WO2021059567A1 - シーリング材用熱伝導シート及びこれを組み込んだ発熱性電気・電子部品 - Google Patents

シーリング材用熱伝導シート及びこれを組み込んだ発熱性電気・電子部品 Download PDF

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WO2021059567A1
WO2021059567A1 PCT/JP2020/015092 JP2020015092W WO2021059567A1 WO 2021059567 A1 WO2021059567 A1 WO 2021059567A1 JP 2020015092 W JP2020015092 W JP 2020015092W WO 2021059567 A1 WO2021059567 A1 WO 2021059567A1
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Prior art keywords
heat
heat conductive
electronic component
sheet
group
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English (en)
French (fr)
Japanese (ja)
Inventor
服部真和
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Fuji Polymer Industries Co Ltd
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Fuji Polymer Industries Co Ltd
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Priority to CN202080005605.3A priority Critical patent/CN112840498A/zh
Priority to EP20859619.7A priority patent/EP3836292A4/en
Priority to US17/210,054 priority patent/US20210210814A1/en
Publication of WO2021059567A1 publication Critical patent/WO2021059567A1/ja
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/183—Sealing members
    • H01M50/19—Sealing members characterised by the material
    • H01M50/198—Sealing members characterised by the material characterised by physical properties, e.g. adhesiveness or hardness
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/61—Types of temperature control
    • H01M10/613—Cooling or keeping cold
    • 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
    • C08G77/48—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 in which at least two but not all the silicon atoms are connected by linkages other than oxygen atoms
    • C08G77/50—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 in which at least two but not all the silicon atoms are connected by linkages other than oxygen atoms by carbon linkages
    • 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
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
    • C09K5/08—Materials not undergoing a change of physical state when used
    • C09K5/14—Solid materials, e.g. powdery or granular
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/62—Heating or cooling; Temperature control specially adapted for specific applications
    • H01M10/625—Vehicles
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/65—Means for temperature control structurally associated with the cells
    • H01M10/651—Means for temperature control structurally associated with the cells characterised by parameters specified by a numeric value or mathematical formula, e.g. ratios, sizes or concentrations
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/65—Means for temperature control structurally associated with the cells
    • H01M10/653—Means for temperature control structurally associated with the cells characterised by electrically insulating or thermally conductive materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/65—Means for temperature control structurally associated with the cells
    • H01M10/655—Solid structures for heat exchange or heat conduction
    • H01M10/6552—Closed pipes transferring heat by thermal conductivity or phase transition, e.g. heat pipes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/65—Means for temperature control structurally associated with the cells
    • H01M10/655—Solid structures for heat exchange or heat conduction
    • H01M10/6556—Solid parts with flow channel passages or pipes for heat exchange
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/65—Means for temperature control structurally associated with the cells
    • H01M10/656—Means for temperature control structurally associated with the cells characterised by the type of heat-exchange fluid
    • H01M10/6567—Liquids
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/183—Sealing members
    • H01M50/184—Sealing members characterised by their shape or structure
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/183—Sealing members
    • H01M50/19—Sealing members characterised by the material
    • H01M50/195—Composite material consisting of a mixture of organic and inorganic materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/204—Racks, modules or packs for multiple batteries or multiple cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/249—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders specially adapted for aircraft or vehicles, e.g. cars or trains
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
    • C08K3/20—Oxides; Hydroxides
    • C08K3/22—Oxides; Hydroxides of metals
    • C08K2003/2227—Oxides; Hydroxides of metals of aluminium
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K2201/00—Specific properties of additives
    • C08K2201/001—Conductive additives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present invention relates to a heat conductive sheet for a sealing material useful for an in-vehicle battery module or the like and a heat-generating electric / electronic component incorporating the heat conductive sheet.
  • a plurality of single batteries (storage elements) are arranged and electrically connected.
  • the power generation element of the cell is housed in the case.
