JPWO2019026745A1 - Thermally conductive resin molded product - Google Patents
Thermally conductive resin molded product Download PDFInfo
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- JPWO2019026745A1 JPWO2019026745A1 JP2018540879A JP2018540879A JPWO2019026745A1 JP WO2019026745 A1 JPWO2019026745 A1 JP WO2019026745A1 JP 2018540879 A JP2018540879 A JP 2018540879A JP 2018540879 A JP2018540879 A JP 2018540879A JP WO2019026745 A1 JPWO2019026745 A1 JP WO2019026745A1
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- thermally conductive
- conductive filler
- filler
- heat
- sheet
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- 229920005989 resin Polymers 0.000 title claims abstract description 68
- 239000011347 resin Substances 0.000 title claims abstract description 68
- 239000011231 conductive filler Substances 0.000 claims abstract description 150
- 239000002245 particle Substances 0.000 claims abstract description 41
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 claims abstract description 23
- 239000000945 filler Substances 0.000 claims abstract description 23
- 229910052582 BN Inorganic materials 0.000 claims abstract description 22
- 239000000463 material Substances 0.000 claims abstract description 14
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 claims description 8
- 239000001095 magnesium carbonate Substances 0.000 claims description 8
- 229910000021 magnesium carbonate Inorganic materials 0.000 claims description 8
- 239000000395 magnesium oxide Substances 0.000 claims description 8
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 8
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 claims description 8
- -1 polyethylene Polymers 0.000 description 19
- 239000002994 raw material Substances 0.000 description 18
- 238000004132 cross linking Methods 0.000 description 17
- 239000002243 precursor Substances 0.000 description 13
- 239000000203 mixture Substances 0.000 description 11
- 229920001296 polysiloxane Polymers 0.000 description 10
- 238000002156 mixing Methods 0.000 description 9
- 238000004519 manufacturing process Methods 0.000 description 8
- 239000011159 matrix material Substances 0.000 description 8
- 238000000034 method Methods 0.000 description 7
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 6
- 229920000642 polymer Polymers 0.000 description 6
- 229920002379 silicone rubber Polymers 0.000 description 6
- 239000004945 silicone rubber Substances 0.000 description 6
- 229920001577 copolymer Polymers 0.000 description 5
- 238000001125 extrusion Methods 0.000 description 5
- 229920002725 thermoplastic elastomer Polymers 0.000 description 5
- 239000003431 cross linking reagent Substances 0.000 description 4
- 229920001971 elastomer Polymers 0.000 description 4
- 150000002978 peroxides Chemical class 0.000 description 4
- 239000005060 rubber Substances 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 229910000019 calcium carbonate Inorganic materials 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 3
- 229920000459 Nitrile rubber Polymers 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 2
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 2
- 230000001133 acceleration Effects 0.000 description 2
- 229920000122 acrylonitrile butadiene styrene Polymers 0.000 description 2
- 239000002041 carbon nanotube Substances 0.000 description 2
- 229910021393 carbon nanotube Inorganic materials 0.000 description 2
- 238000005520 cutting process Methods 0.000 description 2
- 239000004205 dimethyl polysiloxane Substances 0.000 description 2
- 235000013870 dimethyl polysiloxane Nutrition 0.000 description 2
- 150000002148 esters Chemical class 0.000 description 2
- 238000005187 foaming Methods 0.000 description 2
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 2
- 238000000465 moulding Methods 0.000 description 2
- 239000004014 plasticizer Substances 0.000 description 2
- 229920000435 poly(dimethylsiloxane) Polymers 0.000 description 2
- 229920001955 polyphenylene ether Polymers 0.000 description 2
- DMWVYCCGCQPJEA-UHFFFAOYSA-N 2,5-bis(tert-butylperoxy)-2,5-dimethylhexane Chemical compound CC(C)(C)OOC(C)(C)CCC(C)(C)OOC(C)(C)C DMWVYCCGCQPJEA-UHFFFAOYSA-N 0.000 description 1
- XMNIXWIUMCBBBL-UHFFFAOYSA-N 2-(2-phenylpropan-2-ylperoxy)propan-2-ylbenzene Chemical compound C=1C=CC=CC=1C(C)(C)OOC(C)(C)C1=CC=CC=C1 XMNIXWIUMCBBBL-UHFFFAOYSA-N 0.000 description 1
- 239000004953 Aliphatic polyamide Substances 0.000 description 1
- 239000004342 Benzoyl peroxide Substances 0.000 description 1
- OMPJBNCRMGITSC-UHFFFAOYSA-N Benzoylperoxide Chemical compound C=1C=CC=CC=1C(=O)OOC(=O)C1=CC=CC=C1 OMPJBNCRMGITSC-UHFFFAOYSA-N 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229920000089 Cyclic olefin copolymer Polymers 0.000 description 1
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 1
- 229920000106 Liquid crystal polymer Polymers 0.000 description 1
- 239000004977 Liquid-crystal polymers (LCPs) Substances 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 229920002845 Poly(methacrylic acid) Polymers 0.000 description 1
- 229930182556 Polyacetal Natural products 0.000 description 1
- 239000004962 Polyamide-imide Substances 0.000 description 1
- 239000004695 Polyether sulfone Substances 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- 239000004721 Polyphenylene oxide Substances 0.000 description 1
- 239000004734 Polyphenylene sulfide Substances 0.000 description 1
- 239000004793 Polystyrene Substances 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- 229920001328 Polyvinylidene chloride Polymers 0.000 description 1
- 229920002125 Sokalan® Polymers 0.000 description 1
- BZHJMEDXRYGGRV-UHFFFAOYSA-N Vinyl chloride Chemical compound ClC=C BZHJMEDXRYGGRV-UHFFFAOYSA-N 0.000 description 1
- 229920000800 acrylic rubber Polymers 0.000 description 1
- XECAHXYUAAWDEL-UHFFFAOYSA-N acrylonitrile butadiene styrene Chemical compound C=CC=C.C=CC#N.C=CC1=CC=CC=C1 XECAHXYUAAWDEL-UHFFFAOYSA-N 0.000 description 1
- 239000004676 acrylonitrile butadiene styrene Substances 0.000 description 1
- 238000007259 addition reaction Methods 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 239000000853 adhesive Substances 0.000 description 1
- 230000001070 adhesive effect Effects 0.000 description 1
- 229920003231 aliphatic polyamide Polymers 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 230000003712 anti-aging effect Effects 0.000 description 1
- 239000002216 antistatic agent Substances 0.000 description 1
- 239000004760 aramid Substances 0.000 description 1
- 229920003235 aromatic polyamide Polymers 0.000 description 1
- 235000019400 benzoyl peroxide Nutrition 0.000 description 1
- 229920005549 butyl rubber Polymers 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- PMHQVHHXPFUNSP-UHFFFAOYSA-M copper(1+);methylsulfanylmethane;bromide Chemical compound Br[Cu].CSC PMHQVHHXPFUNSP-UHFFFAOYSA-M 0.000 description 1
- 239000007822 coupling agent Substances 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000005038 ethylene vinyl acetate Substances 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 239000003063 flame retardant Substances 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229920000554 ionomer Polymers 0.000 description 1
- 238000004898 kneading Methods 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 239000010445 mica Substances 0.000 description 1
- 229910052618 mica group Inorganic materials 0.000 description 1
- CWQXQMHSOZUFJS-UHFFFAOYSA-N molybdenum disulfide Chemical compound S=[Mo]=S CWQXQMHSOZUFJS-UHFFFAOYSA-N 0.000 description 1
- 229910052982 molybdenum disulfide Inorganic materials 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 1
- 150000001451 organic peroxides Chemical class 0.000 description 1
- 229920003023 plastic Polymers 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
- 229920001643 poly(ether ketone) Polymers 0.000 description 1
- 229920003207 poly(ethylene-2,6-naphthalate) Polymers 0.000 description 1
- 229920001200 poly(ethylene-vinyl acetate) Polymers 0.000 description 1
- 229920002285 poly(styrene-co-acrylonitrile) Polymers 0.000 description 1
- 229920002492 poly(sulfone) Polymers 0.000 description 1
- 229920000058 polyacrylate Polymers 0.000 description 1
- 239000004584 polyacrylic acid Substances 0.000 description 1
- 229920002239 polyacrylonitrile Polymers 0.000 description 1
- 229920002312 polyamide-imide Polymers 0.000 description 1
- 229920001707 polybutylene terephthalate Polymers 0.000 description 1
- 239000004417 polycarbonate Substances 0.000 description 1
- 229920000515 polycarbonate Polymers 0.000 description 1
- 229920000728 polyester Polymers 0.000 description 1
- 229920000570 polyether Polymers 0.000 description 1
- 229920006393 polyether sulfone Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 239000011112 polyethylene naphthalate Substances 0.000 description 1
- 229920000139 polyethylene terephthalate Polymers 0.000 description 1
- 239000005020 polyethylene terephthalate Substances 0.000 description 1
- 229920001470 polyketone Polymers 0.000 description 1
