WO2019026745A1 - 熱伝導性樹脂成型品 - Google Patents

熱伝導性樹脂成型品 Download PDF

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Publication number
WO2019026745A1
WO2019026745A1 PCT/JP2018/028025 JP2018028025W WO2019026745A1 WO 2019026745 A1 WO2019026745 A1 WO 2019026745A1 JP 2018028025 W JP2018028025 W JP 2018028025W WO 2019026745 A1 WO2019026745 A1 WO 2019026745A1
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Prior art keywords
thermally conductive
conductive filler
filler
sheet
gap
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PCT/JP2018/028025
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English (en)
French (fr)
Japanese (ja)
Inventor
孝太郎 山浦
史博 向
祐希 細川
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バンドー化学株式会社
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Application filed by バンドー化学株式会社 filed Critical バンドー化学株式会社
Priority to JP2018540879A priority Critical patent/JP6490877B1/ja
Priority to DE112018003897.1T priority patent/DE112018003897B4/de
Priority to CN201880048210.4A priority patent/CN110945082B/zh
Publication of WO2019026745A1 publication Critical patent/WO2019026745A1/ja

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    • 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
    • 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

Definitions

  • the present invention relates to a thermally conductive resin molded article.
  • Patent Document 1 discloses that a kneaded product containing scaly particles of a resin and / or rubber and boron nitride is extruded into a plurality of strip-like plasticizers, assembled by a lip and sheeted, and then cured or sheeted. While, a manufacturing method to cure is proposed.
  • Patent Document 2 discloses a silicone laminate containing 50 to 75% by volume of a thermally conductive filler containing two kinds of boron nitride powders (A) and (B) having different average particle sizes as a thermally conductive molded body. A heat conductive molded body has been proposed which is characterized in that it is cut from the laminating direction.
  • the resin molded product having thermal conductivity described in Patent Documents 1 and 2 preferably employs a filler made of boron nitride as the thermal conductive filler.
  • Boron nitride fillers have the advantage of being easy to impart excellent thermal conductivity.
  • boron nitride is expensive, and it is difficult to provide a resin molded product having thermal conductivity at low cost when it contains a large amount of filler made of boron nitride as in Patent Documents 1 and 2 above.
  • a filler made of boron nitride is used as the thermally conductive filler, it is difficult to orient the filler if the content of the filler is small.
  • the produced resin molded product has used the filler made from boron nitride, it had the subject that it was inferior to thermal conductivity.
  • the present invention has been made in view of such problems, and an object thereof is to provide a thermally conductive resin molded product having excellent thermal conductivity and capable of being manufactured inexpensively.
  • the thermally conductive resin molded article of the present invention is What is claimed is: 1.
  • 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 that of 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 diameter of 30 ⁇ m 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.
  • the thermally conductive resin molded article of the present invention is composed of a first thermally conductive filler consisting 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 smaller in diameter than 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 consisting of boron nitride is small, and the thermally conductive resin is molded The product is excellent in thermal conductivity. Moreover, the said heat conductive resin molded article can be provided cheaply.
  • the particle diameter of the second thermally conductive filler is preferably 3 to 20 ⁇ m.
  • the second thermally conductive filler is suitable for enhancing the thermal conductivity of the thermally conductive resin molded article by being interposed between the first thermally conductive fillers, and thermally conductive resin molding It is also suitable for orienting the first thermally conductive filler in the product manufacturing process.
  • the second thermally conductive filler is preferably made of magnesium oxide or magnesium carbonate.
  • the second thermally conductive filler is suitable for enhancing the thermal conductivity of the thermally conductive resin molded article by being interposed between the first thermally conductive fillers, and thermally conductive resin molding It is suitable to offer goods inexpensively.
  • the thermally conductive resin molded article of the present invention has excellent thermal conductivity. Moreover, the said heat conductive resin molded article can be provided cheaply.
