheet 10 and the heat sink 20 of the embodiment is a coating apparatus.
• the coating apparatus include known coaters, such as a die coater and a comma coater.
• thermosetting resin compositions The following components were used as the components contained in the thermosetting resin compositions in the examples and comparative examples.
• epoxy resin (1) jER (registered trademark) 828: bisphenol A type epoxy resin, epoxy equivalent 190 g/eq, manufactured by Mitsubishi Chemical Corporation.
• VMX4017 ethylene acrylic copolymer having a carboxyl group in the side chain, glass transition temperature -41°C, manufactured by DuPont
• GLS ethylene acrylic copolymer having a carboxyl group in the side chain, glass transition temperature -24°C, manufactured by DuPont
• 1HY-3006Y an acrylic copolymer having a carboxyl group in the side chain (containing no ethylene in the main chain), having a weight average molecular weight of about 280,000 and a glass transition temperature of -53°C, manufactured by Taisei Fine Chemical Co., Ltd.
• 1HY-2002M an acrylic copolymer having a carboxy group in the side chain (not containing ethylene in the main chain), with a weight average molecular weight of about 280,000 and a glass transition temperature of -3°C, manufactured by Taisei Fine Chemical Co., Ltd.
• DAM-45 spherical alumina, average particle size (D50) 45 ⁇ m, thermal conductivity 36 W/m ⁇ K, manufactured by Denka Company
• DAM-20 spherical alumina, average particle size (D50) 20 ⁇ m, thermal conductivity 36 W / m K, manufactured by Denka Company
• DAM-10 spherical alumina, average particle size (D50) 10 ⁇ m, thermal conductivity 36 W / m K, manufactured by Denka Company
• DAM-03 spherical alumina, average particle size (D50) 3 ⁇ m, thermal conductivity 36 W / m K, manufactured by Denka Company
• AA18 non-spherical alumina, average particle size (D50) 20 ⁇ m, thermal conductivity 36 W / m K, manufactured by Sumitomo Chemical Co., Ltd.
• AS-50 non-spherical alumina, average particle size (D50) 10 ⁇ m, thermal conductivity 36 W / m K, manufactured by Showa Denko K.K.
• LS-210 non-spherical alumina, average particle size (D50) 2 ⁇ m, thermal conductivity 36 W / m ⁇ K, manufactured by Nippon Light Metal Co., Ltd.
• AO-502 spherical alumina, average particle size (D50) 0.25 ⁇ m, thermal conductivity 36 W/m ⁇ K, manufactured by Admatechs Co., Ltd.
• FAN-f50-A1 spherical aluminum nitride, average particle size (D50) 50 ⁇ m, thermal conductivity 170 W / m K, manufactured by Furukawa Electronics Co., Ltd.
• FAN-f05 polyhedral shape, aluminum nitride, average particle size (D50) 5.0 ⁇ m, thermal conductivity 170 W / m K, manufactured by Furukawa Electronics Co., Ltd.
• FB-40R spherical silica, average particle size (D50) 40 ⁇ m, thermal conductivity 1 W / m K, manufactured by Denka Company
• FB-5SDC spherical silica, average particle size (D50) 3.0 ⁇ m, thermal conductivity 1 W/m ⁇ K, manufactured by Denka Company.
• thermosetting resin composition was prepared.
• a resin sheet 10 composed of the thermosetting resin composition was also produced.
• the storage modulus of the thermosetting resin composition after curing was measured using the resin sheet 10.
• the thermal conductivity of the resin sheet 10 was also measured.
• a heat cycle test was performed on the heat sink 20 using the resin sheet 10.
• thermosetting resin composition (Preparation of Thermosetting Resin Composition) Into a container were added 100 parts by weight of jER (registered trademark) 828, 10 parts by weight of Seikacure-S, 800 parts by weight of VMX4017, 4006 parts by weight of DAM-45, 2670 parts by weight of DAM-03, and 500 parts by weight of methyl ethyl ketone as an organic solvent. These were then stirred at room temperature to obtain a thermosetting resin composition.
