WO2017022012A1 - アルミニウム‐炭化珪素質複合体及びその製造方法 - Google Patents
アルミニウム‐炭化珪素質複合体及びその製造方法 Download PDFInfo
- Publication number
- WO2017022012A1 WO2017022012A1 PCT/JP2015/071802 JP2015071802W WO2017022012A1 WO 2017022012 A1 WO2017022012 A1 WO 2017022012A1 JP 2015071802 W JP2015071802 W JP 2015071802W WO 2017022012 A1 WO2017022012 A1 WO 2017022012A1
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- Prior art keywords
- silicon carbide
- mass
- less
- particle size
- aluminum
- Prior art date
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- 229910010271 silicon carbide Inorganic materials 0.000 title claims abstract description 91
- 239000002131 composite material Substances 0.000 title claims abstract description 73
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 9
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims abstract description 117
- 239000002245 particle Substances 0.000 claims abstract description 104
- 229910000838 Al alloy Inorganic materials 0.000 claims abstract description 36
- CSDREXVUYHZDNP-UHFFFAOYSA-N alumanylidynesilicon Chemical compound [Al].[Si] CSDREXVUYHZDNP-UHFFFAOYSA-N 0.000 claims description 32
- 238000000034 method Methods 0.000 claims description 31
- 229910052710 silicon Inorganic materials 0.000 claims description 14
- 239000010703 silicon Substances 0.000 claims description 14
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 13
- 229910052749 magnesium Inorganic materials 0.000 claims description 13
- 239000011777 magnesium Substances 0.000 claims description 13
- 239000000843 powder Substances 0.000 claims description 12
- 238000010304 firing Methods 0.000 claims description 10
- 238000000465 moulding Methods 0.000 claims description 6
- 229910021426 porous silicon Inorganic materials 0.000 claims description 3
- 239000002994 raw material Substances 0.000 claims description 3
- 238000009826 distribution Methods 0.000 claims description 2
- 230000005484 gravity Effects 0.000 abstract description 7
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 21
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 13
- 239000011230 binding agent Substances 0.000 description 11
- 239000008119 colloidal silica Substances 0.000 description 11
- 239000000463 material Substances 0.000 description 10
- 238000002156 mixing Methods 0.000 description 10
- 239000002002 slurry Substances 0.000 description 10
- 239000007787 solid Substances 0.000 description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 8
- 239000000126 substance Substances 0.000 description 7
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 6
- 238000005470 impregnation Methods 0.000 description 6
- 239000001301 oxygen Substances 0.000 description 6
- 229910052760 oxygen Inorganic materials 0.000 description 6
- 238000011049 filling Methods 0.000 description 5
- 238000005242 forging Methods 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- 229910052802 copper Inorganic materials 0.000 description 3
- 239000010949 copper Substances 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 229910052751 metal Inorganic materials 0.000 description 3
- 239000002184 metal Substances 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 238000004512 die casting Methods 0.000 description 2
- 239000000155 melt Substances 0.000 description 2
- 238000002844 melting Methods 0.000 description 2
- 230000008018 melting Effects 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 239000011505 plaster Substances 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 238000011282 treatment Methods 0.000 description 2
- 229910000831 Steel Inorganic materials 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 238000003763 carbonization Methods 0.000 description 1
- 238000005266 casting Methods 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 230000001419 dependent effect Effects 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 239000001307 helium Substances 0.000 description 1
- 229910052734 helium Inorganic materials 0.000 description 1
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 125000004435 hydrogen atom Chemical class [H]* 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 229920000609 methyl cellulose Polymers 0.000 description 1
- 239000001923 methylcellulose Substances 0.000 description 1
- 235000010981 methylcellulose Nutrition 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000009740 moulding (composite fabrication) Methods 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- 238000004663 powder metallurgy Methods 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 229910000679 solder Inorganic materials 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
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- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
- C04B2235/74—Physical characteristics
- C04B2235/78—Grain sizes and shapes, product microstructures, e.g. acicular grains, equiaxed grains, platelet-structures
- C04B2235/782—Grain size distributions
- C04B2235/783—Bimodal, multi-modal or multi-fractional
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
- C04B2235/74—Physical characteristics
- C04B2235/78—Grain sizes and shapes, product microstructures, e.g. acicular grains, equiaxed grains, platelet-structures
- C04B2235/786—Micrometer sized grains, i.e. from 1 to 100 micron
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
- C04B2235/96—Properties of ceramic products, e.g. mechanical properties such as strength, toughness, wear resistance
- C04B2235/9607—Thermal properties, e.g. thermal expansion coefficient
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C1/00—Making non-ferrous alloys
- C22C1/10—Alloys containing non-metals
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C1/00—Making non-ferrous alloys
- C22C1/10—Alloys containing non-metals
- C22C1/1005—Pretreatment of the non-metallic additives
- C22C1/1015—Pretreatment of the non-metallic additives by preparing or treating a non-metallic additive preform
- C22C1/1021—Pretreatment of the non-metallic additives by preparing or treating a non-metallic additive preform the preform being ceramic
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C1/00—Making non-ferrous alloys
- C22C1/10—Alloys containing non-metals
- C22C1/1036—Alloys containing non-metals starting from a melt
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- 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
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12007—Component of composite having metal continuous phase interengaged with nonmetal continuous phase
Definitions
- the present invention relates to an aluminum-silicon carbide composite and a method for producing the same.
