CN112823214B - Aluminium-carbon particle composite material and its production method - Google Patents
Aluminium-carbon particle composite material and its production method Download PDFInfo
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Abstract
An aluminum-carbon particle composite (1) comprises an aluminum matrix (2) and carbon particles (3) dispersed in the aluminum matrix (2). As the aluminum material of the aluminum matrix (2), an aluminum alloy is used in which Mg is added to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm.
Description
Technical Field
The present invention relates to an aluminum-carbon particle composite material and a method for producing the same.
Background
Aluminum-carbon particle composites generally have high thermal conductivity or low linear expansion. As a method for producing such a composite material, japanese patent No. 4441768 (patent document 1) discloses a method for producing a metal-carbon particle composite material by sintering a mixture of flaky powder made of aluminum or the like and flaky graphite powder as carbon particles.
However, as for the material of the cooling member or the heat dissipation member of the semiconductor device, high thermal conductivity is required in order to obtain high cooling performance or high heat dissipation performance. Therefore, an aluminum-carbon particle composite material is considered as a material for such a member.
Documents of the prior art
Patent document 1: japanese patent No. 4441768 publication
Disclosure of Invention
However, in the aluminum-carbon particle composite material, aluminum carbide (Al) is easily formed at the interface between the aluminum matrix and the carbon particles 4 C 3 ). It is considered that if aluminum carbide is formed at this interface, the thermal conductivity of the composite material decreases, and interfacial separation occurs.
The present invention has been made in view of the above-mentioned background, and an object of the present invention is to provide an aluminum-carbon particle composite material having high thermal conductivity with the generation of aluminum carbide suppressed, and a method for producing the same.
Other objects and advantages of the present invention will become apparent from the following preferred embodiments.
The present invention provides the following methods.
1) An aluminum-carbon particle composite comprising an aluminum matrix and carbon particles dispersed in the aluminum matrix,
as the aluminum material of the aluminum matrix, an aluminum alloy obtained by adding Mg to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm is used.
2) An aluminum-carbon particle composite comprising an aluminum matrix and carbon particles dispersed in the aluminum matrix, the aluminum-carbon particle composite being obtained by subjecting,
a step of adding Mg to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm, thereby preparing an aluminum alloy; and
and a step of sintering a sintered material including an aluminum material made of the aluminum alloy and carbon particles.
3) The aluminum-carbon particle composite material according to the foregoing item 1 or 2, wherein a compound layer of Al and O is formed at the interface of the aluminum matrix and the carbon particles,
the thickness of the compound layer of Al and O is 20nm or less.
4) The aluminum-carbon particle composite material according to any one of the preceding items 1 to 3, wherein a compound layer of Al, O and C is formed at the interface between the aluminum matrix and the carbon particles,
the thickness of the compound layer of Al, O and C is 20nm or less.
5) The aluminum-carbon particle composite material as recited in any one of the preceding items 1 to 4, wherein Mg is concentrated at the interface between the aluminum matrix and the carbon particles.
6) The aluminum-carbon particle composite material as recited in any one of the aforementioned items 1 to 5, wherein at least one selected from the group consisting of graphite particles, graphene, carbon fibers and carbon nanotubes is used as the carbon particles.
7) The aluminum-carbon particle composite material according to any one of the preceding items 1 to 6, which is used as a material for a cooler or a heat sink.
8) A method for producing an aluminum-carbon particle composite material, comprising:
a step of adding Mg to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm, thereby preparing an aluminum alloy; and
a step of sintering the first sintered compact 1,
the step of sintering the 1 st sintered compact includes: a step of producing an aluminum foil made of the aluminum alloy, and a step of producing a carbon particle-coated foil by coating a coating material containing carbon particles on the aluminum foil and drying the coating material,
in the step of sintering the 1 st sintered compact, a laminate in which a plurality of carbon particle-coated foils are laminated is sintered as the 1 st sintered compact.
9) A method for producing an aluminum-carbon particle composite material, comprising:
a step of adding Mg to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm, thereby preparing an aluminum alloy; and
a step of sintering the No. 2 sintered compact,
the step of sintering the 2 nd sintered compact includes a step of producing aluminum particles made of the aluminum alloy,
in the step of sintering the 2 nd sintered compact, a mixture of the aluminum particles and the carbon particles is sintered as the 2 nd sintered compact.
10 The method for producing an aluminum-carbon particle composite material according to the aforementioned item 8 or 9, wherein at least one selected from the group consisting of graphite particles, graphene, carbon fibers and carbon nanotubes is used as the carbon particles.