- 229920000306 polymethylpentene Polymers 0.000 description 1
- 239000011116 polymethylpentene Substances 0.000 description 1
- 229920006324 polyoxymethylene Polymers 0.000 description 1
- 229920000069 polyphenylene sulfide Polymers 0.000 description 1
- 229920002223 polystyrene Polymers 0.000 description 1
- 229920000346 polystyrene-polyisoprene block-polystyrene Polymers 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 229920002635 polyurethane Polymers 0.000 description 1
- 239000004814 polyurethane Substances 0.000 description 1
- 229920002689 polyvinyl acetate Polymers 0.000 description 1
- 239000011118 polyvinyl acetate Substances 0.000 description 1
- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 229920000915 polyvinyl chloride Polymers 0.000 description 1
- 239000004800 polyvinyl chloride Substances 0.000 description 1
- 239000005033 polyvinylidene chloride Substances 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 230000002250 progressing effect Effects 0.000 description 1
- 239000012744 reinforcing agent Substances 0.000 description 1
- 238000000790 scattering method Methods 0.000 description 1
- 238000010008 shearing Methods 0.000 description 1
- SCPYDCQAZCOKTP-UHFFFAOYSA-N silanol Chemical group [SiH3]O SCPYDCQAZCOKTP-UHFFFAOYSA-N 0.000 description 1
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 229920002545 silicone oil Polymers 0.000 description 1
- 229920002050 silicone resin Polymers 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000003746 surface roughness Effects 0.000 description 1
- GJBRNHKUVLOCEB-UHFFFAOYSA-N tert-butyl benzenecarboperoxoate Chemical compound CC(C)(C)OOC(=O)C1=CC=CC=C1 GJBRNHKUVLOCEB-UHFFFAOYSA-N 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 229920001169 thermoplastic Polymers 0.000 description 1
- 229920006345 thermoplastic polyamide Polymers 0.000 description 1
- 239000004416 thermosoftening plastic Substances 0.000 description 1
- 238000011144 upstream manufacturing Methods 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
- 239000004711 α-olefin Substances 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L83/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon only; Compositions of derivatives of such polymers
- C08L83/04—Polysiloxanes
-
- 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
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B27/08—Layered products comprising a layer of synthetic resin 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
- B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
- B32B7/02—Physical, chemical or physicochemical properties
-
- 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
- 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
- C08K3/24—Acids; Salts thereof
- C08K3/26—Carbonates; Bicarbonates
-
- 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
- C08K3/38—Boron-containing compounds
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L101/00—Compositions of unspecified macromolecular compounds
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K7/00—Constructional details common to different types of electric apparatus
- H05K7/20—Modifications to facilitate cooling, ventilating, or heating
-
- 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
- C08G77/00—Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule
- C08G77/04—Polysiloxanes
- C08G77/20—Polysiloxanes containing silicon bound to unsaturated aliphatic groups
-
- 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
- C08K3/24—Acids; Salts thereof
- C08K3/26—Carbonates; Bicarbonates
- C08K2003/267—Magnesium carbonate
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- Chemical & Material Sciences (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Engineering & Computer Science (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Compositions Of Macromolecular Compounds (AREA)
- Cooling Or The Like Of Semiconductors Or Solid State Devices (AREA)
Abstract
樹脂と、第1熱伝導性フィラー及び前記第1熱伝導性フィラーより小さい粒径を有する第2熱伝導性フィラーを含む熱伝導性フィラーと、を含む熱伝導性樹脂成型品であって、前記熱伝導性フィラーの含有量は、30〜50体積%であり、前記第1熱伝導性フィラーは、30μm以上の粒径及び10以上のアスペクト比を有する窒化ホウ素からなるフィラーであり、前記第1熱伝導性フィラーの含有量は、5〜20体積%であり、前記第2熱伝導性フィラーは、窒化ホウ素以外の材質からなるフィラーである、熱伝導性樹脂成型品。A thermally conductive resin molded article comprising a resin and a thermally conductive filler comprising a first thermally conductive filler and a second thermally conductive filler having a particle size smaller than the first thermally conductive filler, The content of the thermally conductive filler is 30 to 50% by volume, and the first thermally conductive filler is a filler made of boron nitride having a particle size of 30 μm or more and an aspect ratio of 10 or more, and the first The content of the heat conductive filler is 5 to 20% by volume, and the second heat conductive filler is a filler made of a material other than boron nitride.
Description
本発明は、熱伝導性樹脂成型品に関する。 The present invention relates to a thermally conductive resin molded product.
近年、電子機器の高密度化・薄型化が急速に進み、ICやパワー部品、高輝度LEDから発生する熱の影響が重大な問題となっている。これに対して、例えば、チップ等の発熱体と放熱体の間の熱を効率よく伝達する部材として、シート状の熱伝導性樹脂成型品の利用が進んでいる。
ここで、樹脂成型品に高い熱伝導性を付与する手段として、効率よく熱伝導パスを形成するために、熱伝導性フィラーを配向させて樹脂中に分散させることが知られている。In recent years, electronic devices have rapidly become denser and thinner, and the influence of heat generated from ICs, power components, and high-brightness LEDs has become a serious problem. On the other hand, for example, as a member for efficiently transferring heat between a heat generating body such as a chip and a heat radiating body, use of a sheet-like thermally conductive resin molded product is progressing.
Here, as a means for imparting high thermal conductivity to a resin molded product, in order to efficiently form a thermal conduction path, it is known that a thermal conductive filler is oriented and dispersed in the resin.
特許文献1には、樹脂及び/又はゴムと窒化ホウ素の鱗片状粒子を含む混練物を複数の帯状可塑物に押出成型しながらそれらをリップで集成しシート化した後硬化させるか、又はシート化しながら硬化させる製造方法が提案されている。
特許文献2には、熱伝導性成形体として、平均粒子径の異なる2種類の窒化ホウ素粉末(A)及び(B)を含む熱伝導性フィラーを50〜75体積%含有してなるシリコーン積層体を、積層方向から切断することを特徴とする熱伝導性成形体が提案されている。Patent Document 1 discloses that a kneaded product containing resin and / or rubber and boron nitride scaly particles is extruded into a plurality of strip-shaped plastics, and these are assembled with a lip to form a sheet and then cured or sheeted. However, a production method for curing the resin has been proposed.
Patent Document 2 discloses a silicone laminate comprising 50 to 75% by volume of a thermally conductive filler containing two types of boron nitride powders (A) and (B) having different average particle diameters as a thermally conductive molded body. Has been proposed that is cut from the stacking direction.
上記特許文献1、2に記載されている熱伝導性を有する樹脂成型品は、熱伝導性フィラーとして、窒化ホウ素製のフィラーを好ましく採用している。窒化ホウ素製のフィラーは優れた熱伝導性を付与させやすいという利点を有する。しかしながら、窒化ホウ素は高価であり、上記特許文献1、2のように窒化ホウ素製のフィラーを多量に含有する場合、熱伝導性を有する樹脂成型品を安価に提供することが困難であった。
一方、熱伝導性フィラーとして窒化ホウ素製のフィラーのみを用いる場合、フィラーの含有量が少ないと、このフィラーを配向させることが困難となる。その結果、作製した樹脂成型品は、窒化ホウ素製のフィラーを使用しているにも関わらず、熱伝導性に劣るという課題があった。The resin molded product having thermal conductivity described in Patent Documents 1 and 2 preferably employs a boron nitride filler as the thermal conductive filler. Boron nitride filler has the advantage of easily imparting excellent thermal conductivity. However, boron nitride is expensive, and when a large amount of boron nitride filler is contained as in Patent Documents 1 and 2, it is difficult to provide a resin molded product having thermal conductivity at low cost.
On the other hand, when only a boron nitride filler is used as the thermally conductive filler, it is difficult to orient the filler if the filler content is low. As a result, the produced resin molded product has a problem that it is inferior in thermal conductivity even though a boron nitride filler is used.
本発明は、このような課題に鑑みてなされたものであり、優れた熱伝導性を有し、安価に製造することができる熱伝導性樹脂成型品を提供することを目的する。 This invention is made | formed in view of such a subject, and it aims at providing the heat conductive resin molded product which has the outstanding heat conductivity and can be manufactured cheaply.
(1)本発明の熱伝導性樹脂成型品は、
樹脂と、第1熱伝導性フィラー及び上記第1熱伝導性フィラーより小さい粒径を有する第2熱伝導性フィラーを含む熱伝導性フィラーと、を含む熱伝導性樹脂成型品であって、
上記熱伝導性フィラーの含有量は、30〜50体積%であり、
上記第1熱伝導性フィラーは、30μm以上の粒径及び10以上のアスペクト比を有する窒化ホウ素からなるフィラーであり、
上記第1熱伝導性フィラーの含有量は、5〜20体積%であり、
上記第2熱伝導性フィラーは、窒化ホウ素以外の材質からなるフィラーである
ことを特徴とする。(1) The thermally conductive resin molded product of the present invention is
A thermally conductive resin molded article comprising a resin and a thermally conductive filler comprising a first thermally conductive filler and a second thermally conductive filler having a particle size smaller than the first thermally conductive filler,
Content of the said heat conductive filler is 30-50 volume%,
The first thermally conductive filler is a filler made of boron nitride having a particle size of 30 μm or more and an aspect ratio of 10 or more,
The content of the first thermally conductive filler is 5 to 20% by volume,
The second thermally conductive filler is a filler made of a material other than boron nitride.