- the silicon carbide composite can suppress its thermal expansion coefficient to 10 ppm / K or less by increasing the content of silicon carbide in the composite, and can exhibit high thermal conductivity.
- it due to its low specific gravity and the like, it has recently attracted attention as a heat sink material (Patent Documents 1, 2, and 3).
- the thermal conductivity of the conventional silicon carbide composites is at most about 200 W / mK at room temperature, which is less than that of copper (400 W / mK), and has a higher thermal conductivity. A complex was desired.
- the thermal conductivity of the silicon carbide based composite has a particle size of silicon carbide particles constituting the composite and the silicon carbide It is highly dependent on the content, and the composite having a specific range of particle size and silicon carbide content exhibits a high thermal conductivity of 230 W / mK or more, and a silicon carbide powder having a larger particle size is used. Then, the silicon carbide content in the composite cannot be increased, and a high thermal conductivity of 230 W / mK or more cannot be achieved.
- JP 2000-154080 A Japanese Patent Laid-Open No. 2000-141022 JP 2000-169267 A
- the present invention has been made in view of the above circumstances, and has been made for the purpose of obtaining an aluminum-silicon carbide composite having high thermal conductivity, low thermal expansion, and low specific gravity.
- the aluminum-silicon carbide composite according to the present invention is an aluminum-silicon carbide composite obtained by impregnating a porous silicon carbide molded body with an aluminum alloy, and the proportion of silicon carbide in the composite is 60 volumes.
- the aluminum-silicon carbide based composite has a thermal conductivity at 25 ° C. of 230 W / mK or more.
- the aluminum-silicon carbide composite is characterized by having a thermal expansion coefficient at 25 ° C. to 150 ° C. of 7.0 ppm / K or less.
- the aluminum alloy in the aluminum-silicon carbide based composite, contains 10% by mass to 14% by mass of silicon and 0.5% by mass to 2.5% by mass of magnesium. It is characterized by comprising.
- the above-mentioned aluminum-silicon carbide composite is obtained by adding an inorganic binder to a raw material powder containing three or more types of silicon carbide powders having different particle size distributions, and forming and firing steps. It is characterized by going through.
- the aluminum-silicon carbide composite according to the present invention or the aluminum-silicon carbide composite provided by the production method according to the present invention has high thermal conductivity, low thermal expansion, and low specific gravity.
- the aluminum-silicon carbide composite according to the present embodiment is an aluminum-silicon carbide composite obtained by impregnating a porous silicon carbide molded body with an aluminum alloy, and the proportion of silicon carbide in the composite is 60. 60% by mass or more and 75% by mass or less of silicon carbide having a particle size of 80 ⁇ m or more and 800 ⁇ m or less, and 20% by mass or more and 30% by mass of silicon carbide having a particle size of 8 ⁇ m or more and less than 80 ⁇ m. It is characterized by containing 5% by mass or more and 10% by mass or less of silicon carbide having a particle size of less than 8 ⁇ m.
- the particle size of silicon carbide means a particle size calculated by an electrical resistance test method.
- the amount of particles having a particle diameter of 80 ⁇ m or more and 800 ⁇ m or less with respect to all silicon carbide particles is set to 60 W% or more and less than 75 wt%, whereby 230 W / mK or more.
- Thermal conductivity can be expressed.
- the particle size is 80 ⁇ m or more, it becomes easy to obtain a target thermal conductivity of 230 W / mK or more. Further, if it is less than 55% by mass, the object of the present invention cannot be achieved even if the silicon carbide content itself in the composite can be increased.
- the amount of particles having a particle size of 8 ⁇ m or more and less than 80 ⁇ m with respect to all silicon carbide particles is reduced to 20% by mass or more and less than 30% by mass, thereby reducing the thermal conductivity. Can be obtained.
