WO2023243225A1 - 結晶性グラファイト材と金属材の接合材およびその製造方法 - Google Patents

結晶性グラファイト材と金属材の接合材およびその製造方法 Download PDF

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WO2023243225A1
WO2023243225A1 PCT/JP2023/016049 JP2023016049W WO2023243225A1 WO 2023243225 A1 WO2023243225 A1 WO 2023243225A1 JP 2023016049 W JP2023016049 W JP 2023016049W WO 2023243225 A1 WO2023243225 A1 WO 2023243225A1
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crystalline graphite
metal
graphite material
metal material
crystalline
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English (en)
French (fr)
Japanese (ja)
Inventor
直巳 西木
涼 桑原
崇 鶴田
秀敏 北浦
茂樹 坂口
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Panasonic Intellectual Property Management Co Ltd
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Panasonic Intellectual Property Management Co Ltd
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • 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
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/20—Graphite
    • C01B32/21—After-treatment

Definitions

  • the present disclosure relates to a bonding material for a crystalline graphite material and a metal material that can be used for heat diffusion materials, heat spreaders, etc. that require high thermal conductivity, and a method for manufacturing the same.
  • crystalline graphite material Since crystalline graphite material has high thermal conductivity, it is expected to be used as a heat diffusion material, heat spreader, etc. However, crystalline graphite materials have a strength difference of 50 times or more between the plane direction and the thickness direction, making it difficult to process screw holes and the like. Furthermore, since the crystalline graphite material is a sublimation material, it cannot be melted and bonded in a normal environment. Therefore, for installation, it is required that the crystalline graphite material be bonded to a metal material with high thermal conductivity that does not impair heat conduction.
  • the crystalline graphite material has a crystal structure in which six-membered ring crystal network structures are stacked.
  • the plane of the six-membered ring crystal network is called the basal plane 11. Since there are free bonds at the edge 12 of the basal surface, metal atoms can bond thereto. On the other hand, there are only ⁇ electrons in the plane of the basal plane 11, making it difficult to bond metal atoms.
  • the graphite material traditionally used is made by solidifying fine graphite powder by sintering, etc., and has bonding elements that can bond with metal atoms in all directions, so it can be used with metals, including coatings such as plating. It is possible to join with materials.
  • Patent No. 6590322 Japanese Patent Application Publication No. 2018-104251
  • a bonding material includes a crystalline graphite material and a metal material, and the crystalline graphite material has a carbon purity of 99.9% or more and a thermal conductivity in the in-plane direction of 600 W/m ⁇ K. or more, and the degree of anisotropy due to at least one of electrical conduction and thermal conduction in the in-plane direction and thickness direction of the basal surface is 50 or more, and the metal material is made of iron, nickel, tungsten, copper, or aluminum.
  • the crystalline graphite material contains at least one selected metal, and in the thickness direction of the basal plane of the crystalline graphite material, crystallinity
  • the graphite material is joined to the metal material, and at the end of the basal surface, the crystalline graphite material is joined to the metal material via the metal carbide.
  • a method for manufacturing a bonding material between a crystalline graphite material and a metal material includes placing the crystalline graphite material and the metal material in a heating furnace with the metal material overlaid on the basal surface of the crystalline graphite material. installation step, a step of heating and pressurizing the crystalline graphite material and metal material with the atmosphere inside the heating furnace mixed with inert gas and air, and a step of cooling the heating furnace to room temperature and heating it.
  • the heating and pressurizing step which includes the step of taking out the bonding material between the crystalline graphite material and the metal material from the furnace, 0.1 vol% to 4 vol% of air is mixed with the inert gas and flowed.
  • FIG. 2 is a schematic diagram of a six-membered ring crystal network structure of a crystalline graphite material.
  • FIG. 2 is a schematic cross-sectional view showing a cross-sectional structure of a bonding material in which a crystalline graphite material and a metal material are bonded together according to Embodiment 1.
  • FIG. 2 is a diagram showing Table 1 that summarizes a list of conditions and results for Examples and Comparative Examples.
  • the crystalline graphite material has a coefficient of thermal expansion of approximately "0" in the in-plane direction of the basal plane 11, while a coefficient of thermal expansion in the direction perpendicular to the basal plane 11 is comparable to that of metal.
  • a crystalline graphite material In order to bond a crystalline graphite material to a metal plate, which is one of the metal materials, it is necessary to raise the temperature. However, since the metal plate expands thermally, cracks occur due to the difference in thermal expansion between the metal plate and the crystalline graphite material, making it difficult to join the metal plate and the crystalline graphite material.