本発明の熱伝導性樹脂成型品は、熱伝導性フィラーの総含有量の上限を50体積%に抑えつつ、窒化ホウ素からなる第1熱伝導性フィラーと、窒化ホウ素以外の材質からなり、粒径が第1熱伝導性フィラーよりも小さい第2熱伝導性フィラーとをそれぞれ所定量含有している。
そのため、上記熱伝導性樹脂成型品によれば、窒化ホウ素からなる第1熱伝導性フィラーの含有量が少なくても上記第1熱伝導性フィラーを配向させることができ、上記熱伝導性樹脂成型品は、熱伝導性に優れる。
また、上記熱伝導性樹脂成型品は、安価に提供することができる。The thermally conductive resin molded article of the present invention is composed of a first thermally conductive filler made of boron nitride and a material other than boron nitride while suppressing the upper limit of the total content of the thermally conductive filler to 50% by volume. A predetermined amount of a second thermally conductive filler having a diameter smaller than that of the first thermally conductive filler is contained.
Therefore, according to the thermally conductive resin molded product, the first thermally conductive filler can be oriented even if the content of the first thermally conductive filler made of boron nitride is small. The product has excellent thermal conductivity.
Moreover, the said heat conductive resin molded product can be provided in low cost.
(2)上記熱伝導性樹脂成型品において、上記第2熱伝導性フィラーの粒径は、3〜20μmであることが好ましい。
この場合、上記第2熱伝導性フィラーは、第1熱伝導性フィラー同士の間に介在して上記熱伝導性樹脂成型品の熱伝導性を高めるのに適しており、かつ熱伝導性樹脂成型品の製造工程において、第1熱伝導性フィラーを配向させるのにも適している。(2) In the thermally conductive resin molded product, the particle size of the second thermally conductive filler is preferably 3 to 20 μm.
In this case, the second thermally conductive filler is suitable for increasing the thermal conductivity of the thermally conductive resin molded product by being interposed between the first thermally conductive fillers, and the thermally conductive resin molded product. It is also suitable for orienting the first thermally conductive filler in the product manufacturing process.
(3)上記熱伝導性樹脂成型品において、上記第2熱伝導性フィラーは、酸化マグネシウム又は炭酸マグネシウムからなることが好ましい。
この場合、上記第2熱伝導性フィラーは、第1熱伝導性フィラー同士の間に介在して上記熱伝導性樹脂成型品の熱伝導性を高めるのに適しており、かつ熱伝導性樹脂成型品を安価で提供するのに適している。(3) In the thermally conductive resin molded product, the second thermally conductive filler is preferably made of magnesium oxide or magnesium carbonate.
In this case, the second thermally conductive filler is suitable for increasing the thermal conductivity of the thermally conductive resin molded product by being interposed between the first thermally conductive fillers, and the thermally conductive resin molded product. Suitable for providing goods at low cost.
本発明の熱伝導性樹脂成型品は、優れた熱伝導性を有する。
また、上記熱伝導性樹脂成型品は、安価に提供することができる。The thermally conductive resin molded product of the present invention has excellent thermal conductivity.
Moreover, the said heat conductive resin molded product can be provided in low cost.
以下、本発明の実施形態について説明する。
本発明において、「熱伝導性樹脂成型品」とは、原料組成物を成型して作製したブロック状物、及び、当該ブロック状物を切断して得られた切断物(スライスしたシート状物を含む)のいずれも含む概念である。
本実施形態では、熱伝導性シートを例にして、熱伝導性樹脂成型品の実施形態を説明する。Hereinafter, embodiments of the present invention will be described.
In the present invention, the “thermally conductive resin molded product” means a block-like product produced by molding a raw material composition, and a cut product (sliced sheet-like product obtained by cutting the block-like product). It is a concept that includes all of
In the present embodiment, an embodiment of a thermally conductive resin molded product will be described using a thermally conductive sheet as an example.
図1は、本発明の実施形態に係る熱伝導性シートを模式的に示す断面図であり、上記熱伝導性シートの厚さ方向に平行な断面図である。なお、図1は模式図であり、各部材(特に第1熱伝導性フィラー及び第2熱伝導性フィラー)は、実寸法を正確に反映したものではない。
本実施形態に係る熱伝導性シート1は、ICチップ等の発熱部材とヒートシンク等の放熱部材との間に配置し、一方の面を発熱部材に接触させ、他方の面を放熱部材に接触させて使用する。FIG. 1 is a cross-sectional view schematically showing a heat conductive sheet according to an embodiment of the present invention, which is a cross-sectional view parallel to the thickness direction of the heat conductive sheet. In addition, FIG. 1 is a schematic diagram, and each member (especially 1st heat conductive filler and 2nd heat conductive filler) does not reflect an actual dimension correctly.
The heat conductive sheet 1 according to the present embodiment is disposed between a heat generating member such as an IC chip and a heat radiating member such as a heat sink, and has one surface in contact with the heat generating member and the other surface in contact with the heat radiating member. To use.
熱伝導性シート1は、図1に示すように、マトリックス成分2と、第1熱伝導性フィラー4及び第2熱伝導性フィラー5とを有しており、第1熱伝導性フィラー4が熱伝導性シート1の略厚さ方向(図1中、上下方向)に配向している。熱伝導性シート1では、第1熱伝導性フィラー4及び第2熱伝導性フィラー5による熱伝導パスが、熱伝導性シート1の略厚さ方向に形成されている。従って、熱伝導性シート1は厚さ方向における熱伝導性に優れる。
なお、上記熱伝導性シートでは、熱伝導性フィラー以外の成分をまとめてマトリックス成分と称する。As shown in FIG. 1, the heat conductive sheet 1 has a matrix component 2, a first heat conductive filler 4 and a second heat conductive filler 5, and the first heat conductive filler 4 is heated. The conductive sheet 1 is oriented substantially in the thickness direction (vertical direction in FIG. 1). In the heat conductive sheet 1, a heat conductive path by the first heat conductive filler 4 and the second heat conductive filler 5 is formed in a substantially thickness direction of the heat conductive sheet 1. Therefore, the heat conductive sheet 1 is excellent in heat conductivity in the thickness direction.
In addition, in the said heat conductive sheet, components other than a heat conductive filler are collectively called a matrix component.
熱伝導性シート1は、マトリックス成分2中の第1熱伝導性フィラー4がその面方向に配向分散した薄い樹脂シートが垂直方向に折り畳んだ状態で密着されたブロック状物をシート状にスライスしたものである。このような熱伝導性シート1には略厚さ方向にウェルドライン6が形成される場合もある。 The thermally conductive sheet 1 is obtained by slicing a block-like material in which a thin resin sheet in which the first thermally conductive filler 4 in the matrix component 2 is oriented and dispersed in the plane direction is folded in the vertical direction into a sheet shape. Is. Such a heat conductive sheet 1 may have a weld line 6 formed substantially in the thickness direction.
マトリックス成分2は、少なくとも樹脂(ゴムを含む)を含有する。
上記樹脂としては、従来公知の種々の樹脂を適宜選択して用いることができる。
具体的には、例えば、ポリエチレン、ポリプロピレン、エチレン−プロピレン共重合体等のエチレン−α−オレフィン共重合体、ポリメチルペンテン、ポリ塩化ビニル、ポリ塩化ビニリデン、ポリ酢酸ビニル、エチレン−酢酸ビニル共重合体、ポリビニルアルコール、ポリアセタール、ポリフッ化ビニリデンやポリテトラフルオロエチレン等のフッ素系樹脂、ポリエチレンテレフタレート、ポリブチレンテレフタレート、ポリエチレンナフタレート、ポリスチレン、ポリアクリロニトリル、スチレン−アクリロニトリル共重合体、アクリロニトリル−ブタジエン−スチレン共重合体(ABS)樹脂、ポリフェニレンエーテル、変性ポリフェニレンエーテル、脂肪族ポリアミド類、芳香族ポリアミド類、ポリアミドイミド、ポリメタクリル酸又はそのエステル、ポリアクリル酸又はそのエステル、ポリカーボネート、ポリフェニレンスルフィド、ポリサルホン、ポリエーテルサルホン、ポリエーテルニトリル、ポリエーテルケトン、ポリケトン、液晶ポリマー、シリコーン樹脂、アイオノマーなどを用いることができる。
また、例えば、スチレン−ブタジエン共重合体又はその水添ポリマー、スチレン−イソプレンブロック共重合体又はその水添ポリマー等のスチレン系熱可塑性エラストマー、オレフィン系熱可塑性エラストマー、塩化ビニル系熱可塑性エラストマー、ポリエステル系熱可塑性エラストマー、ポリウレタン系熱可塑性エラストマー、ポリアミド系熱可塑性エラストマーなどを用いることができる。
更には、例えば、シリコーンゴム、アクリルゴム、ブチルゴム、フッ素ゴム、ニトリルゴム、水素化ニトリルゴム等を用いることもできる。
これらは単独で用いても良いし、2種以上を併用しても良い。
これらのなかでは、成型体とした際の柔軟性、形状追従性、電子部品に接触させる際の発熱面への密着性、及び、耐熱性に優れる点からシリコーンゴムが好ましい。The matrix component 2 contains at least a resin (including rubber).