- the amount of particles having a particle size of less than 8 ⁇ m with respect to all silicon carbide particles is set to 5 ppm by mass to less than 10 mass%, thereby achieving the intended 7.0 ppm. It becomes easy to obtain a coefficient of thermal expansion of / K or less.
- the particle size of silicon carbide particles and the content of silicon carbide constituting the composite are important factors that largely control the thermal conductivity.
- the silicon carbide based composite obtained simply by using silicon carbide powder having a large particle size has a large particle size of the silicon carbide particles themselves, there is little mixing of oxygen from the raw material, and the composite Although it has a relatively high thermal conductivity because it is difficult to mix oxygen under the influence of oxidation or the like during the manufacturing process of the above, it is difficult to develop a high thermal conductivity of 230 W / mK or more, because the particle size is large Therefore, it is difficult to improve the silicon carbide content in the composite, and further, the silicon carbide powder with a small particle size added to improve the silicon carbide content is limited to a specific range. Otherwise, it is based on the knowledge that high thermal conductivity of 230 W / mK or more at room temperature cannot be expressed.
- examples of the aluminum alloy include a silicon-containing aluminum alloy, an aluminum alloy containing silicon and magnesium, and a magnesium-containing aluminum alloy that are usually used when producing a silicon carbide composite.
- an aluminum alloy containing silicon and magnesium is preferable because the melting point of the molten metal is low and workability is good, and a magnesium-containing aluminum alloy is preferably selected from the viewpoint of improving the thermal conductivity of the resulting composite. .
- the silicon content is preferably 18% by mass or less. More preferably, the silicon content is 10% by mass to 14% by mass.
- the magnesium content 0.5% by mass or more is considered in view of the fact that workability is good because the melting point of the alloy is lowered, and that the thermal conductivity of the resulting composite is lowered. It is preferable that it is 5 mass% or less. Furthermore, at 0.5 to 1.6% by mass, the thermal conductivity at 25 ° C. is 230 W / mK or more, and at 1.6 to 2.5% by mass, the thermal conductivity at 25 ° C. The rate is more preferable because it is 240 W / mK or more.
- the use of the aluminum-silicon carbide composite according to the present embodiment is not limited, but the carbonization in the composite is particularly required in applications requiring further low thermal expansion, such as a heat sink for a semiconductor module.
- a high silicon content is desirable.
- the silicon carbide content in the composite is preferably 60% by volume or more.
- particles having a particle size of 80 ⁇ m or more and 800 ⁇ m or less in all silicon carbide particles are 60% by mass or more and 75% by mass or less, and 8 ⁇ m or more and less than 80 ⁇ m.
- silicon carbide powder configured such that particles having a particle size are 20% by mass or more and 30% by mass or less and particles having a particle size of less than 8 ⁇ m are 5% by mass or more and 10% by mass or less.
- a porous molded body having a filling degree (or relative density) of 60% by volume or more is obtained, and an aluminum alloy is impregnated into the porous molded body by applying a conventionally known impregnation method.
- the conventionally known impregnation methods include a method in which a predetermined amount of silicon carbide powder is stirred into a molten aluminum alloy, a powder metallurgy method in which silicon carbide powder and aluminum alloy powder are mixed and fired, and a pre-made silicon carbide powder.
- a melt forging method, a die casting method, and the like in which a reform is produced and a molten aluminum alloy is impregnated therein.
- a method in which the silicon carbide content in the composite can be increased and a dense composite is easily obtained, and therefore, a method in which a preform is prepared and impregnated with molten aluminum is a preferable method.
- a more preferred impregnation method is a melt forging method.
- This method is a method in which a preform is placed in a mold, an aluminum alloy is charged, and then pressurized with mechanical pressure. The work is easy and, for example, when the pre-heat treatment of the preform is performed in air, This is because the aluminum alloy can be impregnated under a temperature condition in which the remaining heat does not cause significant oxidation of the preform.
- the molten aluminum alloy temperature when impregnating the aluminum alloy is 700 ° C. to 850 ° C., and the pressure during the impregnation is 30 MPa or more.
- known molding methods such as a press molding method, a casting molding method, and an extrusion molding method can be adopted as the molding method, and conventionally known treatments such as drying and firing can be applied.
- an organic binder such as methyl cellulose or PVA, an inorganic binder such as colloidal silica or alumina sol, and water or an organic solvent as a solvent.
- the preform immediately before impregnation is 60% by mass to 75% by mass of particles having a particle size of 80 ⁇ m or more and 800 ⁇ m or less in all silicon carbide particles, and 8 ⁇ m or more and less than 80 ⁇ m.
- Particles having a particle size of 20 mass% to 30 mass%, particles having a particle diameter of less than 8 ⁇ m are composed of 5 mass% to 10 mass%, and the filling degree of silicon carbide is 60 volume% or more. It is sufficient if the configuration is maintained.