  • heat is generated from the power generation element. If this heat accumulates in the cell and the temperature of the cell rises, there is a concern that the battery performance will deteriorate. Further, in the case of an assembled battery, there is a concern that the temperature of each cell will vary due to heat generation, and that the progress of deterioration of battery performance will also differ.
  • Patent Document 1 proposes arranging a bag body in which a silicone gel is sealed in a bag of a resin film between a cell assembly and a storage container.
  • Patent Document 3 proposes arranging an insulating heat-dissipating gel member between the cell and the storage container.
  • the heat radiating material between the conventional battery and the storage container has the following problems.
  • (1) The heat conductive sheet has a problem that it is difficult to fill the space between the battery module and the case without a gap.
  • the present invention can prevent the liquid material from leaking even if the heat conductive liquid material is directly injected between the heat-generating electrical / electronic component such as a battery module and the case.
  • a heat conductive sheet for sealing materials that has a level of flexibility that does not impose a load on heat-generating electrical / electronic components and has high adhesion between the heat-generating electrical / electronic components and the case, and heat-generating electrical / electronic components that incorporate this. Provide parts.
  • the heat conductive sheet for a sealing material of the present invention is a heat conductive sheet for a sealing material arranged between a heat-generating electric / electronic component and a heat radiating case, and the hardness of the sheet is 5 or more and 55 or less on a shore 00.
  • the sheet is a frame-shaped sheet, and the inside of the frame is a space for filling the liquid heat conductive composition.
  • the heat-generating electric / electronic component of the present invention is a heat-generating electric / electronic component incorporating the heat-conducting sheet for a sealing material, and the heat-conducting sheet is formed between the heat-generating electric / electronic component and the case. It is characterized in that the space between the heat-generating electrical / electronic component, the case, and the heat-conducting sheet is filled with the liquid heat-conducting composition.
  • the heat conductive sheet for a sealing material of the present invention has a hardness of 5 or more and 55 or less on a shore 00, the sheet is a frame-shaped sheet, and the inside of the frame is a space for filling a liquid heat conductive composition.
  • the liquid heat conductive composition does not leak even when the heat conductive liquid material is directly injected between the heat-generating electric / electronic component and the case, or even during operation after mounting, and the heat-generating electricity is generated.
  • -It is possible to provide a heat-generating electrical / electronic component that has a level of flexibility that does not impose a load on the electronic component and has a high degree of adhesion between the heat-generating electric / electronic component and the case.
  • the sheet is attached between the heat-generating electric / electronic component and the case, and the heat-generating electric / electronic component, the case, and the heat-conducting sheet are attached to each other. Since the space is filled with the liquid heat conductive composition, it is possible to provide a heat generating electric / electronic component having high adhesion between the heat generating electric / electronic component and the case and having high heat dissipation.
  • FIG. 1 is a schematic perspective view of a heat conductive sheet for a sealing material according to an embodiment of the present invention.
  • FIG. 2A is a schematic perspective view in which the heat conductive sheet for the sealing material of one embodiment of the present invention is attached to the battery module
  • FIG. 2B is the same
  • FIG. 2C is a schematic perspective view in which the battery module is put in a case
  • FIG. 2C is FIG. 2B.
  • FIG. 1I is a cross-sectional view taken along the line II, showing a state in which a liquid heat conductive composition is filled in a space between a heat conductive sheet for a sealing material, a battery module, and a case.
  • FIG. 3A and 3B are explanatory views showing a method of measuring the thermal conductivity of the heat conductive sheet according to the embodiment of the present invention.
  • FIG. 4A-B is a photograph showing a pressure resistance test method when a liquid heat conductive composition is filled in a heat conductive sheet for a sealing material according to an embodiment of the present invention.
  • the present invention is a heat conductive sheet for a sealing material arranged between a heat-generating electric / electronic component and a case, and this sheet is a frame-shaped sheet for filling the inside of the frame with a liquid heat conductive composition. It is a space part. The space is filled with a liquid heat conductive composition. Therefore, the hardness of the sheet is 5 or more on the shore 00. As a result, even if the space is filled with the liquid heat conductive composition under pressure, it can be prevented from overflowing to the outside of the sheet.