As the resin, various conventionally known resins can be appropriately selected and used.
Specifically, for example, ethylene-α-olefin copolymers such as polyethylene, polypropylene, ethylene-propylene copolymer, polymethylpentene, polyvinyl chloride, polyvinylidene chloride, polyvinyl acetate, ethylene-vinyl acetate copolymer Polymer, polyvinyl alcohol, polyacetal, fluororesin such as polyvinylidene fluoride and polytetrafluoroethylene, polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polystyrene, polyacrylonitrile, styrene-acrylonitrile copolymer, acrylonitrile-butadiene-styrene copolymer Polymer (ABS) resin, polyphenylene ether, modified polyphenylene ether, aliphatic polyamides, aromatic polyamides, polyamideimide, polymethacrylic acid or Esters thereof, polyacrylic acid or its ester, polycarbonate, polyphenylene sulfide, polysulfone, polyether sulfone, polyether nitrile, polyether ketone, may be used polyketone, liquid crystal polymer, silicone resin, ionomer and the like.
Further, for example, styrene-based thermoplastic elastomers such as styrene-butadiene copolymers or hydrogenated polymers thereof, styrene-isoprene block copolymers or hydrogenated polymers thereof, olefin-based thermoplastic elastomers, vinyl chloride-based thermoplastic elastomers, polyesters. A thermoplastic thermoplastic elastomer, a polyurethane thermoplastic elastomer, a polyamide thermoplastic elastomer, or the like can be used.
Furthermore, for example, silicone rubber, acrylic rubber, butyl rubber, fluorine rubber, nitrile rubber, hydrogenated nitrile rubber, and the like can be used.
These may be used alone or in combination of two or more.
Among these, silicone rubber is preferable because it is excellent in flexibility when it is formed into a molded body, shape followability, adhesion to a heat generating surface when contacting an electronic component, and heat resistance.
上記シリコーンゴムとしては、シリコーン骨格を有する高分子(シリコーン)が架橋したものが挙げられる。
ここで、シリコーンの架橋は、過酸化物架橋であっても良いし、付加反応型の架橋であっても良いが、過酸化物架橋が好ましい。過酸化物架橋によって架橋されたシリコーンゴムの方が耐熱性に優れるからである。Examples of the silicone rubber include those obtained by crosslinking a polymer having a silicone skeleton (silicone).
Here, the crosslinking of silicone may be peroxide crosslinking or addition reaction type crosslinking, but peroxide crosslinking is preferable. This is because the silicone rubber crosslinked by peroxide crosslinking is superior in heat resistance.
上記シリコーンゴムとしては、例えば、側鎖が全てメチル基で不飽和基を含まないシリコーンと側鎖(末端も含む)の一部にビニル基を有するシリコーンとの混合物を過酸化物架橋させたものが好ましい。
このとき、上記側鎖の一部にビニル基を有するシリコーンは、上記側鎖が全てメチル基で不飽和基を含まないシリコーンに対する架橋剤とみなすこともできる。Examples of the silicone rubber include those obtained by peroxide-crosslinking a mixture of silicone having all methyl groups and no unsaturated groups and silicone having a vinyl group in a part of the side chains (including terminals). Is preferred.
At this time, the silicone having a vinyl group in a part of the side chain can also be regarded as a crosslinking agent for the silicone in which the side chain is entirely a methyl group and does not contain an unsaturated group.
上記側鎖の一部にビニル基を有するシリコーンの具体例としては、例えば、分子鎖両末端ジメチルビニルシロキシ基封鎖ジメチルポリシロキサン、分子鎖両末端メチルフェニルビニルシロキシ基封鎖ジメチルポリシロキサン、分子鎖両末端ジメチルビニルシロキシ基封鎖ジメチルシロキサン・メチルフェニルシロキサン共重合体、分子鎖両末端ジメチルビニルシロキシ基封鎖ジメチルシロキサン・メチルビニルシロキサン共重合体、分子鎖両末端トリメチルシロキシ基封鎖ジメチルシロキサン・メチルビニルシロキサン共重合体、分子鎖両末端ジメチルビニルシロキシ基封鎖メチル(3,3,3−トリフルオロプロピル)ポリシロキサン、分子鎖両末端シラノール基封鎖ジメチルシロキサン・メチルビニルシロキサン共重合体、分子鎖両末端シラノール基封鎖ジメチルシロキサン・メチルビニルシロキサン・メチルフェニルシロキサン共重合体等が挙げられる。これらは単独で用いても良いし、2種以上併用しても良い。 Specific examples of the silicone having a vinyl group in a part of the side chain include, for example, molecular chain both ends dimethylvinylsiloxy group-capped dimethylpolysiloxane, molecular chain both ends methylphenylvinylsiloxy group-capped dimethylpolysiloxane, both molecular chains Terminal dimethylvinylsiloxy group-blocked dimethylsiloxane / methylphenylsiloxane copolymer, molecular chain both ends dimethylvinylsiloxy group-blocked dimethylsiloxane / methylvinylsiloxane copolymer, molecular chain both ends trimethylsiloxy group-blocked dimethylsiloxane / methylvinylsiloxane copolymer Polymer, both ends of molecular chain dimethylvinylsiloxy-blocked methyl (3,3,3-trifluoropropyl) polysiloxane, both ends of molecular chain silanol-blocked dimethylsiloxane / methylvinylsiloxane copolymer, both ends of molecular chain Silanol group-blocked dimethylsiloxane-methylvinylsiloxane-methylphenylsiloxane copolymers. These may be used alone or in combination of two or more.
上記過酸化物架橋を行う際の有機過酸化物としては、例えば、ベンゾイルパーオキサイド、ジクミルパーオキサイド、2,5−ジメチル−2,5−ジ(t−ブチルパーオキシ)ヘキサン、ジ−t−ブチルパーオキサイド、t−ブチルパーベンゾエート等が挙げられる。これらは単独で用いても良いし、2種以上併用しても良い。
更に、架橋時には、架橋促進剤や架橋促進助剤を併用しても良い。Examples of the organic peroxide used for the above-described peroxide crosslinking include benzoyl peroxide, dicumyl peroxide, 2,5-dimethyl-2,5-di (t-butylperoxy) hexane, and di-t. -Butyl peroxide, t-butyl perbenzoate, etc. are mentioned. These may be used alone or in combination of two or more.
Further, at the time of crosslinking, a crosslinking accelerator or a crosslinking acceleration assistant may be used in combination.
マトリックス成分2は、上記樹脂に加えて、上述したように架橋剤、架橋促進剤、架橋促進助剤を含有しても良い。また、マトリックス成分2は、補強剤、充填剤、軟化剤、可塑剤、老化防止剤、粘着付与剤、帯電防止剤、練り込み接着剤、難燃剤、カップリング剤等の一般的な添加剤を含有していても良い。 In addition to the above resin, the matrix component 2 may contain a crosslinking agent, a crosslinking accelerator, and a crosslinking acceleration assistant as described above. The matrix component 2 contains general additives such as reinforcing agents, fillers, softeners, plasticizers, anti-aging agents, tackifiers, antistatic agents, kneading adhesives, flame retardants, and coupling agents. You may contain.
熱伝導性シート1は、2種類の熱伝導性フィラーとして、第1熱伝導性フィラー4と、第1熱伝導性フィラー4よりも粒径の小さい第2熱伝導性フィラー5とを含有する。
第1熱伝導性フィラー4は、窒化ホウ素(BN)からなる。そのため、熱伝導性シート1は優れた熱伝導性を有する。
第1熱伝導性フィラー4は、所定の粒径及びアスペクト比を有していればその形状は特に限定されない。第1熱伝導性フィラー4の具体的な形状としては、例えば、鱗片状、板状、膜状、繊維状、円柱状、角柱状、楕円状、扁平形状などが挙げられる。
これらのなかでは鱗片状が好ましい。高アスペクト比で、かつ面方向に等方的な熱伝導率を有しているため、鱗片状の熱伝導性フィラーを配向させた場合、成型品の熱伝導率が高くなるからである。The thermally conductive sheet 1 contains a first thermally conductive filler 4 and a second thermally conductive filler 5 having a particle size smaller than that of the first thermally conductive filler 4 as two types of thermally conductive fillers.
The first thermally conductive filler 4 is made of boron nitride (BN). Therefore, the heat conductive sheet 1 has excellent heat conductivity.
The shape of the first thermally conductive filler 4 is not particularly limited as long as it has a predetermined particle size and aspect ratio. Specific examples of the shape of the first heat conductive filler 4 include a scale shape, a plate shape, a film shape, a fiber shape, a columnar shape, a prismatic shape, an elliptical shape, and a flat shape.
Of these, scaly is preferable. This is because, since it has a high aspect ratio and isotropic thermal conductivity in the plane direction, when the scale-like thermal conductive filler is oriented, the thermal conductivity of the molded product becomes high.