- the preform is added with an inorganic binder such as colloidal silica or alumina sol for the purpose of developing its strength, but these binders act in the direction of lowering the thermal conductivity. Therefore, the amount of addition should be appropriately adjusted in accordance with the particle size of the silicon carbide powder used at the time of forming the preform and the silicon carbide filling degree of the preform obtained therefrom.
- colloidal silica is preferable because it becomes silica when bonded to form silicon carbide particles and develops a sufficient preform strength.
- the oxygen increase derived from the inorganic binder can be increased. Will occur, so the amount of addition should be limited.
- the amount of inorganic binder added is preferably 10% by mass or less based on the total silicon carbide particles in the case of silica sol having a solid content concentration of 20% by mass, for example.
- the thermal conductivity at 25 ° C. is 230 W / mK or more
- the thermal conductivity at 25 ° C. is 245 W / mK or more.
- the preform is generally fired for the purpose of developing the strength by the inorganic binder described above. At this time, firing is usually performed in an oxygen-containing atmosphere such as air. However, the silicon carbide powder constituting the preform is slightly oxidized by this firing, which causes a decrease in thermal conductivity in the composite. There is. Therefore, when firing the preform, conditions that are less susceptible to oxidation should be adopted as much as possible according to the particle size of the silicon carbide powder used. For example, firing in air is preferably performed at a temperature lower than 950 ° C., depending on the holding time, to suppress oxidation as much as possible. A preferable temperature range is 750 ° C. to 900 ° C. Examples of the firing method in a non-oxidizing atmosphere include a method of firing in a non-oxidizing gas such as argon, helium, hydrogen, nitrogen, or in vacuum.
- a non-oxidizing gas such as argon, helium, hydrogen, nitrogen, or in vacuum.
- a method of impregnating the preform with the aluminum alloy known methods such as a molten metal forging method, a die casting method, and a modified method thereof can be used.
- a preform pre-heat treatment is generally performed as a preliminary process so that the aluminum alloy can easily permeate.
- the silicon carbide particles constituting the preform are oxidized and the amount of oxygen does not exceed 1.4% by mass, and the amount of oxygen is further suppressed to 1.1% by mass or less. Is preferred.
- the aluminum-silicon carbide composite according to the above embodiment has a high thermal conductivity of 230 W / mK or more, it is suitable as a heat sink material for a power module. Further, since the thermal expansion coefficient at 25 ° C. to 150 ° C. is 7.0 ppm / K or less, it can be used as a heat sink for semiconductor modules.
- the aluminum-silicon carbide composite according to the above embodiment has a low specific gravity of about 3 and is also useful as a mounting material for mobile devices such as automobiles and trains.
- Example 1 65% by mass of silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less, 25% by mass of silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m, 10% by mass of silicon carbide powder having a particle size of less than 8 ⁇ m, and colloidal silica (Nissan 8.9% by mass of Snowtex O manufactured by Chemical Industry Co., Ltd., containing 20% by mass of solids) and 12% by mass of water were weighed and mixed to prepare a slurry. The slurry was poured into a plaster mold and allowed to stand, then demolded and dried to obtain a molded body. This molded body was calcined in air at 1000 ° C. for 4 hours to form a preform.
- NG-F80 manufactured by Taiyo Random Co., Ltd.
- GC- # 500 Yakushima made by Nanko Ceramics Co., Ltd., so that the silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m is 25% by mass and the silicon carbide powder having a particle size of less than 8 ⁇ m is 10% by mass.
- Electric powder GC-1000F and Nanko Ceramics Co., Ltd. GC- # 4000 mixed at a mixing ratio of 13.5: 16.5: 5.0 were used.
- a part of the preform was processed to a diameter of 50 mm and a thickness of 5 mm in order to measure the density.
- the filling degree of the silicon carbide in the preform was 69.6%.
- the silicon carbide filling degree of the preform was defined as a percentage by dividing the density of the processed product by the theoretical density of silicon carbide of 3.21 g / cm 3 .
- the remaining preform was preheated by firing at 650 ° C. for 1 hour in air.
- the front surface of the preform is sufficiently hidden so that the aluminum alloy containing 12% by mass of silicon and 1% by mass of magnesium and melted at 850 ° C. It was put in the mold. Thereafter, it was quickly pressed by a punch at a pressure of 56 MPa for 14 minutes, and after cooling, an aluminum alloy lump containing a silicon carbide based composite was taken out from the mold. Further, a silicon carbide composite was cut out from this lump.