• jER registered trademark
• Seikacure-S 800 parts by weight of VMX4017
• VMX4017 4006 parts by weight of DAM-45, 2670 parts by weight of DAM-03
• 500 parts by weight of methyl ethyl ketone as an organic solvent.
• thermosetting resin composition was applied to the release-treated surface of a 50 ⁇ m-thick release PET (polyethylene terephthalate) film (PET5011 manufactured by Lintec Corporation) so that the thickness after pressing was 100 ⁇ m, and the film was covered with another release PET film. Then, the laminate in which the release PET film, the thermosetting resin composition, and the release PET film were laminated in this order was heated and pressed under conditions of 180 ° C., 3 MPa, and 60 minutes. After cooling, a cured resin sheet 10 having a thickness of 100 ⁇ m was obtained. The obtained cured resin sheet 10 was cut into a rectangle with a length of 30 mm and a width of 4 mm to obtain a sample for measuring the storage modulus.
• PET5011 polyethylene terephthalate
• the storage modulus was measured by dynamic viscoelasticity measurement using an RSA-G2 (manufactured by TA Instruments). Measurement conditions were temperature range -50°C to 200°C, heating rate 10°C/min, frequency 1 Hz, chuck distance 20 mm, and tensile mode.
• the storage modulus of the cured thermosetting resin composition of Example 1 was 325 MPa at -30°C, 15 MPa at 25°C, and 8 MPa at 125°C.
• thermosetting resin composition was applied to the release-treated surface of a 50 ⁇ m-thick release PET film (PET5011 manufactured by Lintec Corporation) so that the thickness after heating would be 100 ⁇ m.
• the composition was then heated at 120° C. for 10 minutes and cooled to obtain a resin sheet 10 having a release PET film on one side.
• the cured state of the resin sheet 10 was a semi-cured state (B stage).
• Thermal conductivity [W/(m ⁇ K)] ⁇ [mm 2 /s] ⁇ Cp[J/g ⁇ K] ⁇ [g/cm 3 ] ⁇ [mm 2 /s]: thermal diffusion coefficient, Cp [J / g K]: specific heat, ⁇ [g/cm 3 ]: Density.
• the evaluation criteria were as follows: Good: 2W/(m ⁇ K) or more, Poor: Less than 2W/(m ⁇ K). The samples for thermal conductivity measurement that received an evaluation result of Good had excellent thermal conductivity.
• the laser flash method was adopted to measure the temperature change on one side of a sample for measuring thermal conductivity when the other side was irradiated with pulsed light.
• the obtained measurement data was analyzed by the half-time method to obtain the thermal diffusion coefficient ( ⁇ ).
• the measurement was performed at 25°C using a NETZSCH LFA447 measuring device.
• the specific heat Cp (J/g ⁇ K) of the sample for measuring thermal conductivity was determined by differential scanning calorimetry (DSC) in accordance with JIS K7123.
• DSC differential scanning calorimetry
• a TA Instruments Q200 was used as the measuring device, and the measurement was performed under conditions of a temperature rise rate of 10° C./min and a temperature range of ⁇ 30° C. to 50° C.
• the density ( ⁇ ) was measured by the liquid immersion method using Shimadzu Corporation's AUX220 and SMK-401 as measuring instruments.
• the thermal conductivity was calculated by substituting the thermal diffusion coefficient ( ⁇ ), specific heat (Cp), and density ( ⁇ ) values obtained above into the thermal conductivity formula.
• the thermal conductivity of the resin sheet 10 of Example 1 was 2.9 W / (m K), and the evaluation was Good. It was found that the resin sheet 10 of Example 1 has excellent thermal conductivity.
• a rolled copper foil (BHY manufactured by JX Nippon Mining & Metals Corporation) having a thickness of 35 ⁇ m was prepared assuming the substrate 30 and the circuit 31.