  • the sheet is sandwiched between the heat-generating electric / electronic component and the heat-dissipating case, it has a level of flexibility that does not impose a load on the heat-generating electric / electronic component, has good adhesion, and is a liquid heat conductive composition.
  • the hardness is preferably 55 or less because the sheet shape is maintained even if the sheet is filled with.
  • the preferred hardness is 7 to 40 on Shore 00, more preferably 10 to 30.
  • the sheet is preferably frame-shaped. If it has a frame shape, the liquid heat conductive composition can be filled in the internal space.
  • the size, width, and frame shape of the frame can be selected according to the shape of the heat-generating electrical / electronic component. As an example, in the case of an in-vehicle lithium battery module, it is rectangular. In addition, it can be molded into various shapes such as circles and polygons other than rectangles.
  • the thickness of the sheet is preferably 0.2 to 5 mm, more preferably 0.3 to 4 mm, and even more preferably 0.5 to 3 mm. With the above thickness, it is convenient to sandwich the heat-generating electrical / electronic component and the heat radiating case, and it is possible to prevent liquid leakage when filling the liquid heat conductive composition.
  • the width of the sheet can be arbitrary, but is preferably 1 to 50 mm. Similarly, the width is convenient for sandwiching between the heat-generating electrical / electronic component and the heat-dissipating case, and it is possible to prevent liquid leakage when filling the liquid heat conductive composition.
  • the thermal conductivity of the heat conductive sheet is preferably 0.8 W / m ⁇ K or more, and more preferably 1.0 W / m ⁇ K or more. If the thermal conductivity is 0.8 W / m ⁇ K or more, it is suitable for conducting heat from the heat generating portion to the radiator.
  • the heat-generating electrical / electronic component can be applied to any semiconductor such as a power module or any heat-generating electric / electronic component such as a lithium battery module.
  • any semiconductor such as a power module or any heat-generating electric / electronic component such as a lithium battery module.
  • an in-vehicle lithium battery module generates a lot of heat and is suitable for applying the present invention.
  • the matrix resin of the heat conductive sheet is preferably a silicone polymer. Silicone polymers have high heat resistance and have been put to practical use as thermal interface materials (TIM) materials for various heat-generating electrical and electronic components.
  • TIM thermal interface materials
  • the matrix resin contains a cross-linking component and a catalyst component, and is preferably an addition-curable silicone polymer. This is because it has a good affinity with the liquid heat conductive composition filled in the space of the heat conductive sheet.
  • the heat-conducting sheet is attached between the heat-generating electric / electronic component and the case, and the heat-generating electric / electronic component, the case, and the heat-conducting sheet are attached to each other.
  • the space is filled with a liquid heat conductive composition.
  • a radiating fin or a cooling device may be provided on the outside of the case. After filling the space with the liquid heat conductive composition, the liquid heat conductive composition may remain uncured or may be cured.
  • the liquid heat conductive composition is a silicone polymer as the matrix resin, and the composition containing the heat conductive material particles is preferably 0.8 W / m ⁇ K or more, more preferably 1.0 W / m ⁇ K. That is all. If the thermal conductivity is 0.8 W / m ⁇ K or more, it is suitable for conducting heat from the heat generating portion to the radiator.
  • Thermally conductive particles are mixed in the matrix resin of the heat conductive sheet used in the present invention and the matrix resin of the liquid heat conductive composition.
  • the thermally conductive particles are preferably inorganic particles such as alumina, zinc oxide, magnesium oxide, aluminum nitride, boron nitride, aluminum hydroxide, and silica. These inorganic particles may be added alone or in combination of two or more.
  • the matrix resin is 100 parts by mass
  • the heat conductive particles are preferably added in an amount of 100 to 4000 parts by mass, more preferably 500 to 3000 parts by mass.