  • a thermally conductive resin molded product refers to a block-like product produced by molding the raw material composition, and a cut product obtained by cutting the block-like product (a sliced sheet product Is a concept that includes any of In the present embodiment, an embodiment of a thermally conductive resin molded article will be described by taking a thermally conductive sheet as an example.
  • FIG. 1 is a cross-sectional view schematically showing a thermally conductive sheet according to an embodiment of the present invention, and is a cross-sectional view parallel to the thickness direction of the thermally conductive sheet.
  • FIG. 1 is a schematic diagram, and each member (especially the 1st thermally conductive filler and the 2nd thermally 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 one surface is in contact with the heat generating member and the other surface is in contact with the heat radiating member. To use.
  • the thermally conductive sheet 1 includes a matrix component 2, a first thermally conductive filler 4 and a second thermally conductive filler 5, and the first thermally conductive filler 4 is thermally
  • the conductive sheet 1 is oriented substantially in the thickness direction (vertical direction in FIG. 1).
  • a thermally conductive path by the first thermally conductive filler 4 and the second thermally conductive filler 5 is formed in the substantially thickness direction of the thermally conductive sheet 1. Therefore, the thermally conductive sheet 1 is excellent in thermal conductivity in the thickness direction.
  • components other than the heat conductive filler are collectively referred to as a matrix component.
  • the thermally conductive sheet 1 is sliced into a sheet of block-like material in which the thin resin sheet in which the first thermally conductive fillers 4 in the matrix component 2 are oriented and dispersed in the surface direction is folded in the vertical direction. It is a thing.
  • a weld line 6 may be formed on such a thermally conductive sheet 1 substantially in the thickness direction.
  • the matrix component 2 contains at least a resin (including rubber).
  • resin conventionally well-known various resin can be selected suitably and can be used.
  • ethylene- ⁇ -olefin copolymer such as polyethylene, polypropylene and ethylene-propylene copolymer, polymethylpentene, polyvinyl chloride, polyvinylidene chloride, polyvinyl acetate, ethylene-vinyl acetate co-weight Combination, polyvinyl alcohol, polyacetal, fluorocarbon resin 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,
  • styrene-butadiene copolymer or hydrogenated polymer thereof styrene-based thermoplastic elastomer such as styrene-isoprene block copolymer or hydrogenated polymer thereof, olefin-based thermoplastic elastomer, vinyl chloride-based thermoplastic elastomer, polyester Thermoplastic elastomers, polyurethane thermoplastic elastomers, polyamide thermoplastic elastomers, etc.
  • silicone rubber, acrylic rubber, butyl rubber, fluororubber, nitrile rubber, hydrogenated nitrile rubber and the like can also be used. These may be used alone or in combination of two or more. Among these, silicone rubber is preferable in terms of flexibility in forming a molded product, shape followability, adhesion to a heat generating surface when contacting an electronic component, and heat resistance.
  • silicone rubber what the polymer (silicone) which has silicone frame
  • the crosslinking of silicone may be peroxide crosslinking or addition reaction type crosslinking, but peroxide crosslinking is preferable. This is because silicone rubber crosslinked by peroxide crosslinking is more excellent in heat resistance.
  • the silicone rubber for example, a peroxide-crosslinked mixture of a silicone having all methyl groups and no unsaturated group and a silicone having a vinyl group as part of the side chains (including the end).
  • the silicone having a vinyl group in a part of the side chain can also be regarded as a cross-linking agent for silicone in which all the side chains are methyl groups and which do not contain an unsaturated group.