• the rolled copper foil and the resin sheet 10 were laminated so that the rough surface of the rolled copper foil and the resin surface of the resin sheet 10 were in contact with each other.
• the aluminum foil and the resin sheet 10 were laminated so that the rough surface of the aluminum foil (soft single-sided aluminum foil manufactured by Toyo Aluminum Corporation) having a thickness of 50 ⁇ m corresponding to the metal plate 21 was in contact with the resin surface opposite to the resin surface on which the rolled copper foil was laminated, to obtain a laminate.
• the obtained laminate has a configuration in which the rolled copper foil, the resin sheet 10, and the aluminum foil are laminated in this order.
• the laminate was heated and pressed under conditions of 180° C., 5 MPa, and 60 minutes. After cooling, the laminate was cut into a rectangle of 10 mm x 50 mm.
• the resin sheet 10 was used after peeling off the release PET film.
• the laminate was placed in a container, and resin was poured in so that the entire surface of the laminate was covered with resin, and the resin was hardened by heating at 100°C for 24 hours. After cooling, the resin-covered laminate was removed from the container and polished until the end face (cross section) of the laminate was exposed. On the end face (cross section) of the polished laminate, it was possible to confirm the structure in which the rolled copper foil, resin sheet, and aluminum foil were laminated in that order. This was used as a sample for heat cycle test measurement.
• the resin used was a two-liquid epoxy adhesive (Denatite, manufactured by Nagase ChemteX Corporation). Specifically, a resin obtained by mixing the base agent (XNR5021) and hardener (XNH5021) was poured into the container containing the laminate.
• the sample for the heat cycle test was placed in a thermal shock tester (TSA-72EL-A manufactured by Espec Corp.). After placement, the temperature inside the tester was cooled to -40°C and kept at that temperature for 30 minutes, then heated to 150°C and kept at that temperature for 30 minutes. This constitutes one cycle, and 3000 cycles were performed. (evaluation) After 3000 cycles, the end face (cross section) of the laminate after polishing was observed with an optical microscope (VHX-8000, manufactured by Keyence Corporation) and evaluated according to the following criteria. Good: When the end surface (cross section) of the laminate was checked, no cracks were found in the copper foil layer. Poor: When the end face (cross section) of the laminate was examined, cracks were found in the copper foil layer. After the heat cycle test, the sample for measurement in the heat cycle test of Example 1 had no cracks and was evaluated as Good.
• the resin sheet 10 of Example 1 has excellent thermal conductivity.
• the heat sink using the resin sheet 10 of Example 1 has excellent thermal conductivity.
• the heat sink of Example 1 has excellent heat cycle characteristics.
• thermosetting resin composition was prepared in the same manner as in Example 1 except that the type and content of each component contained in the thermosetting resin composition were changed, and the resin sheet 10 was produced.
• the ratio of the first spherical filler to the second spherical filler could not be calculated, so the column "First spherical filler: Second spherical filler” was marked with "-”.
• the storage modulus of the cured thermosetting resin composition prepared in each Example and Comparative Example was measured by the same method as that measured in Example 1.
• the measurement of the thermal conductivity and the heat cycle test of the resin sheet prepared in each Example and Comparative Example were performed by the same method as the test method performed in Example 1.
• the unit of the content in the table is "parts by weight” unless otherwise specified.
• Example 1 the peel strength, dielectric breakdown voltage, and dielectric breakdown voltage after a long-term wet heat test were measured for the resin sheets 10 of Examples 1 to 15, and the adhesiveness and dielectric breakdown voltage characteristics were evaluated.
• Example 1 the peel strength, dielectric breakdown voltage, and dielectric breakdown voltage after a long-term wet heat test was measured for the resin sheets 10 of Examples 1 to 15, and the adhesiveness and dielectric breakdown voltage characteristics were evaluated.
• Example 1 describes Example 1 as an example.