第1熱伝導性フィラー4の粒径は30μm以上である。上記粒径が30μm未満では、熱伝導パスが形成しにくく、熱伝導性に劣る場合がある。
一方、第1熱伝導性フィラー4の粒径の好ましい上限は、熱伝導性樹脂成型品を作製する際の加工性の観点から100μmである。The particle size of the first thermally conductive filler 4 is 30 μm or more. When the particle size is less than 30 μm, it is difficult to form a heat conduction path and the heat conductivity may be inferior.
On the other hand, the preferable upper limit of the particle size of the first thermally conductive filler 4 is 100 μm from the viewpoint of workability when producing a thermally conductive resin molded product.
第1熱伝導性フィラー4のアスペクト比は10以上である。この場合、第1熱伝導性フィラー4の間隙に、第1熱伝導性フィラー4より粒径の小さい第2熱伝導性フィラー5が分散して熱伝導パスを形成しやすく、また、第1熱伝導性フィラー4がマトリックス成分2中で配向し易い。
一方、第1熱伝導性フィラー4のアスペクト比の上限は、100が好ましい。この場合、第1熱伝導性フィラーを熱伝導性樹脂成型品に充填しやすく、また、熱伝導性樹脂成型品を作製する際の加工性にも優れることになる。The aspect ratio of the first thermally conductive filler 4 is 10 or more. In this case, the second heat conductive filler 5 having a particle diameter smaller than that of the first heat conductive filler 4 is easily dispersed in the gap between the first heat conductive fillers 4 to form a heat conduction path. The conductive filler 4 is easily oriented in the matrix component 2.
On the other hand, the upper limit of the aspect ratio of the first thermally conductive filler 4 is preferably 100. In this case, it is easy to fill the thermally conductive resin molded product with the first thermally conductive filler, and the processability when producing the thermally conductive resin molded product is excellent.
本発明において、熱伝導性フィラーの「粒径」とは、粒度分布測定における平均粒径という概念である。上記平均粒径は、レーザー回析散乱法(装置:マイクロトラック・ベル株式会社社製、マイクロトラックMT3300EXII)によって測定されたものである。
また、本発明において、熱伝導性フィラーの「アスペクト比」は、短径に対する長径の比の平均値という概念である。上記アスペクト比は、SEMで撮影された画像から200個以上の粒子を任意に選択し、それぞれの長径と短径の比を求めて平均値を算出する。ここで、長径及び短径は、各粒子の観察画像において、最も長い部分の長さを長径とし、この長径の中点を通り、かつ当該長径に直行する部分の長さを短径とする。In the present invention, the “particle size” of the thermally conductive filler is a concept of an average particle size in the particle size distribution measurement. The average particle diameter is measured by a laser diffraction scattering method (apparatus: manufactured by Microtrac Bell Co., Ltd., Microtrac MT3300EXII).
In the present invention, the “aspect ratio” of the thermally conductive filler is a concept of an average value of the ratio of the major axis to the minor axis. As the aspect ratio, 200 or more particles are arbitrarily selected from an image taken with an SEM, and the ratio between the major axis and the minor axis is obtained to calculate an average value. Here, in the observation image of each particle, the major axis and the minor axis are the longest part, and the length of the part that passes through the midpoint of the major axis and is perpendicular to the major axis is the minor axis.
第2熱伝導性フィラー5は、第1熱伝導性フィラーより小さい粒径を有し、窒化ホウ素以外の材質からなる。
第2熱伝導性フィラー5は、窒化ホウ素以外の材質からなり、かつ熱伝導性を有するものであれば良い。第2熱伝導性フィラー5の具体例としては、例えば、黒鉛、炭素繊維、カーボンナノチューブ(CNT)、雲母、アルミナ、窒化アルミニウム、炭化珪素、シリカ、酸化亜鉛、酸化マグネシウム、炭酸カルシウム、炭酸マグネシウム、二硫化モリブデン、銅、アルミニウム等からなるものが挙げられる。
これらのなかでは、酸化マグネシウムからなる熱伝導性フィラー、及び、炭酸マグネシウムからなる熱伝導性フィラーが好ましい。第1熱伝導性フィラー4同士の間に介在して熱伝導性シート1の熱伝導性を高めるのに適しており、かつ熱伝導性シート1を安価で提供するのに適しているからである。The 2nd heat conductive filler 5 has a particle size smaller than the 1st heat conductive filler, and consists of materials other than boron nitride.
The second thermally conductive filler 5 may be made of a material other than boron nitride and has thermal conductivity. Specific examples of the second thermally conductive filler 5 include, for example, graphite, carbon fiber, carbon nanotube (CNT), mica, alumina, aluminum nitride, silicon carbide, silica, zinc oxide, magnesium oxide, calcium carbonate, magnesium carbonate, The thing which consists of molybdenum disulfide, copper, aluminum, etc. is mentioned.
In these, the heat conductive filler which consists of magnesium oxide, and the heat conductive filler which consists of magnesium carbonate are preferable. This is because it is suitable for increasing the thermal conductivity of the thermal conductive sheet 1 by being interposed between the first thermal conductive fillers 4 and for providing the thermal conductive sheet 1 at a low cost. .
第2熱伝導性フィラー5の形状は特に限定されず、具体的な形状としては、例えば、球状、鱗片状、板状、膜状、円柱状、角柱状、楕円状、扁平形状などが挙げられる。
第2熱伝導性フィラー5の形状は、球状、鱗片状が好ましい。この場合、第1熱伝導性フィラー4間に熱伝導パスを形成しやすく、また、第1熱伝導性フィラー4を配向させるのに適しているからである。The shape of the 2nd heat conductive filler 5 is not specifically limited, As a specific shape, spherical shape, scale shape, plate shape, film | membrane shape, cylindrical shape, prismatic shape, elliptical shape, flat shape etc. are mentioned, for example. .
The shape of the second thermally conductive filler 5 is preferably spherical or scaly. In this case, it is easy to form a heat conduction path between the first heat conductive fillers 4 and is suitable for orienting the first heat conductive fillers 4.
第2熱伝導性フィラー5の粒径は、第1熱伝導性フィラー4の粒径よりも小さければ特に限定されないが、3〜20μmが好ましい。
第2熱伝導性フィラー5の粒径がこの範囲にあると、第1熱伝導性フィラー4同士の間に介在して熱伝導パスを形成すること、及び、第1熱伝導性フィラー4を配向させること、により適している。更に、第2熱伝導性フィラー5の粒径がこの範囲にあると、熱伝導性シート1の表面粗さを抑え、発熱部材や放熱部材と接触した際の接触熱抵抗(熱伝導性シート1の表面の熱抵抗)を小さくするのに適している。
一方、第2熱伝導性フィラー5の粒径が20μmを超えると、第1熱伝導性フィラー4が配向しにくくなり、熱伝導性シート1は熱伝導性に劣る場合がある。
また、第2熱伝導性フィラー5の粒径が3μm未満の場合は、第2熱伝導性フィラー5の材質によっては、熱伝導性シート1は熱伝導性に劣ることがある。例えば、第2熱伝導性フィラー5の材質が酸化マグネシウム又は炭酸マグネシウムの場合は、熱伝導性シート1の製造過程で第2熱伝導性フィラー5の発泡が生じる場合があり、このような発泡が生じると、製造された熱伝導性シート1の熱伝導性が低下する場合がある。
第2熱伝導性フィラー5の粒径は、5〜20μmがより好ましく、5〜15μmがさらに更に好ましく、5〜10μmが特に好ましい。Although the particle size of the 2nd heat conductive filler 5 will not be specifically limited if it is smaller than the particle size of the 1st heat conductive filler 4, 3-20 micrometers is preferable.
When the particle size of the second thermally conductive filler 5 is within this range, a heat conductive path is formed between the first thermally conductive fillers 4 and the first thermally conductive filler 4 is oriented. More suitable. Furthermore, when the particle size of the second heat conductive filler 5 is within this range, the surface roughness of the heat conductive sheet 1 is suppressed, and the contact thermal resistance (heat conductive sheet 1) when contacting the heat generating member or the heat radiating member. It is suitable for reducing the thermal resistance of the surface.
On the other hand, when the particle size of the second thermally conductive filler 5 exceeds 20 μm, the first thermally conductive filler 4 becomes difficult to be oriented, and the thermally conductive sheet 1 may be inferior in thermal conductivity.
Moreover, when the particle size of the 2nd heat conductive filler 5 is less than 3 micrometers, depending on the material of the 2nd heat conductive filler 5, the heat conductive sheet 1 may be inferior to heat conductivity. For example, when the material of the second thermally conductive filler 5 is magnesium oxide or magnesium carbonate, foaming of the second thermally conductive filler 5 may occur in the manufacturing process of the thermally conductive sheet 1, and such foaming may occur. When it arises, the heat conductivity of the manufactured heat conductive sheet 1 may fall.
As for the particle size of the 2nd heat conductive filler 5, 5-20 micrometers is more preferable, 5-15 micrometers is still more preferable, 5-10 micrometers is especially preferable.