  • silicone having a vinyl group in part of the side chain are, for example, dimethylpolysiloxane capped with dimethylvinylsiloxy at both ends of molecular chain, dimethylpolysiloxane capped with methylphenylvinylsiloxy at both ends of molecular chain, both molecular chains Terminal dimethylvinylsiloxy group-capped dimethylsiloxane / methylphenylsiloxane copolymer, molecular chain both terminal dimethylvinylsiloxy group-capped dimethylsiloxane / methylvinylsiloxane copolymer, molecular chain both terminally trimethylsiloxy group-blocked dimethylsiloxane / methylvinylsiloxane co-polymer Polymer, both-end dimethylvinylsiloxy-blocked methyl (3,3,3-trifluoropropyl) polysiloxane, both-end silanol group blocked dimethyls
  • organic peroxide at the time of performing the above-mentioned peroxide crosslinking examples include benzoyl peroxide, dicumyl peroxide, 2,5-dimethyl-2,5-di (t-butylperoxy) hexane, di-t Butyl peroxide, t-butyl perbenzoate and the like. These may be used alone or in combination of two or more. Furthermore, at the time of crosslinking, a crosslinking accelerator or a crosslinking accelerator may be used in combination.
  • the matrix component 2 may contain, in addition to the above-described resin, a crosslinking agent, a crosslinking accelerator, and a crosslinking accelerator as described above. Moreover, the matrix component 2 is a general additive such as a reinforcing agent, a filler, a softener, a plasticizer, an antiaging agent, a tackifier, an antistatic agent, a kneading agent, a flame retardant, and a coupling agent. You may contain.
  • the thermally conductive sheet 1 contains a first thermally conductive filler 4 and a second thermally conductive filler 5 smaller in particle size than 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 thermally conductive sheet 1 has excellent thermal conductivity.
  • the shape of the first thermally conductive filler 4 is not particularly limited as long as it has a predetermined particle diameter and aspect ratio.
  • As a specific shape of the 1st heat conductive filler 4 scaly shape, plate shape, film shape, fibrous shape, cylindrical shape, prismatic shape, elliptical shape, flat shape etc. are mentioned, for example. Among these, scaly is preferable. This is because the thermal conductivity of the molded article is high when the scale-like thermally conductive filler is oriented because it has a high aspect ratio and an isotropic thermal conductivity in the surface direction.
  • the particle diameter of the first heat conductive filler 4 is 30 ⁇ m or more. If the particle diameter is less than 30 ⁇ m, it is difficult to form a heat conduction path, and the heat conductivity may be poor. On the other hand, the preferable upper limit of the particle diameter of the 1st heat conductive filler 4 is 100 micrometers from a viewpoint of the workability at the time of producing a heat conductive resin molded product.
  • the aspect ratio of the first thermally conductive filler 4 is 10 or more.
  • the second thermally conductive filler 5 having a particle diameter smaller than that of the first thermally conductive filler 4 is dispersed in the gaps of the first thermally conductive filler 4 to easily form a thermally conductive path, and the first heat The conductive filler 4 is easy to be oriented in the matrix component 2.
  • the upper limit of the aspect ratio of the first heat conductive filler 4 is preferably 100. In this case, the first thermally conductive filler can be easily filled into the thermally conductive resin molded product, and the processability at the time of producing the thermally conductive resin molded product is also excellent.
  • the “particle size” of the thermally conductive filler is the concept of the average particle size in the particle size distribution measurement.
  • the average particle size is measured by a laser diffraction scattering method (apparatus: Microtrac MT3300EXII manufactured by Microtrac Bell Inc.).
  • the “aspect ratio” of the thermally conductive filler is a concept of the average value of the ratio of the major axis to the minor axis. The above-mentioned aspect ratio arbitrarily selects 200 or more particles from the image photographed by SEM, calculates the ratio of the major axis to the minor axis, and calculates the average value.
  • the length of the longest portion is the major axis
  • the length of a portion passing through the middle point of this major axis and orthogonal to the major axis is the minor axis.
  • the second thermally conductive filler 5 has a particle size smaller than that of the first thermally conductive filler, and is made of a material 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 heat 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, What consists of molybdenum disulfide, copper, aluminum etc. is mentioned.