• Example for measuring dielectric breakdown voltage The sample for measuring the dielectric breakdown voltage in Example 1 was prepared as follows. First, the resin sheet 10 prepared in Example 1, the rolled copper foil (BHY manufactured by JX Nippon Mining & Metals Corporation) having a thickness of 35 ⁇ m assuming the substrate 30 and the circuit 31, and the aluminum plate (A1100 manufactured by Showa Denko K.K.) having a thickness of 1 mm corresponding to the metal plate 21 were prepared. Next, the rolled copper foil and the resin sheet 10 were laminated so that the rough surface of the rolled copper foil was in contact with the resin surface of the resin sheet 10.
• the obtained laminate has a configuration in which the rolled copper foil, the resin sheet 10, and the aluminum plate are laminated in this order.
• the laminate was heated and pressed under conditions of 185° C., 5 MPa, and 180 minutes. Furthermore, the laminate was heated in an oven at 160° C. for another 5 hours, and then cooled.
• the rolled copper foil of the obtained laminate was etched to a circular shape with a diameter of 20 mm. After that, it was washed with water and dried to obtain a sample for measuring the dielectric breakdown voltage.
• the resin sheet 10 was used after removing the release PET film.
• the dielectric breakdown tester used was a B-5120AT-2 manufactured by Nippon Technart Co., Ltd. A voltage was applied between the circularly etched rolled copper foil and the aluminum plate while the sample for measuring the dielectric breakdown voltage was immersed in oil at 25°C. The voltage was increased at a rate of 1 kV/0.5 sec, and the voltage at which dielectric breakdown occurred was measured. This test was performed five times, and the average value was calculated and evaluated according to the following criteria.
• This dielectric breakdown voltage is also referred to as the dielectric breakdown voltage before the long-term wet heat test. Good: Voltage is 2 kV or more; Poor: Voltage is less than 2 kV. The dielectric breakdown voltage of Example 1 was 3.5 kV, and the evaluation was Good. It was found that the resin sheet 10 of Example 1 had excellent insulating properties.
• Example for measuring peel strength A laminate obtained in the process of producing a sample for measuring the dielectric breakdown voltage was prepared separately. The rolled copper foil of this laminate was etched so that the laminate had a width of 10 mm and a length of 100 mm. The laminate after etching was washed with water and dried to obtain a sample for measuring the peel strength of Example 1.
• the measurement device used was an autograph AGS-500 manufactured by Shimadzu Corporation.
• the rolled copper foil was peeled off in a 90° direction (perpendicular to the main surface of the sample) to measure the peel strength at the interface between the rolled copper foil and the resin sheet 10.
• the test speed was 50 mm/min.
• the test was performed twice, and the average value was calculated.
• the evaluation criteria were as follows: Good: Peel strength is 2N/cm or more; Poor: Peel strength is less than 2 N/cm.
• the peel strength of Example 1 was 10 N/cm, and the evaluation was Good.
• ⁇ Breakdown voltage after long-term damp heat test> The insulating property of the resin sheet 10 after the long-term wet heat test was evaluated by measuring the dielectric breakdown voltage of the resin sheet 10 . (Sample for measuring dielectric breakdown voltage after long-term damp heat test) The samples used in this evaluation were prepared in the same manner as the samples for measuring the dielectric breakdown voltage described above.
• the sample for measuring the dielectric breakdown voltage after the long-term wet heat test was stored under an atmosphere of 85° C. ⁇ 85% RH ⁇ 1000 hours, and then the moisture adhering to the surface of the sample was wiped off, and the dielectric breakdown voltage was measured under the same measurement conditions as those for the above-mentioned dielectric breakdown voltage.
• the evaluation criteria were as follows: Good: Voltage is 1 kV or more; Poor: Voltage is less than 1 kV.
• the dielectric breakdown voltage of Example 1 after the long-term wet heat test was 0.5 kV, and the evaluation was Poor.