  • the thermally conductive particles used in the present invention may be partially or wholly surface-treated with a silane coupling agent.
  • the silane coupling agent may be mixed with the heat conductive particles in advance and pretreated, or may be added when the matrix resin, the curing catalyst and the heat conductive particles are mixed (integral blend method).
  • integral blend method 0.01 to 10 parts by mass of the silane coupling agent is added to 100 parts by mass of the heat conductive particles not surface-treated used in the heat-resistant heat conductive composition of the present invention. It is preferable to add it.
  • the surface treatment makes it easier to mix with the matrix resin, and also has the effect of preventing the curing catalyst from being adsorbed on the heat conductive particles and preventing curing inhibition. This is useful for storage stability.
  • the dielectric breakdown voltage (JIS K6249) of the heat conductive sheet is preferably 11 to 16 kV / mm. As a result, a heat-resistant heat conductive sheet having high electrical insulation can be obtained.
  • the heat conductive sheet of the present invention preferably contains the following components (A) to (D), and is preferably mixed with components (E), (F), (G) and the like as optional components and cured (crosslinked).
  • the matrix component is an organopolysiloxane containing two or more alkenyl groups bonded to silicon atoms in one molecule, and the organopolysiloxane containing two alkenyl groups is the main agent (base polymer) in the silicone gel composition of the present invention.
  • Ingredient This organopolysiloxane has two or more alkenyl groups bonded to silicon atoms, such as vinyl group and allyl group, having 2 to 8 carbon atoms, particularly 2 to 6, as alkenyl groups.
  • the viscosity is preferably 10 to 100,000 mPa ⁇ s at 25 ° C., particularly 100 to 10,000 mPa ⁇ s, from the viewpoint of workability and curability.
  • an organopolysiloxane containing an average of two or more alkenyl groups bonded to silicon atoms at both ends of the molecular chain is used in one molecule represented by the following general formula (Chemical formula 1).
  • the side chain is a linear organopolysiloxane sealed with an alkyl group.
  • a viscosity at 25 ° C. of 10 to 100,000 mPa ⁇ s is desirable from the viewpoint of workability and curability.
  • the linear organopolysiloxane may contain a small amount of branched structure (trifunctional siloxane unit) in the molecular chain.
  • R 1 is an unsubstituted or substituted monovalent hydrocarbon group that does not have the same or different aliphatic unsaturated bonds
  • R 2 is an alkenyl group
  • k is 0 or a positive integer.
  • the unsubstituted or substituted monovalent hydrocarbon group having no aliphatic unsaturated bond of R 1 for example, one having 1 to 10 carbon atoms, particularly 1 to 6 is preferable, and specifically, , Methyl group, ethyl group, propyl group, isopropyl group, butyl group, isobutyl group, tert-butyl group, pentyl group, neopentyl group, hexyl group, cyclohexyl group, octyl group, nonyl group, decyl group and other alkyl groups, phenyl Aryl groups such as groups, trill groups, xsilyl groups and naphthyl groups, aralky
  • Examples thereof include those substituted with a halogen atom, a cyano group, etc., such as a halogen-substituted alkyl group such as a chloromethyl group, a chloropropyl group, a bromoethyl group, and a trifluoropropyl group, and a cyanoethyl group.
  • a halogen-substituted alkyl group such as a chloromethyl group, a chloropropyl group, a bromoethyl group, and a trifluoropropyl group, and a cyanoethyl group.
  • alkenyl group of R 2 for example, those having 2 to 8 carbon atoms, particularly 2 to 6 are preferable, and specifically, a vinyl group, an allyl group, a propenyl group, an isopropenyl group, a butenyl group, an isobutenyl group and a hexenyl group.
  • k is generally 0 or a positive integer satisfying 0 ⁇ k ⁇ 10000, preferably 5 ⁇ k ⁇ 2000, and more preferably 10 ⁇ k ⁇ 1200. It is a positive integer.