The present invention can exhibit the following effects.
In the aforementioned item 1, as the aluminum material of the aluminum matrix of the aluminum-carbon particle composite material, an aluminum alloy in which Mg is added to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm is used. This suppresses the formation of aluminum carbide at the interface between the aluminum matrix and the carbon particles. Therefore, the composite material has high thermal conductivity.
In the above item 2, the same effects as in the above item 1 can be exhibited.
In the aforementioned item 3, by forming a compound layer of Al and O with a predetermined thickness at the interface between the aluminum matrix and the carbon particles, the formation of aluminum carbide at the interface can be reliably suppressed, and the occurrence of cracks in the compound layer of Al and O can be reliably suppressed.
In the aforementioned item 4, by forming a compound layer of Al, O and C in a predetermined thickness at the interface between the aluminum matrix and the carbon particles, the formation of aluminum carbide at the interface can be reliably suppressed, and the occurrence of cracks in the compound layer of Al, O and C can be reliably suppressed.
In the aforementioned item 5, since Mg is concentrated at the interface between the aluminum matrix and the carbon particles, the formation of aluminum carbide at the interface can be suppressed reliably, and the bonding between the aluminum matrix and the carbon particles at the interface can be enhanced.
In the aforementioned item 6, the thermal conductivity of the composite material can be reliably improved by using at least one selected from the group consisting of graphite particles, graphene, carbon fibers, and carbon nanotubes as the carbon particles.
In the foregoing item 7, a cooler or a heat sink having high cooling performance or high heat dissipation performance may be provided.
In the above items 8 to 10, the aluminum-carbon particle composite material described in any one of the above items 1 to 6 can be produced.
Drawings
Fig. 1 is a schematic enlarged sectional view of an aluminum-carbon particle composite according to an embodiment of the present invention.
Fig. 2 is a flowchart of the manufacturing process in the method 1 for manufacturing the composite material.
Fig. 3 is a schematic perspective view of a laminate as the 1 st sintered compact.
Fig. 4 is a flowchart of the manufacturing process in the method 2 for manufacturing the composite material.
Fig. 5 is a schematic perspective view of a mixture as a 2 nd sintered compact.
Fig. 6 is a schematic enlarged sectional view of the interface of the aluminum matrix and carbon particles in the composite.
Detailed Description
Hereinafter, some embodiments of the present invention will be described with reference to the drawings.
As shown in fig. 1, an aluminum-carbon particle composite material 1 according to an embodiment of the present invention includes an aluminum matrix 2 and a plurality of carbon particles 3. Carbon particles 3 are dispersed in the aluminum matrix 2. The dispersed state of the carbon particles 3 in the aluminum matrix 2 is, for example, substantially uniform. The term "carbon particles" is intended to include carbon powder.
As the carbon particles 3, at least one selected from graphite particles, graphene, carbon fibers, and carbon nanotubes is used.
As the graphite particles, natural graphite particles (for example, flaky graphite particles), artificial graphite particles, pyrolytic graphite particles, and the like are used, and particularly, those having high thermal conductivity (for example, flaky graphite particles) are preferably used.
As the graphene, single-layer graphene, multilayer graphene, or the like is used.
As the carbon fiber, PAN-based carbon fiber, pitch-based carbon fiber, and the like are used, and pitch-based carbon fiber is particularly preferably used. The reason for this is that pitch-based carbon fibers have high thermal conductivity.
As the carbon nanotube, a single-walled carbon nanotube, a multi-walled carbon nanotube, a vapor grown carbon fiber (including VGCF (registered trademark)), or the like is used.
The size of the carbon particles 3 is not limited. When the carbon particles 3 are graphite particles, the average length of the graphite particles in the longest axis direction is particularly preferably 30 μm or more. The upper limit of the average length of the graphite particles in the longest axis direction is not particularly limited, and is usually 3mm. The length of the graphite particles in the longest axis direction means the length of the graphite particles in the longest direction. When the carbon particles 3 are carbon fibers, the carbon fibers preferably have an average fiber length of 10 μm to 2mm. When the carbon particles 3 are carbon nanotubes, the average length of the carbon nanotubes is particularly preferably 1 μm to 10 μm.
When the carbon particles 3 are graphite particles, the aspect ratio of the graphite particles is not limited, and is particularly preferably 30 or more. The upper limit of the aspect ratio is not limited, and is usually 100.
Further, the carbon particles 3 may be heat-treated at a temperature of 2000 to 3000 ℃ in an inert atmosphere.