  • the present inventors have discovered that a metal oxide and a metal carbide are provided between the basal plane of the crystalline graphite material and the metal material as a layer to alleviate the difference in thermal expansion between the crystalline graphite material and the metal material. , resulting in the bonding material of the present disclosure.
  • the structure of the bonding material described above can be obtained by heating and pressurizing a metal material layered on the basal surface of a crystalline graphite material while mixing a small amount of air into an inert gas. The inventors have discovered that this can be done, and have arrived at a method for manufacturing a bonding material between a crystalline graphite material and a metal material according to the present disclosure.
  • the present disclosure aims to solve the conventional problems and to provide a bonding material in which a basal surface of a crystalline graphite material and a metal material are bonded together.
  • the bonding material according to the first aspect includes a crystalline graphite material and a metal material, and the crystalline graphite material has a carbon purity of 99.9% or more and an in-plane thermal conductivity of 600 W/m ⁇ K or more. and the degree of anisotropy due to at least one of electrical conduction and thermal conduction in the in-plane direction and the thickness direction of the basal surface is 50 or more, and the metal material is selected from iron, nickel, tungsten, copper, and aluminum.
  • the crystalline graphite material is formed through a metal oxide containing at least one metal and a metal carbide containing at least one metal. is joined to the metal material, and at the end of the basal surface, the crystalline graphite material is joined to the metal material via the metal carbide.
  • the carbon content of the metal carbide in contact with the crystalline graphite material may be 0.001 atm% to 10 atm%.
  • the metal oxide interposed between the metal carbide and the crystalline graphite material has an oxygen content of 0.1 atm% to 5 atm%. There may be.
  • a method for manufacturing a bonding material between a crystalline graphite material and a metal material includes placing the crystalline graphite material and the metal material in a heating furnace with the metal material being stacked on the basal surface of the crystalline graphite material. a step of heating and pressurizing the crystalline graphite material and metal material with the atmosphere in the heating furnace mixed with inert gas and air; and a step of cooling the heating furnace to room temperature and heating and pressurizing it. In the heating and pressurizing step, 0.1 vol% to 4 vol% of air is mixed with the inert gas and flowed.
  • the bonding material between a crystalline graphite material and a metal material according to the present disclosure enables processes such as screw hole drilling and soldering on the metal part, and the high thermal conductivity of the crystalline graphite material can be used as a heat diffusion material or a heat spreader. It will be widely used as a heat countermeasure material.
  • FIG. 2 is a schematic cross-sectional view showing a cross-sectional structure of a bonding material obtained by bonding a crystalline graphite material 21 and a metal material 22 according to the first embodiment.
  • the bonding material according to the first embodiment includes a crystalline graphite material 21 and a metal material 22.
  • the crystalline graphite material 21 has a carbon purity of 99.9% or more, a thermal conductivity in the plane direction of 600 W/m ⁇ K or more, and at least electrical conduction and thermal conduction in the basal plane direction and the thickness direction. The degree of anisotropy on one side is 50 or more.
  • the metal material 22 includes at least one selected from iron, nickel, tungsten, copper, and aluminum. In the thickness direction of the basal surface 11 of the crystalline graphite material 21, the crystalline graphite material 21 is joined to the metal material 22 via the metal oxide layer 23 and the metal carbide layer 24. At the end portion 12 of the basal surface of the crystalline graphite material 21, the crystalline graphite material 21 is joined to the metal material 22 via the metal carbide layer 24.
  • ⁇ Crystalline graphite material> As the crystalline graphite material 21, for example, a graphite plate produced by using polyimide as a starting material and heating it at 2500° C. or higher may be used. Note that the material is not limited to this, and a graphite sheet, graphite plate, etc. having anisotropy may also be used. Anisotropy here means that when the conductivity (at least one of thermal conductivity and electrical conductivity) is compared in the in-plane direction and the thickness direction, the conductivity in the in-plane direction of the basal surface is higher than that in the thickness direction. The conductivity is more than 50 times that of . Further, it is desirable that the graphite plate has a thermal conductivity in the in-plane direction of 600 W/m ⁇ K or more, preferably 800 W/m ⁇ K or more.
  • the crystalline graphite material has a crystal structure in which six-membered ring crystal network structures are stacked.
  • FIG. 1 shows a six-membered ring crystal network structure having three layers, the structure is not limited to this.
  • the metal material may contain at least one selected from iron, nickel, tungsten, copper, and aluminum.
  • This bonding material between a crystalline graphite material and a metal material can be manufactured by the following steps.