  • the organopolysiloxane of component A contains 3 or more alkenyl groups bonded to silicon atoms having 2 to 8 carbon atoms such as vinyl group and allyl group, particularly 2 to 6 in one molecule, usually 3 to 30. , Preferably, an organopolysiloxane having about 3 to 20 may be used in combination.
  • the molecular structure may be any of linear, cyclic, branched, and three-dimensional network-like molecular structures.
  • the main chain consists of repeating diorganosiloxane units, both ends of the molecular chain are sealed with triorganosyloxy groups, and the viscosity at 25 ° C. is 10 to 100,000 mPa ⁇ s, especially 100 to 10,000 mPa ⁇ s.
  • s is a linear organopolysiloxane.
  • the alkenyl group may be attached to any part of the molecule.
  • those bonded to a silicon atom at the end of the molecular chain or at the non-end of the molecular chain (in the middle of the molecular chain) may be included.
  • each having 1 to 3 alkenyl groups on the silicon atoms at both ends of the molecular chain represented by the following general formula (Chemical Formula 2) (however, the alkenyl group bonded to the silicon atom at the end of the molecular chain is If the total number of both ends is less than 3, the direct group having at least one alkenyl group bonded to a silicon atom at the non-terminal of the molecular chain (in the middle of the molecular chain) (for example, as a substituent in the diorganosiloxane unit).
  • the linear organopolysiloxane may contain a small amount of branched structure (trifunctional siloxane unit) in the molecular chain.
  • R 3 is an unsubstituted or substituted monovalent hydrocarbon group which is the same as or different from each other, and at least one is an alkenyl group.
  • R 4 is an unsubstituted or substituted monovalent hydrocarbon group having no identical or heterologous aliphatic unsaturated bond
  • R 5 is an alkenyl group
  • l and m are 0 or positive integers.
  • the monovalent hydrocarbon group of R 3 preferably has 1 to 10 carbon atoms, particularly 1 to 6, and specifically, a methyl group, an ethyl group, a propyl group, an isopropyl group, a butyl group, and the like.
  • Alkyl groups such as isobutyl group, tert-butyl group, pentyl group, neopentyl group, hexyl group, cyclohexyl group, octyl group, nonyl group and decyl group, aryl group such as phenyl group, tolyl group, xsilyl group and naphthyl group, benzyl Aralkyl groups such as groups, phenylethyl groups and phenylpropyl groups, vinyl groups, allyl groups, propenyl groups, isopropenyl groups, butenyl groups, hexenyl groups, cyclohexenyl groups, octenyl groups and other alkenyl groups, and hydrogens of these groups.
  • halogen atoms such as fluorine, bromine and chlorine, cyano groups, etc.
  • halogen-substituted alkyl groups such as chloromethyl group, chloropropyl group, bromoethyl group, trifluoropropyl group and cyanoethyl group. And so on.
  • the monovalent hydrocarbon group of R 4 those having 1 to 10 carbon atoms, particularly 1 to 6 are preferable, and the same group as the specific example of R 1 can be exemplified, but the alkenyl group is not included. ..
  • the alkenyl group of R 5 for example, a group having 2 to 8 carbon atoms, particularly a group having 2 to 6 carbon atoms is preferable, and specifically, the same group as R 2 of the above formula (Chemical Formula 1) is exemplified, and a vinyl group is preferable. Is.
  • l, m are generally 0 or a positive integer satisfying 0 ⁇ l + m ⁇ 10000, preferably 5 ⁇ l + m ⁇ 2000, more preferably 10 ⁇ l + m ⁇ 1200, and 0 ⁇ l / (l + m). ) ⁇ 0.2, preferably 0.0011 ⁇ l / (l + m) ⁇ 0.1.
  • the organohydrogenpolysiloxane of the B component of the present invention acts as a cross-linking agent, and a cured product is formed by an addition reaction (hydrosilylation) between the SiH group in this component and the alkenyl group in the A component. It is a thing.