As the aluminum material of the aluminum substrate 2, an aluminum alloy obtained by adding Mg to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm is used. Hereinafter, this aluminum alloy is referred to as "specific aluminum alloy".
The aluminum purity (i.e., al content) of the specific aluminum alloy is 98.97 mass% or more, and particularly preferably 99.00 mass% or more.
The pure aluminum having a purity of 99.00 mass% or more is preferably selected from aluminum alloy a1000 series aluminum specified by JIS (japanese industrial standards). Specifically, as a 1000-based aluminum, A1N99, a1050, A1N30, a1100, and the like are preferably used.
Such pure aluminum has a purity of 99.00 mass% or more, i.e., an Al content of 99.00 mass% or more, and further contains Si (silicon), fe (iron), cu (copper), and Mg (magnesium).
Here, in JIS, the Mg content of pure aluminum is defined to be 0.05 mass% (500 mass ppm) or less. However, if the chemical composition of each of the pure aluminum actually available was quantitatively analyzed by ICP emission spectrometry, the Mg content was 0.001 mass% (10 mass ppm) or less.
Among the four elements of Si, fe, si, and Mg contained in pure aluminum, in addition to Al, si, fe, and Cu are inevitable impurities. These elements (Si, fe and Cu) are derived from an aluminum raw material, i.e., a bauxite component (Al) 2 O 3 、SiO 2 、Fe 2 O 3 ) And impurity elements derived from an electrolytic bath or an electrode for molten salt electrolysis.
On the other hand, as regards Mg, mg and Mg compounds are not used at all in the bayer process, which is an industrial process for alumina (bauxite → alumina), and in the Hall-heroult process, which is a purification process for aluminum (alumina → aluminum). Therefore, the Mg content in the pure aluminum does not fall within the range of 20 to 300 mass ppm unless Mg is added to the pure aluminum. In other words, in order to set the Mg content in the pure aluminum in the range of 20 to 300 mass ppm, mg must be intentionally added to the pure aluminum.
The aluminum-carbon particle composite material 1 of the present embodiment is basically produced by the following steps: preparing a specific aluminum alloy; and a step of sintering a sintered material including an aluminum material made of a specific aluminum alloy and carbon particles.
Two preferred 1 st and 2 nd manufacturing methods capable of manufacturing the composite material 1 are described in detail below. However, the composite material of aluminum-carbon particles of the present invention is not limited to the composite materials produced by the production methods 1 and 2, and may be produced by other production methods.
As shown in fig. 2 and 3, the method 1 for producing the composite material 1 includes: a step S1 of preparing a specific aluminum alloy; and a step S2 of sintering the 1 st sintered compact 11.
In the step S1 of preparing a specific aluminum alloy, mg is added to a pure aluminum melt (e.g., a melt of a 1000-based aluminum) having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm, thereby preparing the specific aluminum alloy (specifically, a melt of the specific aluminum alloy or a molten specific aluminum alloy). Then, a specific aluminum alloy casting is produced by casting the specific aluminum alloy.
The step S2 of sintering the 1 st sintered compact 11 includes: a step S2a of producing an aluminum foil 6 made of a specific aluminum alloy, and a step S2b of producing a carbon particle-coated foil 7 by coating a coating material (not shown) containing carbon particles 3 on the aluminum foil 6 and drying the coating material.
In the step S2a of producing the aluminum foil 6, the specific aluminum alloy prepared in the step S1 of preparing the specific aluminum alloy is used as a material of the aluminum foil 6, and the aluminum foil 6 is produced by a conventional method. Specifically, the aluminum foil 6 is manufactured, for example, by hot rolling or cold rolling (including warm rolling) a specific aluminum alloy casting. Further, it is preferable to anneal the aluminum foil 6 after rolling.
The hot rolling temperature is not limited, and is, for example, 300 to 600 ℃. The annealing temperature is not limited, and is, for example, 200 to 400 ℃.
The thickness of the aluminum foil 6 is not limited, but is, for example, 10 to 100 μm.
In step S2b of producing the carbon particle-coated foil 7, the coating material contains the carbon particles 3 and further contains a binder liquid (not shown) as described above.
The binder liquid is basically prepared by dissolving a binder resin in a solvent. It is preferable that the carbon particles 3 in the coating material and the binder liquid are in a mixed state, and the carbon particles 3 are uniformly dispersed in the binder liquid.