  • the crystalline graphite material 21 and the metal plate 22 are placed in a heating furnace with, for example, a metal plate 22 stacked on the basal surface of the crystalline graphite material 21 as the metal material 22.
  • the thickness of the crystalline graphite material may be 0.1 mm or more and 10 mm or less, and preferably 0.5 mm or more and 5 mm or less.
  • the thickness of the metal plate 22 may be 0.1 mm or more and 10 mm or less, and preferably 0.5 mm or more and 5 mm or less.
  • both the crystalline graphite material and the metal plate can be joined even in larger sizes.
  • the size of the resulting bonding material is determined by the size of the heating furnace used during production.
  • the set maximum temperature varies depending on the metal material used, and after being maintained at the set maximum temperature for a certain period of time, the temperature is lowered to room temperature.
  • the pressure for controlling the thickness is preferably in the range of 1 MPa or more and 20 MPa or less per 1 cm square, preferably 5 MPa or more and 10 MPa or less.
  • the heat treatment is performed in an inert gas flow. Air is mixed with the inert gas until the maximum set temperature is maintained.
  • the amount of air mixed into the inert gas is preferably 0.1 vol% or more and 4 vol% or less, preferably 0.3 vol% or more and 2 vol% or less. This is to form a layer that alleviates the difference in thermal expansion between the crystalline graphite material and the metal material.
  • a metal oxide layer 23 and a metal carbide layer 24 are formed on the basal surface. On the other hand, only the metal carbide layer 24 may be formed at the end of the basal surface.
  • the metal carbide layer 24 contains carbon in the metal from 0.001 atm% to 10 atm%.
  • the metal oxide layer 23 contains oxygen atoms of 0.1 atm % or more and 5 atm % or less.
  • a bonding material containing a crystalline graphite material and a metal material was produced.
  • the crystalline graphite material was made by heat treating a polyimide film.
  • the crystalline graphite material has dimensions of 50 mm x 50 mm x 1 mm thickness.
  • a metal plate which is an example of a metal material, has dimensions of 60 mm x 60 mm x 2 mm thickness.
  • the temperature increase/decrease rate was 10° C./min, and the temperature was maintained at the set maximum temperature for 1 hour to stabilize the temperature.
  • Argon gas was used as the inert gas and was flowed at a flow rate of 1 L/min.
  • the evaluation was passed if both the crystalline graphite material and the metal material retained their shape, and when the pasted surface was peeled off, peeled pieces of the crystalline graphite material remained on the metal side with an area of 30% or more. .
  • Example 1 A basal surface of a crystalline graphite material was placed on an iron plate, which is a metal material, and heat treatment was performed at a set maximum temperature of 1500°C.
  • the maximum temperature setting is preferably 1400°C to 1600°C.
  • the crystalline graphite material was in close contact with the iron plate. When the crystalline graphite material was peeled off from the iron plate, peeled pieces of the crystalline graphite material remained on the metal material side.
  • Example 2 The basal surface of the crystalline graphite material was placed on a nickel plate, which is a metal material, and heat treatment was performed at a set maximum temperature of 1450°C. When using a nickel plate as the metal material, a suitable maximum temperature setting is 1400°C to 1550°C. The crystalline graphite material was in close contact with the nickel plate. When the crystalline graphite material was peeled off from the nickel plate, peeled pieces of the crystalline graphite material remained on the metal material side.
  • Example 3 A basal surface of a crystalline graphite material was placed on a tungsten plate, which is a metal material, and heat treatment was performed at a set maximum temperature of 1200°C. When using a tungsten plate as the metal material, a suitable maximum temperature setting is 1150°C to 1300°C. The crystalline graphite material was in close contact with the tungsten plate. When the crystalline graphite material was peeled off from the tungsten plate, peeled pieces of the crystalline graphite material remained on the metal material side.
  • Example 4 A basal surface of a crystalline graphite material was placed on a copper plate, which is a metal material, and heat treatment was performed at a set maximum temperature of 1100°C. When using a copper plate as the metal material, a suitable maximum temperature setting is 1050°C to 1150°C. The crystalline graphite material was in close contact with the copper plate. When the crystalline graphite material was peeled off from the copper plate, peeled pieces of the crystalline graphite material remained on the metal material side.
  • Example 5 A basal surface of a crystalline graphite material was placed on an aluminum plate, which is a metal material, and heat treatment was performed at a set maximum temperature of 660°C. When using an aluminum plate as the metal material, a suitable maximum temperature setting is 620°C to 700°C. The crystalline graphite material was in close contact with the aluminum plate. When the crystalline graphite material was peeled off from the aluminum plate, peeled pieces of the crystalline graphite material remained on the metal material side.
  • the bonding material between a crystalline graphite material and a metal material according to the present disclosure can be used for heat diffusion materials, heat spreaders, etc. that require high thermal conductivity.