第2熱伝導性フィラー5のアスペクト比の上限は100が好ましい。第2熱伝導性フィラーを熱伝導性樹脂成型品に充填しやすく、また、熱伝導性樹脂成型品を作製する際の加工性にも優れるからである。
第2熱伝導性フィラー5のアスペクト比の下限は限定されず、第2熱伝導性フィラー5のアスペクト比は1以上であれば良い。
第2熱伝導性フィラー5の粒径及びアスペクト比のそれぞれの測定方法は、第1熱伝導性フィラー4の粒径及びアスペクト比の測定方法と同様である。The upper limit of the aspect ratio of the second thermally conductive filler 5 is preferably 100. This is because it is easy to fill the thermally conductive resin molded product with the second thermally conductive filler, and the processability when producing the thermally conductive resin molded product is excellent.
The lower limit of the aspect ratio of the second thermally conductive filler 5 is not limited, and the aspect ratio of the second thermally conductive filler 5 may be 1 or more.
The measuring method of the particle size and aspect ratio of the second thermally conductive filler 5 is the same as the measuring method of the particle size and aspect ratio of the first thermally conductive filler 4.
熱伝導性シート1における熱伝導性フィラーの含有量(熱伝導性フィラーの総含有量)は、30〜50体積%である。
上記熱伝導性フィラーの総含有量が30体積%未満では、充分な熱伝導性を確保することができない。また、上記含有量が50体積%を超えると、熱伝導性樹脂成型品を作製する際の加工性に劣ることになり、かつ熱伝導性を有する樹脂成型品を安価で提供することが困難になる。The content of the heat conductive filler in the heat conductive sheet 1 (total content of the heat conductive filler) is 30 to 50% by volume.
When the total content of the heat conductive filler is less than 30% by volume, sufficient heat conductivity cannot be ensured. Further, if the content exceeds 50% by volume, the processability when producing a thermally conductive resin molded product is inferior, and it is difficult to provide a resin molded product having thermal conductivity at low cost. Become.
熱伝導性シート1における第1熱伝導性フィラー4の含有量は、5〜20体積%である。この場合、第1熱伝導性フィラーを配向させ、熱伝導性を確保することができる。
一方、第1熱伝導性フィラー4の含有量が5体積%未満では、第1熱伝導性フィラーを配向させても、充分な熱伝導性を確保することができない。また、上記含有量が20体積%を超えると、安価に熱伝導性樹脂成型品を提供することが困難である。Content of the 1st heat conductive filler 4 in the heat conductive sheet 1 is 5-20 volume%. In this case, the first thermal conductive filler can be oriented to ensure thermal conductivity.
On the other hand, if the content of the first thermal conductive filler 4 is less than 5% by volume, sufficient thermal conductivity cannot be ensured even if the first thermal conductive filler is oriented. Moreover, when the said content exceeds 20 volume%, it is difficult to provide a heat conductive resin molded product cheaply.
熱伝導性シート1における第2熱伝導性フィラー5の含有量は、10〜45体積%が好ましい。
第2熱伝導性フィラー5の含有量が10体積%未満では、成型時に第1熱伝導性フィラーを配向させることが困難になる。一方、第2熱伝導性フィラー5の含有量が45体積%を超えると、第1熱伝導性フィラーの含有量が少なくなりすぎ、充分な熱伝導性を確保することができなくなる。
第2熱伝導性フィラー5の含有量は、20〜45体積%がより好ましい。As for content of the 2nd heat conductive filler 5 in the heat conductive sheet 1, 10-45 volume% is preferable.
If the content of the second thermally conductive filler 5 is less than 10% by volume, it is difficult to orient the first thermally conductive filler during molding. On the other hand, if the content of the second heat conductive filler 5 exceeds 45% by volume, the content of the first heat conductive filler becomes too small to ensure sufficient heat conductivity.
As for content of the 2nd heat conductive filler 5, 20-45 volume% is more preferable.
本実施形態の熱伝導性シート1は、熱伝導性フィラーとして、第1熱伝導性フィラー4及び第2熱伝導性フィラー5を含有している。ここで、第1熱伝導性フィラー4の粒径D1と、第2熱伝導性フィラー5の粒径D2が、D1>D2の関係を有している。
なお、熱伝導性シート1は、本発明の効果を損なわない範囲で、第1熱伝導性フィラー4及び第2熱伝導性フィラー5以外の熱伝導性フィラーを含有しても良い。The heat conductive sheet 1 of this embodiment contains the 1st heat conductive filler 4 and the 2nd heat conductive filler 5 as a heat conductive filler. Here, the particle size D1 of the first thermally conductive filler 4 and the particle size D2 of the second thermally conductive filler 5 have a relationship of D1> D2.
In addition, the heat conductive sheet 1 may contain heat conductive fillers other than the 1st heat conductive filler 4 and the 2nd heat conductive filler 5 in the range which does not impair the effect of this invention.
熱伝導性シート1の厚さは特に限定されないが、例えば、0.1〜3.0mm程度である。
この場合、熱伝導性シート1は、電気部品や自動車部品等において、発熱部材と放熱部材との間で熱を効率良く伝達する部材として好適に使用することができる。Although the thickness of the heat conductive sheet 1 is not specifically limited, For example, it is about 0.1-3.0 mm.
In this case, the heat conductive sheet 1 can be suitably used as a member that efficiently transfers heat between the heat generating member and the heat radiating member in an electrical component, an automobile component, or the like.
次に、本実施形態に係る熱伝導性シートを製造する方法について、図面を参照しながら説明する。
図2は、本発明の実施形態に係る熱伝導性シートの製造で使用する押出機を模式的に示す図である。図2には、押出機100の先端部分及びTダイの断面概略図を示す。
押出機100に投入された熱伝導性フィラーを含む原料組成物は、スクリュー8によって撹拌・混練され、流路10に沿って第1ギャップ12に導入される。Next, a method for producing a thermally conductive sheet according to the present embodiment will be described with reference to the drawings.
Drawing 2 is a figure showing typically an extruder used by manufacture of a heat conductive sheet concerning an embodiment of the present invention. In FIG. 2, the front-end | tip part of the extruder 100 and the cross-sectional schematic of a T die are shown.
The raw material composition containing the thermally conductive filler charged into the extruder 100 is stirred and kneaded by the screw 8 and introduced into the first gap 12 along the flow path 10.
押出機100に投入された原料組成物は、まず、第1ギャップ12によって上下方向(厚さ方向)にしぼり込まれて薄い帯状となる。第1ギャップ12を通過する際、原料組成物にはせん断力が作用し、原料組成物中に混合されている第1熱伝導性フィラーが原料組成物の流れ方向に配向する。従って、第1ギャップ12を通過して成形された厚さの薄い樹脂シート前駆体は、少なくとも第1熱伝導性フィラーが当該樹脂シート前駆体の面方向に配向している。
また、第2熱伝導性フィラーが配向可能な形状を有するフィラーの場合、当該第2熱伝導性フィラーは、第1ギャップ12を通過する際に第1熱伝導性フィラーと同方向に配向する。The raw material composition charged into the extruder 100 is first squeezed in the vertical direction (thickness direction) by the first gap 12 into a thin strip shape. When passing through the first gap 12, a shearing force acts on the raw material composition, and the first thermally conductive filler mixed in the raw material composition is oriented in the flow direction of the raw material composition. Therefore, at least the first thermal conductive filler is oriented in the surface direction of the resin sheet precursor in the thin resin sheet precursor formed through the first gap 12.
When the second thermally conductive filler is a filler having an orientable shape, the second thermally conductive filler is oriented in the same direction as the first thermally conductive filler when passing through the first gap 12.
第1ギャップ12の隙間(図2中、上下方向の寸法)は、0.1mm以上5.0mm以下であることが好ましい。第1ギャップ12の隙間が0.1mmよりも小さいと、押出し圧力が不必要に上昇し、更には、樹脂詰まりが発生してしまうことがある。一方、第1ギャップ12の隙間が5.0mmよりも大きいと、上記薄い樹脂シート前駆体の面方向に対する熱伝導性フィラーの配向度が減少することがある。 The gap (the vertical dimension in FIG. 2) of the first gap 12 is preferably 0.1 mm or greater and 5.0 mm or less. When the gap of the first gap 12 is smaller than 0.1 mm, the extrusion pressure increases unnecessarily, and furthermore, resin clogging may occur. On the other hand, when the gap of the first gap 12 is larger than 5.0 mm, the degree of orientation of the thermally conductive filler with respect to the surface direction of the thin resin sheet precursor may be reduced.