  • a heat conductive filler made of magnesium oxide and a heat conductive filler made of magnesium carbonate are preferable. It is because it intervenes between the first thermally conductive fillers 4 to be suitable for enhancing the thermal conductivity of the thermally conductive sheet 1 and suitable for providing the thermally conductive sheet 1 at low cost. .
  • the shape of the second heat conductive filler 5 is not particularly limited, and specific shapes include, for example, a spherical shape, a scaly shape, a plate shape, a film shape, a columnar shape, a prismatic shape, an elliptical shape, and a flat shape. .
  • 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 suitable for orienting the first heat conductive fillers 4.
  • the particle diameter of the second thermally conductive filler 5 is not particularly limited as long as it is smaller than the particle diameter of the first thermally conductive filler 4, but 3 to 20 ⁇ m is preferable.
  • a thermally conductive path is formed to be interposed between the first thermally conductive fillers 4, and the first thermally conductive filler 4 is oriented It is more suitable to Furthermore, when the particle diameter of the second thermally conductive filler 5 is in this range, the surface roughness of the thermally conductive sheet 1 is suppressed, and the contact thermal resistance (thermally conductive sheet 1) when in contact with the heat generating member or the heat radiating member Suitable for reducing the thermal resistance of the surface of On the other hand, if the particle size of the second thermally conductive filler 5 exceeds 20 ⁇ m, the first thermally conductive filler 4 is difficult to be oriented, and the thermally conductive sheet 1 may be inferior in thermal conductivity.
  • the thermally conductive sheet 1 may be inferior in thermal conductivity depending on the material of the second thermally conductive filler 5.
  • 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 process of producing the thermally conductive sheet 1, and such foaming is If produced, the thermal conductivity of the produced thermally conductive sheet 1 may be reduced.
  • the particle diameter of the second thermally conductive filler 5 is more preferably 5 to 20 ⁇ m, still more preferably 5 to 15 ⁇ m, and particularly preferably 5 to 10 ⁇ m.
  • the upper limit of the aspect ratio of the second thermally conductive filler 5 is preferably 100. This is because the second thermally conductive filler can be easily filled into the thermally conductive resin molded article, and the processability at the time of producing the thermally conductive resin molded article is also 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 each of the particle diameter and the aspect ratio of the second heat conductive filler 5 is the same as the measuring method of the particle diameter and the aspect ratio of the first heat conductive filler 4.
  • the content of the thermally conductive filler in the thermally conductive sheet 1 (the total content of the thermally conductive filler) is 30 to 50% by volume. If the total content of the thermally conductive filler is less than 30% by volume, sufficient thermal conductivity can not be ensured. In addition, when the content exceeds 50% by volume, the processability at the time of producing a thermally conductive resin molded article is inferior, and it is difficult to provide a thermally conductive resin molded article at low cost. Become.
  • the content of the first thermally conductive filler 4 in the thermally conductive sheet 1 is 5 to 20% by volume. In this case, the thermal conductivity can be secured by orienting the first thermally conductive filler. On the other hand, if the content of the first thermally conductive filler 4 is less than 5% by volume, sufficient thermal conductivity can not be ensured even if the first thermally conductive filler is oriented. Moreover, when the said content exceeds 20 volume%, it is difficult to provide a heat conductive resin molded product in low cost.
  • the content of the second thermally conductive filler 5 in the thermally conductive sheet 1 is preferably 10 to 45% by volume.
  • the content of the second thermally conductive filler 5 is less than 10% by volume, it becomes difficult to orient the first thermally conductive filler at the time of molding.
  • the content of the second thermally conductive filler 5 exceeds 45% by volume, the content of the first thermally conductive filler is too small, and sufficient thermal conductivity can not be ensured.
  • the content of the second thermally conductive filler 5 is more preferably 20 to 45% by volume.
  • the thermally conductive sheet 1 of the present embodiment contains a first thermally conductive filler 4 and a second thermally conductive filler 5 as a thermally conductive filler.
  • the particle diameter D1 of the first thermally conductive filler 4 and the particle diameter D2 of the second thermally conductive filler 5 have a relationship of D1> D2.