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PCT/JP2023/016049 2022-06-14 2023-04-24 結晶性グラファイト材と金属材の接合材およびその製造方法 Ceased WO2023243225A1 (ja)

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013157590A (ja) * 2012-01-04 2013-08-15 Jnc Corp 放熱部材、電子デバイスおよびバッテリー
JP2016022730A (ja) * 2014-07-24 2016-02-08 株式会社カネカ グラファイトとグラファイトの接合体、グラファイトと金属の接合体、グラファイト接着用積層体、およびそれらの製造方法
JP2017028247A (ja) * 2015-07-16 2017-02-02 パナソニックＩｐマネジメント株式会社 グラファイトとシリコンとの結合体及びその製造方法
CN206516626U (zh) * 2016-09-28 2017-09-22 厦门恒坤新材料科技股份有限公司 一种由石墨片与金属层复合的导热片
JP2020181926A (ja) * 2019-04-26 2020-11-05 島根県 高結晶性黒鉛の接合構造及び接合方法

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013157590A (ja) * 2012-01-04 2013-08-15 Jnc Corp 放熱部材、電子デバイスおよびバッテリー
JP2016022730A (ja) * 2014-07-24 2016-02-08 株式会社カネカ グラファイトとグラファイトの接合体、グラファイトと金属の接合体、グラファイト接着用積層体、およびそれらの製造方法
JP2017028247A (ja) * 2015-07-16 2017-02-02 パナソニックＩｐマネジメント株式会社 グラファイトとシリコンとの結合体及びその製造方法
CN206516626U (zh) * 2016-09-28 2017-09-22 厦门恒坤新材料科技股份有限公司 一种由石墨片与金属层复合的导热片
JP2020181926A (ja) * 2019-04-26 2020-11-05 島根県 高結晶性黒鉛の接合構造及び接合方法

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