  • the organohydrogenpolysiloxane may be any as long as it has two or more hydrogen atoms (that is, SiH groups) bonded to silicon atoms in one molecule, and the molecular structure of this organohydrogenpolysiloxane is , Linear, cyclic, branched, or three-dimensional network structure, but the number of silicon atoms in one molecule (that is, the degree of polymerization) is 2 to 1000, especially about 2 to 300. Can be used.
  • the position of the silicon atom to which the hydrogen atom is bonded is not particularly limited, and may be the end of the molecular chain or the non-end (in the middle).
  • Examples of the organic group bonded to the silicon atom other than the hydrogen atom include an unsubstituted or substituted monovalent hydrocarbon group having no aliphatic unsaturated bond similar to R 1 of the general formula (Chemical formula 1). ..
  • organohydrogenpolysiloxane of the B component the following general formula (Chemical Formula 3) can be exemplified.
  • R 6 is the same or different alkyl group, phenyl group, epoxy group, acryloyl group, metaacryloyl group, alkoxy group, hydrogen atom, and at least two are hydrogen atoms.
  • L is an integer of 0 to 1,000, particularly an integer of 0 to 300, and M is an integer of 1 to 200.
  • R 6 of the side chain portion is a methyl group
  • R 6 at both ends are hydrogen.
  • the catalyst component of the C component is a component that promotes curing of the present composition.
  • a catalyst used for the hydrosilylation reaction can be used.
  • platinum black for example, platinum black, secondary platinum chloride, platinum chloride, reaction products of platinum chloride and monovalent alcohol, complexes of platinum chloride with olefins and vinyl siloxane, platinum-based catalysts such as platinum bisacetoacetate, palladium.
  • platinum group metal catalysts such as system catalysts and rhodium catalysts.
  • the blending amount of the C component may be any amount necessary for curing, and can be appropriately adjusted according to a desired curing rate and the like. It is preferable to add 0.01 to 1000 ppm as the metal atomic weight with respect to the total of the component A and the platinum group metal catalyst.
  • the D component of the present invention is preferably added in an amount of 100 to 4000 parts by mass with respect to 100 parts by mass of the addition-curable silicone polymer component (A component + B component).
  • the thermal conductivity of the heat-resistant heat-conductive composition and the heat-resistant heat-conductive sheet can be set to 0.8 W / m ⁇ K or more.
  • the heat conductive particles are preferably at least one selected from alumina, zinc oxide, magnesium oxide, aluminum nitride, boron nitride, aluminum hydroxide and silica. Various shapes such as spherical, scaly, and polyhedral can be used.
  • the specific surface area of the thermally conductive particles is preferably in the range of 0.06 to 15 m 2 / g.
  • the specific surface area is the BET specific surface area, and the measuring method follows JIS R1626. When the average particle size is used, the range of 0.1 to 100 ⁇ m is preferable.
  • the particle size is measured by the laser diffraction light scattering method, and the cumulative particle size distribution D50 (median size) based on the volume is measured.
  • this measuring instrument for example, there is a laser diffraction / scattering type particle distribution measuring device LA-950S2 manufactured by HORIBA, Ltd.
  • the heat conductive particles at least two or more inorganic particles having different average particle diameters may be used in combination. This is because, in this way, the thermally conductive inorganic particles having a small particle size are embedded between the large particle diameters, and the particles can be mixed in a state close to the closest packing, and the thermal conductivity becomes high.
  • Inorganic particles are indicated by Ra Si (OR') 3-a (R is an unsubstituted or substituted organic group having 1 to 20 carbon atoms, R'is an alkyl group having 1 to 4 carbon atoms, and a is 0 or 1). It is preferable to surface-treat with the above silane compound or a partial hydrolyzate thereof.
  • the above-mentioned alkoxysilane compound (hereinafter, simply referred to as “silane”) is, for example, methyltrimethoxylan, ethyltrimethoxylan, propyltrimethoxylan, butyltrimethoxylan, pentiltrimethoxylan, hexyltrimethoxylan, hexyltri.