  • the thermally conductive sheet 1 may contain thermally conductive fillers other than the 1st thermally conductive filler 4 and the 2nd thermally conductive filler 5 in the range which does not impair the effect of this invention.
  • the thickness of the thermally conductive sheet 1 is not particularly limited, and is, for example, about 0.1 to 3.0 mm.
  • the heat conductive sheet 1 can be suitably used as a member for efficiently transmitting heat between the heat generating member and the heat dissipating member in an electric part, an automobile part or the like.
  • FIG. 2 is a figure which shows typically the extruder used by manufacture of the heat conductive sheet which concerns on embodiment of this invention.
  • FIG. 2 shows a schematic cross-sectional view of the tip portion of the extruder 100 and the T-die.
  • 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.
  • the raw material composition supplied to the extruder 100 is first squeezed in the vertical direction (thickness direction) by the first gap 12 to form a thin strip.
  • shear 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.
  • the first thermally conductive filler is oriented in the surface direction of the resin sheet precursor.
  • the second thermally conductive filler is oriented in the same direction as the first thermally conductive filler when passing through the first gap 12.
  • the gap (the dimension in the vertical direction in FIG. 2) of the first gap 12 is preferably 0.1 mm or more and 5.0 mm or less. If the gap of the first gap 12 is smaller than 0.1 mm, the extrusion pressure may increase unnecessarily, and further, resin clogging may occur. On the other hand, if the gap of the first gap 12 is larger than 5.0 mm, the degree of orientation of the thermally conductive filler in the surface direction of the thin resin sheet precursor may be reduced.
  • the flow direction of the sheet which has been limited in 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 path 10 after passing through the first gap 12 is expanded, and the length in the vertical direction of the flow path 10 is increased.
  • the thin resin sheet precursor in which the flow direction of the sheet is changed to be substantially perpendicular to the extrusion direction is further extruded toward the second gap 14 after completely passing through the first gap 12. As a result, the resin sheet precursor in the second gap 14 is in a state in which the thin resin sheet precursor is laminated.
  • the resin sheet precursor is heated under predetermined conditions to advance crosslinking, and further, as required, the resin sheet precursor is sliced in the direction perpendicular to the thickness direction.
  • the heat conductive sheet 1 is manufactured through such a process.
  • the gap of the second gap 14 is preferably twice or more and 20 times or less the gap of the first gap 12. If 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 where the resin sheet precursor is partially turbulent flows easily, and as a result, the heat conductive sheet 1 The proportion of the first thermally conductive filler 4 oriented in the thickness direction may be reduced.
  • the gap of the second gap 14 is more preferably twice or more and 10 times or less than the gap of the first gap 12. Further, from the viewpoint of facilitating uniform flow of the resin sheet precursor 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 have a thickness It is preferable to be at substantially the same position in the direction.
  • the shape of the opening connected to the first gap 12 is not particularly limited, but the side surfaces (upper and lower surfaces) of the opening on the upstream side are preferably inclined to reduce pressure loss.
  • the inclination angle (the angle between the extrusion direction and the inclined surface) for upper and lower surfaces).
  • the inclination angle may be, for example, 10 ° to 50 °, and more preferably 20 ° to 25 °.
  • the opening connected to the first gap 12 does not have to be inclined at both the upper and lower sides, and only one of them may have the inclination.
  • the depths of the first gap 12 and the second gap 14 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 are possible according to the product width of the resin sheet.
  • the thermally conductive sheet according to the embodiment of the present invention can also be manufactured by the following manufacturing method. That is, after preparing a raw material composition for producing a thermally conductive sheet, using the raw material composition, a plurality of sheet materials in which at least the first thermally conductive filler is oriented in the plane direction are obtained by a conventionally known method A plurality of sheet-like materials are laminated to form a block-like material, and then the block-like material (laminate of sheet materials) from the direction perpendicular to the direction in which the first thermally conductive filler is oriented It may be produced by cutting. When manufacturing a heat conductive sheet by this method, you may perform a crosslinking process at an appropriate timing as needed.