第1熱伝導性フィラーが面方向に配向した上記薄い樹脂シート前駆体は、第1ギャップ12を完全に通過すると、押出方向に限定されていたシートの流れ方向が解放されて、当該流れ方向が押出方向に対してほぼ垂直となる方向に変化する。これは、第1ギャップ12を通過した後の流路10の断面積が拡大し、流路10の上下方向の長さが長くなるためである。
シートの流れ方向が押出方向に対してほぼ垂直となる方向に変化した上記薄い樹脂シート前駆体は、第1ギャップ12を完全に通過した後、更に第2ギャップ14に向かって押し出される。その結果、第2ギャップ14内の樹脂シート前駆体は、上記薄い樹脂シート前駆体が積層された状態となる。その際に第1熱伝導性フィラーの多くは、第2ギャップ14内の樹脂シート前駆体の厚さ方向(図2中、上下方向)に配向させられる。
その後、必要に応じて、樹脂シート前駆体を所定の条件で加熱することにより架橋を進行させ、更に必要に応じて、樹脂シート前駆体を厚さ方向に垂直な方向にスライス加工する。このような工程を経て、熱伝導性シート1が製造される。When the thin resin sheet precursor in which the first thermally conductive filler is oriented in the plane direction passes through the first gap 12 completely, the flow direction of the sheet limited to the extrusion direction is released, and the flow direction is It changes in a direction substantially perpendicular to the extrusion direction. This is because the cross-sectional area of the flow channel 10 after passing through the first gap 12 is enlarged, and the vertical length of the flow channel 10 is increased.
The thin resin sheet precursor in which the flow direction of the sheet has changed in a direction substantially perpendicular to the extrusion direction is completely pushed through the first gap 12 and then pushed toward the second gap 14. As a result, the resin sheet precursor in the second gap 14 is in a state where the thin resin sheet precursor is laminated. At that time, most of the first thermally conductive filler is oriented in the thickness direction (vertical direction in FIG. 2) of the resin sheet precursor in the second gap 14.
Thereafter, if necessary, the resin sheet precursor is heated under predetermined conditions to cause crosslinking, and if necessary, the resin sheet precursor is sliced in a direction perpendicular to the thickness direction. The heat conductive sheet 1 is manufactured through such steps.
ここで、第2ギャップ14の隙間は第1ギャップ12の隙間の2倍以上20倍以下であることが好ましい。第2ギャップ14の隙間が第1ギャップ12の隙間の2倍よりも小さい場合は、第1熱伝導性フィラー4が熱伝導性シート1の厚さ方向に配向しないことがある。また、第2ギャップ14の隙間が第1ギャップ12の隙間の20倍よりも大きな場合は、部分的に樹脂シート前駆体が乱流した状況が生じやすくなり、その結果、熱伝導性シート1の厚さ方向に配向する第1熱伝導性フィラー4の割合が減少してしまうことがある。
第2ギャップ14の隙間は第1ギャップ12の隙間の2倍以上10倍以下であることがより好ましい。
また、上記樹脂シート前駆体が流路10の上下方向において均等に流れやすくなる観点から、第1ギャップ12における厚さ方向の中心と、第2ギャップ14における厚さ方向の中心とは、厚さ方向において略同一の位置にあることが好ましい。Here, the gap of the second gap 14 is preferably not less than 2 times and not more than 20 times the gap of the first gap 12. When the gap of the second gap 14 is smaller than twice the gap of the first gap 12, the first thermally conductive filler 4 may not be oriented in the thickness direction of the thermally conductive sheet 1. In addition, when the gap of the second gap 14 is larger than 20 times the gap of the first gap 12, a situation in which the resin sheet precursor is partially turbulent easily occurs, and as a result, the heat conductive sheet 1 The ratio of the 1st heat conductive filler 4 orientated in the thickness direction may reduce.
The gap of the second gap 14 is more preferably not less than 2 times and not more than 10 times the gap of the first gap 12.
Further, from the viewpoint that the resin sheet precursor easily flows in the vertical direction of the flow path 10, the thickness direction center of the first gap 12 and the thickness direction center of the second gap 14 are the thicknesses. It is preferable to be in substantially the same position in the direction.
第1ギャップ12に繋がる開口部の形状は特に規定されないが、上流側の開口部の側面(上下面)は圧力損失が少ないように傾斜面とすることが好ましく、下流側の開口部の側面(上下面)については効率良く熱伝導性フィラーを樹脂シートの厚さ方向に配向させるために、傾斜角度(押出方向と傾斜面とのなす角度)を調整することが望ましい。当該傾斜角度としては、例えば、10°〜50°とすることができ、更には、20°〜25°であるのが好ましい。
また、第1ギャップ12に繋がる開口部は、上下共に傾斜を有している必要はなく、どちらか一方のみが傾斜を有していても良い。
なお、第1ギャップ12及び第2ギャップ14の奥行(即ち、図2において紙面に略垂直な方向における第1ギャップ12及び第2ギャップ14の隙間)は、Tダイの全体にわたって略同一である。また、上記第1ギャップ及び上記第2ギャップの奥行寸法は特に規定されず、樹脂シートの製品幅に応じて種々の設計変更が可能である。The shape of the opening connected to the first gap 12 is not particularly defined, but the side surface (upper and lower surfaces) of the upstream opening is preferably an inclined surface so that the pressure loss is small, and the side surface of the downstream opening ( In order to efficiently orient the thermally conductive filler in the thickness direction of the resin sheet, it is desirable to adjust the inclination angle (angle formed by the extrusion direction and the inclined surface). As said inclination-angle, it can be set as 10 degrees-50 degrees, for example, Furthermore, it is preferable that it is 20 degrees-25 degrees.
Moreover, the opening part connected to the 1st gap 12 does not need to have an inclination up and down, and either one may have an inclination.
Note that the depths of the first gap 12 and the second gap 14 (that is, the gap between the first gap 12 and the second gap 14 in the direction substantially perpendicular to the paper surface in FIG. 2) are substantially the same throughout the T-die. Further, the depth dimensions of the first gap and the second gap are not particularly defined, and various design changes can be made according to the product width of the resin sheet.
本発明の実施形態に係る熱伝導性シートは、下記の製造方法によって製造することもできる。
即ち、熱伝導性シートを製造するための原料組成物を調製した後、この原料組成物を用いて少なくとも第1熱伝導性フィラーが面方向に配向したシート状物を従来公知の方法で複数枚作製し、そのシート状物を複数枚積層してブロック状物とした後、上記第1熱伝導性フィラーが配向した方向に対して垂直な方向から上記ブロック状物(シート状物の積層体)をカットすることにより作製しても良い。この方法で熱伝導性シートを製造する場合、必要に応じて、適宜なタイミングで架橋処理を施しても良い。
このような方法で製造された熱伝導性シートもまた、第1熱伝導性フィラーが熱伝導性シートの略厚さ方向に配向した熱伝導性に優れたシートとなる。The heat conductive sheet which concerns on embodiment of this invention can also be manufactured with the following manufacturing method.
That is, after preparing a raw material composition for producing a heat conductive sheet, a plurality of sheet-like materials in which at least a first heat conductive filler is oriented in a plane direction using the raw material composition are formed by a conventionally known method. After producing and laminating a plurality of the sheet-like materials to form a block-like material, the block-like material (laminated body of sheet-like materials) from a direction perpendicular to the direction in which the first thermally conductive filler is oriented. You may produce by cutting. When manufacturing a heat conductive sheet by this method, you may perform a crosslinking process at an appropriate timing as needed.
The heat conductive sheet manufactured by such a method is also a sheet having excellent heat conductivity in which the first heat conductive filler is oriented in the substantially thickness direction of the heat conductive sheet.
次に、本発明を実施例に基づいてさらに詳細に説明するが、本発明は、かかる実施例のみに限定されるものではない。
(実施例1)
表1に記載の配合にて、樹脂成分に、架橋剤並びに第1熱伝導性フィラー及び第2熱伝導性フィラー(以下、全てを合わせて原料成分ともいう)を2本ロールで練り込み、リボンシート(前駆体としての組成物)を得た。
上記樹脂成分としては、シリコーンゴム「東レダウコーニング社製のDY321005U」、及び可塑剤(信越化学工業社製のシリコーンオイル:KF−96−3000CS)を用いた。
上記架橋剤としては、東レダウコーング社製の「MR‐53」及び「RC−4 50P FD」を用いた。表1にはその合計含有量を示した。
上記第1熱伝導性フィラーとしては、窒化ホウ素からなるフィラー(デンカ株式会社製「XGP」(鱗片状、粒径35μm、アスペクト比約30))を用いた。
上記第2熱伝導性フィラーとしては、炭酸マグネシウムからなるフィラー(立方体状、粒径6μm、アスペクト比約1(神島化学工業株式会社製))を用いた。Next, the present invention will be described in more detail based on examples. However, the present invention is not limited to such examples.
Example 1
In the formulation shown in Table 1, a cross-linking agent, a first heat conductive filler, and a second heat conductive filler (hereinafter also referred to as raw material components) are kneaded with two rolls into a resin component, and a ribbon A sheet (composition as a precursor) was obtained.
As the resin component, silicone rubber “DY321010U manufactured by Toray Dow Corning Co., Ltd.” and a plasticizer (silicone oil manufactured by Shin-Etsu Chemical Co., Ltd .: KF-96-3000CS) were used.
As the cross-linking agent, “MR-53” and “RC-4 50P FD” manufactured by Toray Dow Corning Co., Ltd. were used. Table 1 shows the total content.
As the first thermally conductive filler, a filler made of boron nitride (“XGP” (scale-like, particle size 35 μm, aspect ratio about 30) manufactured by Denka Co., Ltd.) was used.