- the thermal conductivity of the composite at room temperature In order to measure the thermal conductivity of the composite at room temperature, a part thereof was processed into a length of 25 mm, a width of 25 mm, and a thickness of 1 mm to prepare a sample. As a result of measuring the thermal conductivity of this sample by the laser flash method, the thermal conductivity was 252 W / mK. About the sample for thermal expansion coefficient measurement, the sample of the predetermined shape was cut out from the said composite, and the thermal expansion coefficient from room temperature (25 degreeC) to 150 degreeC was measured. The results are shown in Table 1.
- Example 2 65% by mass of silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less, 26% by mass of silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m, 9% by mass of silicon carbide powder having a particle size of less than 8 ⁇ m, and colloidal silica (Nissan 11.6% by mass of Snowtex O, manufactured by Kagaku Kogyo Co., Ltd., containing 20% by mass of solids) and 9% by mass of water were weighed and mixed to prepare a slurry.
- colloidal silica Nisan 11.6% by mass of Snowtex O, manufactured by Kagaku Kogyo Co., Ltd., containing 20% by mass of solids
- NG-F80 manufactured by Taiyo Random Co., Ltd. was used.
- Nanko Ceramics Co., Ltd. GC- # 500 Yakushima so that the silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m is 26% by mass and the silicon carbide powder having a particle size of less than 8 ⁇ m is 9% by mass.
- a powder prepared by mixing GC-1000F and GMF-4S manufactured by Denko Co., Ltd. at a blending ratio of 13.5: 16.5: 5.0 was used. Preforms and composites were produced in the same manner as in Example 1. The results are shown in Table 1.
- Example 3 65% by mass of silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less, 25% by mass of silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m, 10% by mass of silicon carbide powder having a particle size of less than 8 ⁇ m, and colloidal silica (Nissan 12.0% by mass of Snowtex O manufactured by Chemical Industry Co., Ltd., containing 20% by mass of solids) and 9% by mass of water were weighed and mixed to prepare a slurry.
- colloidal silica Nisan 12.0% by mass of Snowtex O manufactured by Chemical Industry Co., Ltd., containing 20% by mass of solids
- NG-F80 manufactured by Taiyo Random Co., Ltd.
- GC- # 500 Yakushima made by Nanko Ceramics Co., Ltd., so that the silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m is 25% by mass and the silicon carbide powder having a particle size of less than 8 ⁇ m is 10% by mass.
- Electric powder GC-1000F and Nanko Ceramics Co., Ltd. GC- # 4000 mixed at a mixing ratio of 13.5: 16.5: 5.0 were used.
- a preform was produced in the same manner as in Example 1.
- Example 4 A preform and a composite were produced in the same manner as in Example 3 except that the aluminum alloy was an aluminum alloy containing 12% by mass of silicon and 1.2% by mass of magnesium. The results are shown in Table 1.
- Example 5 A preform and a composite were produced in the same manner as in Example 3 except that the aluminum alloy was an aluminum alloy containing 12% by mass of silicon and 1.6% by mass of magnesium. The results are shown in Table 1.
- Example 6 As a silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less, NG-F80 manufactured by Taiyo Random Co., Ltd. was used. In addition, GC- # 500, Yakushima made by Nanko Ceramics Co., Ltd., so that the silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m is 25% by mass and the silicon carbide powder having a particle size of less than 8 ⁇ m is 10% by mass. Electric powder GC-1000F and Nanko Ceramics Co., Ltd. GC- # 6000 were mixed at a mixing ratio of 13.5: 16.5: 5.0.
- Preforms and composites were produced in the same manner as in Example 3 except that 6% by mass of colloidal silica (Snowtex O manufactured by Nissan Chemical Industries, Ltd., containing 20% by mass of solids) was weighed and the slurry was adjusted. The results are shown in Table 1.
- Example 7 60% by mass of silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less, 30% by mass of silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m, 10% by mass of silicon carbide powder having a particle size of less than 8 ⁇ m, and colloidal silica (Nissan 12% by mass of Snowtex O, manufactured by Chemical Industry Co., Ltd., containing 20% by mass of solids) and 9% by mass of water were weighed and mixed to prepare a slurry.
- colloidal silica Nisan 12% by mass of Snowtex O, manufactured by Chemical Industry Co., Ltd., containing 20% by mass of solids
- the silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less is 60% by mass
- the silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m is 30% by mass
- the silicon carbide powder having a particle size of less than 8 ⁇ m is 10% by mass.
- NG-F54 manufactured by Taiyo Random Co., Ltd., GC- # 500 manufactured by Taiyo Random Co., Ltd., and GC- # 3000 manufactured by Taiyo Random Co., Ltd. were mixed at a blending ratio of 60:30:10. .