If necessary, additives such as a thickener for adjusting the viscosity of the binder liquid, a dispersant for uniformly dispersing the carbon particles in the binder liquid, and a surface conditioner may be added to the binder liquid.
The binder resin is used to bind the carbon particles 3 with the aluminum foil 6. As the binder resin, an organic resin is generally used, and specifically, polyethylene oxide, polyvinyl alcohol, acrylic resin, or the like is used.
The solvent is used to dissolve the binder resin. As the solvent, a hydrophilic solvent (e.g., isopropyl alcohol, water), an organic solvent, or the like is used.
When the binder solution and the carbon particles 3 are mixed and stirred, a disperser, a planetary mixer, a bead mill, or the like is used as a mixer.
The method and apparatus (not shown) for applying the paint to the aluminum foil 6 are not limited. As the coating device, a three-roll coater (offset type), a two-roll coater (direct type), a gravure coater, a knife coater, a die coater, a spray coater, a curtain coater, a reverse roll coater, or the like is used. The coating material is applied to the aluminum foil 6 in layers by such an application device.
The paint applied to the aluminum foil 6 is dried to evaporate the solvent in the paint from the paint. Thereby, a carbon particle-coated foil 7 was obtained.
The carbon particle-coated foil 7 is a foil in which carbon particles 3 are coated in a state of being dispersed in the surface direction of the aluminum foil 6. Further, the carbon particles 3 are bonded to the aluminum foil 6 with a binder resin so that the carbon particles 3 do not fall off the aluminum foil 6. It is preferable that the dispersion state of the carbon particles 3 in the surface direction of the aluminum foil 6 is as uniform as possible.
The method and apparatus (not shown) for drying the coating material are not limited, and a drying oven, for example, may be used as the drying apparatus. The drying conditions of the coating material are not particularly limited as long as the solvent in the coating material can be evaporated and removed from the coating material, and the drying temperature is usually 100 to 200 ℃ and the drying time is usually 1 to 10 minutes.
The coating and drying of the coating material on the aluminum foil 6 are preferably performed by a roll-to-roll method using a unwinding roll (not shown) and a winding roll (not shown). In this case, the coating and drying of the coating material are performed by using a strip of the aluminum foil 6 as the aluminum foil 6, and winding the strip of the aluminum foil 6 unwound from the unwinding roll onto the winding roll so that the strip of the aluminum foil 6 passes through the coating device and the drying device in this order.
When the strip of aluminum foil 6 passes through the coating apparatus, the coating material is continuously applied in layers on the strip of aluminum foil 6 by the coating apparatus. Then, while the strip of the aluminum foil 6 passes through the drying device, the coating material applied to the strip of the aluminum foil 6 is dried by the drying device and the carbon particles 3 are bonded with the strip of the aluminum foil 6 with the binder resin. Therefore, when the strip of the aluminum foil 6 passes through the drying device 6, the strip of the aluminum foil 6 becomes a strip of the carbon particle-coated foil 7, and the strip of the carbon particle-coated foil 7 is wound onto a winding roll.
In step S2 of sintering the 1 st sintered compact 11, the laminate 12 in which the plurality of carbon particle-coated foils 7 are laminated is sintered as the 1 st sintered compact 11.
The laminate 12 is formed by laminating a plurality of carbon particle-coated foils 7, for example, so that the plurality of carbon particle-coated foils 7 are laminated. The carbon particle-coated foil 7 is obtained by, for example, cutting a strip of the carbon particle-coated foil 7 wound onto a winding roll into a predetermined shape (e.g., a square shape).
Next, the laminate 12 is sintered by pressing and heating in a predetermined sintering atmosphere (e.g., non-oxidizing atmosphere, vacuum) in a predetermined direction.
As a result, the plurality of carbon particle-coated foils 7 constituting the laminate 12 are joined and integrated (more specifically, are sintered and integrated), and as a result, the aluminum-carbon particle composite material described above is obtained (see fig. 1).
The direction in which the laminate 12 is pressed when sintering the laminate 12 is generally uniaxial, specifically, the thickness direction of the laminate 12 (that is, the lamination direction of the carbon particle-coated foil 7).
The method of sintering the laminate 12 is not limited, and as the sintering method, a vacuum hot press method, a discharge plasma sintering method (also referred to as a pulse energization sintering method), a hot hydrostatic press sintering method (HIP method), an extrusion method, a rolling method, or the like can be used.
The heating temperature of the laminate 12 for sintering the laminate 12, that is, the sintering temperature of the laminate 12 is not limited, and is particularly preferably a temperature lower than the melting point of the specific aluminum alloy as the aluminum material of the aluminum foil 6.