As the second thermally conductive filler, a filler made of magnesium carbonate (cubic, particle size 6 μm, aspect ratio about 1 (manufactured by Kamishima Chemical Co., Ltd.)) was used.
次に、作製したリボンシートを図2に示したようなゴム用短軸押出機100にて、1mmの第一ギャップ及び10mmの第二ギャップを有する垂直配向金型(口金)を用いて、第1熱伝導性フィラー(鱗片状窒化ホウ素)が厚さ方向に配向した厚さ10mmのシートを作製し、当該シートを170℃で30分間の架橋処理を施した。架橋処理後の当該シートを厚さ方向と垂直にスライス加工し、厚さ500μmの熱伝導性樹脂成型品として熱伝導性シート1を作製した。 Next, the produced ribbon sheet was measured using a vertical alignment mold (die) having a first gap of 1 mm and a second gap of 10 mm using a short shaft extruder 100 for rubber as shown in FIG. 1 A sheet having a thickness of 10 mm in which a thermally conductive filler (flaky boron nitride) was oriented in the thickness direction was prepared, and the sheet was subjected to a crosslinking treatment at 170 ° C. for 30 minutes. The sheet after the cross-linking treatment was sliced perpendicularly to the thickness direction to produce a heat conductive sheet 1 as a 500 μm thick heat conductive resin molded product.
(実施例2)
原料成分の配合量を表1に示したように変更した以外は、実施例1と同様にして熱伝導性シート1を作製した。(Example 2)
A thermally conductive sheet 1 was produced in the same manner as in Example 1 except that the blending amounts of the raw material components were changed as shown in Table 1.
(実施例3)
第2熱伝導性フィラーとして、炭酸マグネシウムからなるフィラー(立方体状、粒径15μm、アスペクト比約1(神島化学工業株式会社製))を使用し、かつ原料成分の配合量を表1に示したように変更した以外は、実施例1と同様にして熱伝導性シート1を作製した。Example 3
As the second thermally conductive filler, a filler made of magnesium carbonate (cubic, particle size of 15 μm, aspect ratio of about 1 (manufactured by Kamijima Chemical Co., Ltd.)) was used, and the blending amounts of the raw material components are shown in Table 1. A heat conductive sheet 1 was produced in the same manner as in Example 1 except that the above was changed.
(実施例4)
原料成分の配合量を表1に示したように変更した以外は、実施例1と同様にして熱伝導性シート1を作製した。Example 4
A thermally conductive sheet 1 was produced in the same manner as in Example 1 except that the blending amounts of the raw material components were changed as shown in Table 1.
(実施例5)
第2熱伝導性フィラーとして、酸化マグネシウムからなるフィラー(堺化学工業株式会社製の「SMO」(球状、粒径10μm、アスペクト比約1))を使用し、かつ原料成分の配合量を表1に示したように変更した以外は、実施例1と同様にして熱伝導性シート1を作製した。(Example 5)
As the second thermally conductive filler, a filler made of magnesium oxide (“SMO” (spherical, particle size 10 μm, aspect ratio of about 1) manufactured by Sakai Chemical Industry Co., Ltd.) is used, and the blending amounts of the raw material components are shown in Table 1. A heat conductive sheet 1 was produced in the same manner as in Example 1 except that the changes were made as shown in FIG.
(実施例6)
原料成分の配合量を表1に示したように変更した以外は、実施例5と同様にして熱伝導性シート1を作製した。(Example 6)
A thermally conductive sheet 1 was produced in the same manner as in Example 5 except that the blending amounts of the raw material components were changed as shown in Table 1.
(実施例7)
第2熱伝導性フィラーとして、炭酸マグネシウムからなるフィラー(立方体状、粒径26μm、アスペクト比約1(神島化学工業株式会社製))を使用し、かつ原料成分の配合量を表1に示したように変更した以外は、実施例1と同様にして熱伝導性シート1を作製した。(Example 7)
As the second thermally conductive filler, a filler made of magnesium carbonate (cubic, particle size of 26 μm, aspect ratio of about 1 (manufactured by Kamijima Chemical Co., Ltd.)) was used, and the blending amounts of the raw material components are shown in Table 1. A heat conductive sheet 1 was produced in the same manner as in Example 1 except that the above was changed.
(実施例8)
原料成分の配合量を表1に示したように変更した以外は、実施例3と同様にして熱伝導性シート1を作製した。(Example 8)
A thermally conductive sheet 1 was produced in the same manner as in Example 3 except that the blending amounts of the raw material components were changed as shown in Table 1.
(実施例9)
原料成分の配合量を表1に示したように変更した以外は、実施例1と同様にして熱伝導性シート1を作製した。Example 9
A thermally conductive sheet 1 was produced in the same manner as in Example 1 except that the blending amounts of the raw material components were changed as shown in Table 1.
(実施例10)
第2熱伝導性フィラーとして、炭酸カルシウムからなるフィラー(丸尾カルシウム株式会社製「軽質炭酸カルシウム」(球状、粒径6μm、アスペクト比約1))を使用した以外は、実施例7と同様にして熱伝導性シート1を作製した。(Example 10)
Except that a filler made of calcium carbonate (“light calcium carbonate” manufactured by Maruo Calcium Co., Ltd. (spherical, particle size 6 μm, aspect ratio of about 1)) was used as the second thermally conductive filler, the same as in Example 7 was used. A thermally conductive sheet 1 was produced.
(実施例11)
第2熱伝導性フィラーとして、酸化マグネシウムからなるフィラー(神島化学工業株式会社製「スターマグMSL」(球状、粒径9μm、アスペクト比1))を使用した以外は、実施例7と同様にして熱伝導性シート1を作製した。(Example 11)
Heat was applied in the same manner as in Example 7 except that a filler made of magnesium oxide (“Starmag MSL” (spherical, particle size 9 μm, aspect ratio 1)) made of magnesium oxide was used as the second thermally conductive filler. A conductive sheet 1 was produced.
(比較例1、2)
原料成分の配合量を表1に示したように変更(第2熱伝導性フィラーを使用しなかった)した以外は、実施例1と同様にして熱伝導性シート1を作製した。(Comparative Examples 1 and 2)
A thermally conductive sheet 1 was produced in the same manner as in Example 1, except that the blending amounts of the raw material components were changed as shown in Table 1 (the second thermally conductive filler was not used).
[評価試験]
(1)硬度
得られた熱伝導性樹脂シートの硬度として、アスカーC硬度を測定した。結果を表1に示した。
(2)熱抵抗
得られた熱伝導性樹脂シートの厚さ方向の熱抵抗をTIM TESTER1300を用いて3水準の測定圧力(0.1MPa、0.3MPa及び0.5MPa)で計測した。計測された値を表1に示した。なお、当該測定は定常法にて米国規格ASTM D5470に準拠した。結果を表1に示した。[Evaluation test]
(1) Hardness The Asker C hardness was measured as the hardness of the obtained heat conductive resin sheet. The results are shown in Table 1.
(2) Thermal resistance The thermal resistance in the thickness direction of the obtained thermal conductive resin sheet was measured at three levels of measurement pressure (0.1 MPa, 0.3 MPa, and 0.5 MPa) using a TIM TESTER 1300. The measured values are shown in Table 1. In addition, the said measurement was based on the American standard ASTM D5470 by the stationary method. The results are shown in Table 1.
表1に示す結果から、本発明の実施形態によれば、高価なBNの使用量を減らしつつ、熱抵抗値の低い熱伝導性樹脂シートを提供することができることが明らかとなった。 From the results shown in Table 1, it became clear that according to the embodiment of the present invention, it is possible to provide a thermally conductive resin sheet having a low thermal resistance value while reducing the amount of expensive BN used.
1 熱伝導性シート
2 マトリックス成分
4 第1熱伝導性フィラー
5 第2熱伝導性フィラー
6 ウェルドライン
8 スクリュー
10 流路
12 第1ギャップ
14 第2ギャップ
100 押出機DESCRIPTION OF SYMBOLS 1 Thermal conductive sheet 2 Matrix component 4 1st thermal conductive filler 5 2nd thermal conductive filler 6 Weld line 8 Screw 10 Flow path 12 1st gap 14 2nd gap 100 Extruder
Claims (3)
前記熱伝導性フィラーの含有量は、30〜50体積%であり、
前記第1熱伝導性フィラーは、30μm以上の粒径及び10以上のアスペクト比を有する窒化ホウ素からなるフィラーであり、
前記第1熱伝導性フィラーの含有量は、5〜20体積%であり、
前記第2熱伝導性フィラーは、窒化ホウ素以外の材質からなるフィラーである
ことを特徴とする熱伝導性樹脂成型品。A thermally conductive resin molded article comprising a resin and a thermally conductive filler comprising a first thermally conductive filler and a second thermally conductive filler having a particle size smaller than the first thermally conductive filler,
The content of the thermally conductive filler is 30 to 50% by volume,
The first thermally conductive filler is a filler made of boron nitride having a particle size of 30 μm or more and an aspect ratio of 10 or more,
The content of the first thermally conductive filler is 5 to 20% by volume,
The thermally conductive resin molded product, wherein the second thermally conductive filler is a filler made of a material other than boron nitride.
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