  • the thermally conductive sheet produced by such a method is also a sheet excellent in thermal conductivity in which the first thermally conductive filler is oriented in the substantially thickness direction of the thermally conductive sheet.
  • Example 1 In the composition described in Table 1, the resin component is mixed with a cross-linking agent and a first heat conductive filler and a second heat conductive filler (hereinafter, all are collectively referred to as a raw material component) by two rolls, and a ribbon A sheet (composition as a precursor) was obtained.
  • a cross-linking agent a first heat conductive filler and a second heat conductive filler (hereinafter, all are collectively referred to as a raw material component) by two rolls, and a ribbon A sheet (composition as a precursor) was obtained.
  • silicone rubber “DY321005U manufactured by Toray Dow Corning” and a plasticizer (silicone oil manufactured by Shin-Etsu Chemical Co., Ltd .: KF-96-3000CS) were used.
  • MR-53 and “RC-450P FD” manufactured by Toray Dow Corneg were used.
  • Table 1 shows the total content.
  • XGP boron nitride
  • the second heat conductive filler a filler made of magnesium carbonate (cube shape, particle diameter 6 ⁇ m, aspect ratio about 1 (manufactured by Kamijima Chemical Co., Ltd.)) was used.
  • the ribbon sheet produced was prepared using a vertically oriented mold (die) having a first gap of 1 mm and a second gap of 10 mm.
  • the sheet after the crosslinking treatment was sliced in the direction perpendicular to the thickness direction to prepare a thermally conductive sheet 1 as a thermally conductive resin molded product with a thickness of 500 ⁇ m.
  • 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.
  • Example 3 As a second heat conductive filler, a filler made of magnesium carbonate (cube shape, particle diameter 15 ⁇ m, aspect ratio about 1 (manufactured by Kamijima Chemical Industries Co., Ltd.)) was used, and the blending amounts of the raw material components are shown in Table 1 A thermally conductive sheet 1 was produced in the same manner as in Example 1 except that it was changed as described above.
  • 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.
  • Example 5 As a second heat conductive filler, a filler made of magnesium oxide (“SMO” (spherical, particle size 10 ⁇ m, aspect ratio about 1) manufactured by Sakai Chemical Industry Co., Ltd.) is used, and the blending amounts of raw material components are shown in Table 1 A thermally conductive sheet 1 was produced in the same manner as in Example 1 except that it was changed as shown in.
  • SMO magnesium oxide
  • 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.
  • Example 7 As a second heat conductive filler, a filler made of magnesium carbonate (cube shape, particle diameter 26 ⁇ m, aspect ratio about 1 (made by Kamijima Chemical Co., Ltd.)) was used, and the blending amounts of the raw material components are shown in Table 1 A thermally conductive sheet 1 was produced in the same manner as in Example 1 except that it was changed as described above.
  • 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.
  • 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.
  • Example 10 The same procedure as in Example 7 was followed, except that a filler consisting of calcium carbonate ("Light calcium carbonate” (spherical, particle size 6 ⁇ m, aspect ratio about 1) manufactured by Maruo Calcium Co., Ltd.) was used as the second thermally conductive filler.
  • a thermally conductive sheet 1 was produced.
  • Example 11 The same procedure as in Example 7 was followed, except that a filler made of magnesium oxide (“Starmag MSL” (spherical, particle size 9 ⁇ m, aspect ratio 1) manufactured by Kamijima Chemical Industry Co., Ltd.) was used as the second thermally conductive filler.
  • the conductive sheet 1 was produced.
  • thermoly 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).
  • thermally conductive sheet 2 matrix component 4 first thermally conductive filler 5 second thermally conductive filler 6 weld line 8 screw 10 flow path 12 first gap 14 second gap 100 extruder

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