- Preforms and composites were produced in the same manner as in Example 1. The results are shown in Table 1.
- Example 8 75% by mass of silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less, 25% by mass of silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m, 5% by mass of silicon carbide powder having a particle size of less than 8 ⁇ m, and colloidal silica (Nissan 12% by mass of Snowtex O, manufactured by Chemical Industry Co., Ltd., containing 20% by mass of solids) and 9% by mass of water were weighed and mixed to prepare a slurry.
- colloidal silica Nisan 12% by mass of Snowtex O, manufactured by Chemical Industry Co., Ltd., containing 20% by mass of solids
- the silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less is 75% by mass
- the silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m is 20% by mass
- the silicon carbide powder having a particle size of less than 8 ⁇ m is 5% by mass.
- a powder prepared by mixing NG-F30 manufactured by Taihei Random Co., Ltd., NG-F220 manufactured by Taihei Random Co., Ltd., and GC- # 2000 manufactured by Taihei Random Co., Ltd. at a blending ratio of 60:30:10 was used.
- Preforms and composites were produced in the same manner as in Example 1. The results are shown in Table 1.
- Example 9 70% by mass of silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less, 20% by mass of silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m, 10% by mass of silicon carbide powder having a particle size of less than 8 ⁇ m, and colloidal silica (Nissan 12% by mass of Snowtex O, manufactured by Chemical Industry Co., Ltd., containing 20% by mass of solids) and 9% by mass of water were weighed and mixed to prepare a slurry.
- colloidal silica Nisan 12% by mass of Snowtex O, manufactured by Chemical Industry Co., Ltd., containing 20% by mass of solids
- NG-F80 As a silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less, NG-F80 manufactured by Taiyo Random Co., Ltd. was used. In addition, GC- # 800 manufactured by Taiyo Random Co., Ltd. is used so that the silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m is 20% by mass and the silicon carbide powder having a particle size of less than 8 ⁇ m is 10% by mass. GC- # 6000 manufactured by Yo Random Co., Ltd. was mixed at a blending ratio of 20:10. A preform was produced in the same manner as in Example 1. The aluminum alloy is 12% by mass of silicon and 1.6% by mass of magnesium.
- Example 10 A preform and a composite were produced in the same manner as in Example 9, except that the aluminum alloy was an aluminum alloy containing 12% by mass of silicon and 2.1% by mass of magnesium.
- Silicon carbide powder having a particle size of 80 ⁇ m or more and 800 ⁇ m or less is 55% by mass
- silicon carbide powder having a particle size of 8 ⁇ m or more and less than 80 ⁇ m is 40% by mass
- silicon carbide powder having a particle size of less than 8 ⁇ m is 5% by mass.
- the powder which mixed NG-F150 by Taiheiyo Random Co., Ltd. and GC-1000F by Yakushima Electric Works Co., Ltd. with a mixture ratio of 2: 1 was used.
- the aluminum-silicon carbide composites of Examples 1 to 10 according to the present invention have high thermal conductivity and a low thermal expansion coefficient. It can also be seen that these aluminum-silicon carbide composites have a low specific gravity.
- the aluminum-silicon carbide composite according to the present invention has a high thermal conductivity and is therefore suitable as a heat sink material for a power module and has a low coefficient of thermal expansion.
- -It can be used as a heat sink for steel. Further, because of its low specific gravity, it is also useful as a mounting material for mobile devices such as automobiles and trains.