  • the silane compound can be used alone or in admixture of two or more.
  • alkoxysilane and one-terminal silanolsiloxane may be used in combination.
  • the surface treatment referred to here includes not only covalent bonds but also adsorption.
  • a heat resistance improver such as red iron oxide, titanium oxide, or cerium oxide
  • a flame retardant aid such as a curing retarder
  • Organic or inorganic particle pigments may be added for the purpose of coloring and toning.
  • Alkoxy group-containing silicone may be added as a material to be added for the purpose of filler surface treatment or the like.
  • an organopolysiloxane having no addition curing reactive group may be added. It is desirable from the viewpoint of workability that the viscosity at 25 ° C. is 10 to 100,000 mPa ⁇ s, particularly 100 to 10,000 mPa ⁇ s.
  • composition of the liquid heat conductive composition may be the same as that of the heat conductive sheet, or may be the following composition.
  • Matrix component Linear organopolysiloxane containing an average of 2 or more in one molecule and an alkenyl group bonded to a silicon atom at both ends of the molecular chain
  • Cross-linking component An average of 2 or more in one molecule The amount of organohydrogenpolysiloxane containing a hydrogen atom bonded to the silicon atom of the above is less than 1 mol with respect to 1 mol of the silicon atom-bonded alkenyl group in the component A.
  • the components (a) to (c) are the matrix component, the cross-linking component, and the heat conductive particles described in the composition of the heat conductive sheet.
  • the liquid heat conductive composition may be held in an uncured state after being filled in the space, or by diffusion of the curing catalyst of the heat conductive sheet. It can also be cured. In the case of the same composition as the heat conductive sheet, it can be cured after filling. Further, the addition ratio of the cross-linking component may be reduced to partially cross-link. In this case, it becomes a paste.
  • dimethyl silicone oil having no reactive group may be used instead of (a) and (b). In this case, it is not crosslinked.
  • the viscosity of the liquid heat conductive material is preferably 50 to 5000 Pa ⁇ s. The viscosity is measured using a HAAKE rheometer MARSIII under the conditions of Gap: 0.5 mm, rotation speed 1 (1 / s), and temperature 25 ° C.
  • FIG. 1 is a schematic perspective view of a heat conductive sheet for a sealing material according to an embodiment of the present invention.
  • the heat conductive sheet 10 for a sealing material is formed in a frame-shaped sheet, and the inside of the frame is a space 11 for filling the liquid heat conductive composition. Further, the hardness of the sheet 10 is 5 or more and 55 or less on the shore 00.
  • the sheet 10 can be placed on the polyethylene terephthalate (PET) film 12 and packaged and transported.
  • PET polyethylene terephthalate
  • FIG. 2A is a schematic perspective view in which the heat conductive sheet 10 for a sealing material according to the embodiment of the present invention is attached to the bottom surface of the battery module 13, and FIG. 2B is a schematic view in which the battery module 13 is turned upside down and placed in the case 14.
  • FIG. 2C is a cross-sectional view taken along the line II of FIG. 2B, showing a state in which the space between the heat conductive sheet 10 for the sealing material, the battery module 13 and the case 14 is filled with the liquid heat conductive composition 15. Shown.
  • FIG. 2A is a schematic perspective view in which the heat conductive sheet 10 for a sealing material according to the embodiment of the present invention is attached to the bottom surface of the battery module 13, and FIG. 2B is a schematic view in which the battery module 13 is turned upside down and placed in the case 14.
  • FIG. 2C is a cross-sectional view taken along the line II of FIG. 2B, showing a state in which the space between the heat conductive sheet 10 for the sealing material, the battery module 13 and
  • the present invention is limited to the bottom surface of the battery module 13. Instead, the heat conductive sheet 10 for a sealing material may be attached to the side surface and the upper surface, and the frame-shaped space portion 11 may be filled with the liquid heat conductive composition.