• the resin sheet 10 made of the thermosetting resin composition of Example 1 had a low breakdown voltage after the long-term damp heat test, but a high breakdown voltage before the long-term damp heat test, demonstrating excellent adhesion to metal.
• the resin sheets 10 made of the thermosetting resin compositions of Examples 2 to 15 were also measured for breakdown voltage, peel strength, and breakdown voltage after the long-term damp heat test in the same manner as in Example 1, and the breakdown voltage characteristics and adhesion were evaluated. The results are shown in Table 3.
• the dielectric breakdown voltage before the long-term damp heat test the dielectric breakdown voltage after the long-term damp heat test, and the peel strength of the resin sheet 10 of Example 2, which is made of a thermosetting resin composition containing an ion scavenger, were high. This shows that the resin sheet 10 of Example 2 has excellent dielectric breakdown voltage characteristics and adhesiveness.
• the resin sheets 10 of Examples 1 to 15 have excellent thermal conductivity and adhesiveness.
• the heat sinks using the resin sheets 10 of Examples 1 to 15 have excellent thermal conductivity.
• the heat sinks 20 of Examples 1 to 15 have excellent heat cycle characteristics.
• the resin sheets 10 of Examples 2 to 6, Examples 8 to 11, Example 13, and Example 14 have excellent dielectric breakdown voltage characteristics.
• Epoxy resin A curing agent for curing the epoxy resin; an ethylene-acrylic copolymer having a glass transition temperature of ⁇ 30° C. or lower and having a carboxy group in a side chain;
• a first spherical filler having a thermal conductivity of 20 W/m ⁇ K or more and an average particle size (D50) of 30 ⁇ m or more and 60 ⁇ m or less;
• a second spherical filler having a thermal conductivity of 20 W/m ⁇ K or more and an average particle diameter (D50) of 1 ⁇ m or more and 10 ⁇ m or less,
• the total weight ratio of the first spherical filler and the second spherical filler is 84% by weight or more and 90% by weight or less with respect to 100% by weight of the total solid content,
• the ratio of the first spherical filler to the second spherical filler is 55:45 to 85:15;
• a thermosetting resin composition wherein the content of the ethylene acrylic
• thermosetting resin composition according to claim 1 wherein the first spherical filler is composed of at least one selected from the group consisting of alumina, boron nitride, aluminum nitride, magnesium oxide, zinc oxide, and silicon nitride.
• thermosetting resin composition according to claim 1 or 2 wherein the second spherical filler is composed of at least one selected from the group consisting of alumina, boron nitride, aluminum nitride, magnesium oxide, zinc oxide, and silicon nitride.
• thermosetting resin composition according to any one of Appendix 1 to Appendix 3, wherein the content of the ion scavenger is 40 parts by weight or more and 60 parts by weight or less with respect to 100 parts by weight of the epoxy resin.
• thermosetting resin composition according to any one of Appendix 1 to Appendix 4, having a thermal conductivity after curing of 2 W/m K or more, a storage modulus after curing at -30°C of 7000 MPa or less, a storage modulus after curing at 25°C of 10 MPa or more and 100 MPa or less, and a storage modulus after curing at 125°C of 1 MPa or more and 100 MPa or less.
• a metal plate A resin layer composed of the thermosetting resin composition according to any one of Supplementary Note 1 to Supplementary Note 5, The resin layer is formed on at least one surface of the metal plate.
• thermosetting resin composition (Appendix 10) A preparation step of preparing a thermosetting resin composition according to any one of Supplementary Note 1 to Supplementary Note 5; forming a resin layer composed of the thermosetting resin composition into a film; and a heating step of heating the film on which the resin layer is formed.
• thermosetting resin composition A preparation step of preparing a thermosetting resin composition according to any one of Supplementary Note 1 to Supplementary Note 5; A forming step of forming a resin layer composed of the thermosetting resin composition on a metal plate; and a heating step of heating the metal plate on which the resin layer is formed.

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