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Abstract
Description
しかし、従来の炭化珪素質複合体の熱伝導率は、いずれも室温下でたかだか200W/mK程度であり、銅のそれ(400W/mK)には及ばず、さらなる高熱伝導率を有する炭化珪素質複合体が望まれていた。
本実施形態に係るアルミニウム‐炭化珪素質複合体では、全炭化珪素粒子に対する80μm以上800μm以下の粒径を有する粒子の量を60質量%以上75質量%未満とすることにより、230W/mK以上の熱伝導率を発現させることができる。
前記の粒径が80μm以上であることにより、目的とする230W/mK以上の熱伝導率を得ることが容易となる。また、55質量%未満であると、たとえ複合体中の炭化珪素含有量自体を大きくできても、本発明の目的を達成できない。
本実施形態において、アルミニウム合金としては、炭化珪素質複合体を作製する際に通常使用されている珪素含有アルミニウム合金、珪素とマグネシウムを含有するアルミニウム合金並びにマグネシウム含有アルミニウム合金が挙げられる。この中で、溶融金属の融点が低く作業性のよいことから珪素とマグネシウムを含有するアルミニウム合金が好ましく、また得られる複合体の熱伝導率向上の面からはマグネシウム含有アルミニウム合金が好ましく選択される。
さらに、0.5質量%以上1.6質量%以下では、25℃での熱伝導率が230W/mK以上であり、1.6質量%以上2.5質量%以下では25℃での熱伝導率が240W/mK以上であるためより好ましい。
本実施形態に係るアルミニウム‐炭化珪素質複合体を作製するには、全炭化珪素粒子中の80μm以上800μm以下の粒径を有する粒子が60質量%以上75質量%以下で、8μm以上80μm未満の粒径を有する粒子が20質量%以上30質量%以下で、8μm未満の粒径を有する粒子が5質量%以上10質量%以下となるように構成された炭化珪素粉末を用いて、炭化珪素の充填度(或いは相対密度)が60体積%以上の多孔質成形体を得て、該多孔質成形体にアルミニウム合金を、従来公知の含浸方法を適用して、含浸すればよい。
このような種々の処理を施しても、含浸直前におけるプリフォ-ムが、全炭化珪素粒子中の80μm以上800μm以下の粒径を有する粒子が60質量%以上75質量%以下で、8μm以上80μm未満の粒径を有する粒子が20質量%以上30質量%以下で、8μm未満の粒径を有する粒子が5質量%以上10質量%以下から構成され、炭化珪素の充填度が60体積%以上である構成が保たれていれば良い。
80μm以上800μm以下の粒径を有する炭化珪素粉末65質量%、8μm以上80μm未満の粒径を有する炭化珪素粉末25質量%、8μm未満の粒径を有する炭化珪素粉末10質量%及びコロイダルシリカ(日産化学工業株式会社製スノーテックスO、固形物を20質量%含有)を8.9質量%、水を12質量%秤量し、これらを混合してスラリ-を調整した。このスラリ-を石膏型に流し込み放置した後、脱型・乾燥し成形体を得た。この成形体を空気中、1000℃で4時間焼成しプリフォ-ムとした。
また、8μm以上80μm未満の粒径を有する炭化珪素粉末が25質量%、8μm未満の粒径を有する炭化珪素粉末が10質量%となるように、南興セラミックス株式会社製GC‐#500、屋久島電工株式会社製GC‐1000F及び南興セラミックス株式会社製GC‐#4000を13.5:16.5:5.0の配合率で混合した粉末を用いた。
80μm以上800μm以下の粒径を有する炭化珪素粉末65質量%、8μm以上80μm未満の粒径を有する炭化珪素粉末26質量%、8μm未満の粒径を有する炭化珪素粉末9質量%及びコロイダルシリカ(日産化学工業株式会社製スノーテックスO、固形物を20質量%含有)を11.6質量%、水を9質量%秤量し、これらを混合してスラリ-を調整した。
また、8μm以上80μm未満の粒径を有する炭化珪素粉末が26質量%、8μm未満の粒径を有する炭化珪素粉末が9質量%となるように、南興セラミックス株式会社製GC‐#500、屋久島電工株式会社製GC‐1000F及びGMF‐4Sを13.5:16.5:5.0の配合率で混合した粉末を用いた。
実施例1と同じ方法でプリフォーム及び複合体を作製した。結果を表1に示す。
80μm以上800μm以下の粒径を有する炭化珪素粉末65質量%、8μm以上80μm未満の粒径を有する炭化珪素粉末25質量%、8μm未満の粒径を有する炭化珪素粉末10質量%及びコロイダルシリカ(日産化学工業株式会社製スノーテックスO、固形物を20質量%含有)を12.0質量%、水を9質量%秤量し、これらを混合してスラリ-を調整した。
また、8μm以上80μm未満の粒径を有する炭化珪素粉末が25質量%、8μm未満の粒径を有する炭化珪素粉末が10質量%となるように、南興セラミックス株式会社製GC‐#500、屋久島電工株式会社製GC‐1000F及び南興セラミックス株式会社製GC‐#4000を13.5:16.5:5.0の配合率で混合した粉末を用いた。実施例1と同じ方法でプリフォームを作製した。