  • FIGS. 3A and 3B are explanatory views showing a method of measuring the thermal conductivity of the heat conductive sheet according to the embodiment of the present invention.
  • the thermal conductivity of the heat conductive sheet was measured by a hot disk (ISO 22007-2 compliant).
  • the thermal conductivity measuring device 1 sandwiches the polyimide film sensor 2 between two samples 3a and 3b, applies a constant power to the sensor 2, generates a constant heat, and starts from the temperature rise value of the sensor 2.
  • the sensor 2 has a tip 4 having a diameter of 7 mm and has a double spiral structure of electrodes as shown in FIG. 3B, and an applied current electrode 5 and a resistance value electrode (temperature measurement electrode) 6 are arranged at the bottom. Has been done.
  • FIG. 4A-B is a photograph showing a pressure resistance test method when a liquid heat conductive composition is filled in a heat conductive sheet for a sealing material according to an embodiment of the present invention.
  • the heat conductive sheet 10 is placed on the aluminum plate 16.
  • an acrylic resin plate 17 having a thickness of 10 mm is placed on the heat conductive sheet 10 and fixed to the aluminum plate 16 with four bolts. The gap between the aluminum plate 16 and the acrylic resin plate 17 maintains a predetermined distance.
  • the acrylic resin plate 17 is provided with an injection port 18 and a pressure sensor 19.
  • the liquid heat conductive composition is filled by applying pressure from the injection port 18, and the pressure applied to the heat conductive sheet 10 is measured.
  • the liquid heat conductive composition can be put into a dispenser or the like and press-fitted from the injection port 18.
  • Example 1 Creation of frame-shaped sheet ⁇ Material> The following materials were prepared. (1) 50 g of solution A containing a catalyst component (component C) and a matrix component (component A) of a commercially available two-component addition-curable silicone polymer. (2) 40 g of liquid B containing a cross-linking component (component B1) and a matrix component (component A) of a commercially available two-component addition-curable silicone polymer.
  • the outer shape of this frame-shaped sheet was 40 mm in length, 70 mm in width, 5 mm in width, and 2 mm and 1 mm in thickness.
  • the cutting method the outer shape and the inner shape were cut with a cutting plotter, and the outer peripheral portion and the central portion were removed.
  • the material kneaded in (3) may be applied onto the PET foil with a dispenser or the like to form a frame shape.
  • Aluminum oxide and aluminum hydroxide that have already been surface-treated with a silane coupling agent may be used. In that case, the steps (1) and (2) are not necessary.
  • Examples 2 to 4 Comparative Examples 1 to 2 It was carried out in the same manner as in Example 1 except that it is shown in Table 1.
  • the frame-shaped sheet has a shore of 5 or more, lateral pressure is applied to the frame-shaped sheet when the liquid heat conductive material is press-fitted, and no liquid leaks. It was. If the shore 00 exceeds 55, the repulsive stress at the time of assembling the battery becomes high, and the load applied to the battery module may cause a failure.
  • the heat conductive sheet for the sealing material of the present invention and the heat-generating electric / electronic parts incorporating the heat-conducting sheet are any semiconductors such as power modules and heat-generating electric / electronic parts such as lithium battery modules. Can also be applied to.
  • an in-vehicle lithium battery module generates a lot of heat and is suitable for applying the present invention.

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PCT/JP2020/015092 2019-09-25 2020-04-01 シーリング材用熱伝導シート及びこれを組み込んだ発熱性電気・電子部品 Ceased WO2021059567A1 (ja)

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EP20859619.7A EP3836292A4 (en) 2019-09-25 2020-04-01 HEAT TRANSFER FILM FOR SEALING MATERIALS AND HEAT GENERATING ELECTRICAL / ELECTRONIC COMPONENTS THEREOF
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DE102022130233A1 (de) 2022-11-15 2024-05-16 Audi Aktiengesellschaft Batterieanordnung für ein Kraftfahrzeug und Verfahren zum Herstellen einer Batterieanordnung mit verbesserter mechanischer Stabilität
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