アルミニウム合金を珪素12質量%、マグネシム1.2質量%を含有するアルミニウム合金とした以外は、実施例3と同じ方法でプリフォーム及び複合体を作製した。結果を表1に示す。
アルミニウム合金を珪素12質量%、マグネシム1.6質量%を含有するアルミニウム合金とした以外は、実施例3と同じ方法でプリフォーム及び複合体を作製した。結果を表1に示す。
80μm以上800μm以下の粒径を有する炭化珪素粉末として、大平洋ランダム株式会社製NG‐F80を用いた。
また、8μm以上80μm未満の粒径を有する炭化珪素粉末が25質量%、8μm未満の粒径を有する炭化珪素粉末が10質量%となるように、南興セラミックス株式会社製GC‐#500、屋久島電工株式会社製GC‐1000F及び南興セラミックス株式会社製GC‐#6000を13.5:16.5:5.0の配合率で混合した粉末を用いた。
コロイダルシリカ(日産化学工業株式会社製スノーテックスO、固形物を20質量%含有)を6質量%秤量し、スラリ-を調整した以外実施例3と同じ方法でプリフォーム及び複合体を作製した。結果を表1に示す。
80μm以上800μm以下の粒径を有する炭化珪素粉末60質量%、8μm以上80μm未満の粒径を有する炭化珪素粉末30質量%、8μm未満の粒径を有する炭化珪素粉末10質量%及びコロイダルシリカ(日産化学工業株式会社製スノーテックスO、固形物を20質量%含有)を12質量%、水を9質量%秤量し、これらを混合してスラリ-を調整した。
実施例1と同じ方法でプリフォーム及び複合体を作製した。結果を表1に示す。
80μm以上800μm以下の粒径を有する炭化珪素粉末75質量%、8μm以上80μm未満の粒径を有する炭化珪素粉末25質量%、8μm未満の粒径を有する炭化珪素粉末5質量%及びコロイダルシリカ(日産化学工業株式会社製スノーテックスO、固形物を20質量%含有)を12質量%、水を9質量%秤量し、これらを混合してスラリ-を調整した。
実施例1と同じ方法でプリフォーム及び複合体を作製した。結果を表1に示す。
80μm以上800μm以下の粒径を有する炭化珪素粉末70質量%、8μm以上80μm未満の粒径を有する炭化珪素粉末20質量%、8μm未満の粒径を有する炭化珪素粉末10質量%及びコロイダルシリカ(日産化学工業株式会社製スノーテックスO、固形物を20質量%含有)を12質量%、水を9質量%秤量し、これらを混合してスラリ-を調整した。
また、8μm以上80μm未満の粒径を有する炭化珪素粉末が20質量%、8μm未満の粒径を有する炭化珪素粉末が10質量%となるように、大平洋ランダム株式会社製GC‐#800、大平洋ランダム株式会社製GC‐#6000を20:10の配合率で混合した。
実施例1と同じ方法でプリフォームを作製した。アルミニウム合金は、珪素12質量%、マグネシム1.6質量%である。
アルミニウム合金を珪素12質量%、マグネシム2.1質量%含有するアルミニウム合金とした以外は、実施例9と同じ方法でプリフォーム及び複合体を作製した。
80μm以上800μm以下の粒径を有する炭化珪素粉末55質量%、8μm以上80μm未満の粒径を有する炭化珪素粉末40質量%、8μm未満の粒径を有する炭化珪素粉末5質量%及びコロイダルシリカ(日産化学工業株式会社製スノーテックスO、固形物を20質量%含有)を12質量%、水を12質量%秤量し、これらを混合してスラリ-を調整した。このスラリ-を石膏型に流し込み放置した後、脱型・乾燥し成形体を得た。この成形体を空気中、1000℃で4時間焼成しプリフォ-ムとした。
Claims (5)
- 多孔質炭化珪素成形体にアルミニウム合金を含浸してなるアルミニウム‐炭化珪素質複合体であって、
該複合体中の炭化珪素の割合が60体積%以上であり、
粒径が80μm以上800μm以下である炭化珪素を60質量%以上75質量%以下含有し、
粒径が8μm以上粒径80μm未満である炭化珪素を20質量%以上30質量%以下含有し、
粒径が8μm未満である炭化珪素を5質量%以上10質量%以下含有することを特徴とするアルミニウム‐炭化珪素質複合体。 - 25℃での熱伝導率が230W/mK以上であることを特徴とする請求項1に記載のアルミニウム‐炭化珪素質複合体。
- 25℃ないし150℃における熱膨張係数が7.0ppm/K以下であることを特徴とする請求項1または2に記載のアルミニウム‐炭化珪素質複合体。
- 前記アルミニウム合金が、10質量%~14質量%の珪素と、0.5質量%~2.5質量%のマグネシウムを含有してなることを特徴とする請求項1から3のいずれか一項に記載のアルミニウム‐炭化珪素質複合体。
- 異なる粒度分布を有する3種以上の炭化珪素粉末を配合した原料粉末に、無機バインダーを添加し、成形工程及び焼成工程を経ることを特徴とする請求項1から4のいずれか一項に記載のアルミニウム‐炭化珪素質複合体の製造方法。
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