As the sintering conditions of the laminate 12, preferred sintering conditions of the laminate 12 when the sintering method of the laminate 12 is the discharge plasma sintering method are as follows.
The sintering temperature of the laminate 12 is 450 to 660 ℃, the sintering time (i.e., the holding time of the sintering temperature) is 10 to 300 minutes, and the pressing force to the laminate 12 is 10 to 40MPa.
The binder resin present in the laminate 12 is removed from the laminate 12 by sublimation, thermal decomposition, or the like in the process of heating the laminate 21 in the step S2 of sintering the 1 st sintered compact 11 so that the temperature of the laminate 12 rises from substantially room temperature to the sintering temperature of the laminate 12.
In the case where the solvent remains in the stacked body 12, the remaining solvent is evaporated and removed from the stacked body 12 in the step S2 of sintering the 1 st sintered compact 11 so that the temperature of the stacked body 12 rises from substantially room temperature to the sintering temperature of the stacked body 12.
In the step S2 of sintering the first sintered compact 11, the laminate 12 is sintered as described above, so that the aluminum material of the aluminum foil 6 of the carbon particle-coated foil 7, i.e., the specific aluminum alloy, is changed to the aluminum matrix 2 of the composite material 1. In the composite material 1, the aluminum matrix 2 penetrates into the gap between the carbon particles 3, 3 so that the gap disappears.
In the present embodiment, the laminate 12 is formed in a state in which a plurality of carbon particle-coated foils 7 are laminated by laminating a plurality of carbon particle-coated foils 7 as described above, but in the present invention, for example, a plurality of carbon particle-coated foils 7 (specifically, the strips of the carbon particle-coated foils 7) may be wound into a roll shape by a laminate to form a plurality of carbon particle-coated foils 7 laminated.
As shown in fig. 4 and 5, the method 2 for producing the composite material 1 includes: a step S11 of preparing a specific aluminum alloy and a step S12 of sintering the No. 2 sintered compact 13. The term "aluminum particles" is intended to include aluminum powder.
The step S1 of preparing the specific aluminum alloy is performed, for example, in the same manner as the step S1 of preparing the specific aluminum alloy in the first method for producing the composite material 1.
The step S12 of sintering the 2 nd sintered compact 13 includes a step S12a of producing aluminum particles 8 made of a specific aluminum alloy.
In step S12a of producing the aluminum particles 8, the specific aluminum alloy prepared in step S11 of preparing the specific aluminum alloy is used as a material of the aluminum particles 8, and the aluminum particles 8 are produced by a conventional method. Specifically, the aluminum particles 8 are produced by a direct pulverization method (for example, an atomization method, a melt stirring method, a centrifugal force method), a mechanical pulverization method (for example, a masher method, a vibration pulverization method), or the like.
In the step S12 of sintering the 2 nd sintered compact 13, the mixture 14 of the aluminum particles 8 and the carbon particles 3 is sintered as the 2 nd sintered compact 13.
The mixture 14 is obtained by mixing the aluminum particles 8 and the carbon particles 3. In fig. 5, a green compact obtained by mixing and compression-molding aluminum particles 8 and carbon particles 3 is used as the mixture 14. It is desirable that the state of mixing of the aluminum particles 8 with the carbon particles 3 in the mixture 14 is uniform.
Then, the mixture 14 is sintered by pressurizing and heating in a predetermined sintering atmosphere (e.g., non-oxidizing atmosphere, vacuum) in a predetermined direction.
The mixture 14 was sintered in this manner, whereby the above-described aluminum-carbon particle composite material (see fig. 1) 1 was obtained.
The direction of pressing the mixture 14 when sintering the mixture 14 is generally uniaxial, specifically, for example, the thickness direction of the mixture 14.
In the step S12 of sintering the 2 nd sintered compact 13, the mixture 14 is sintered as described above, and the aluminum material of the aluminum particles 8, i.e., the specific aluminum alloy, becomes the aluminum matrix 2 of the composite material 1. In the composite material 1, the aluminum matrix 2 penetrates into the gap between the carbon particles 3, 3 so that the gap disappears.
The sintering method and sintering conditions of the mixture 14 are not limited, and are, for example, the same as those of the laminate 12 in the above-described method 1 for producing the composite material 1.
In the composite material 1 obtained by the above-described production method 1 or 2, by using a specific aluminum alloy as the aluminum material of the aluminum substrate 2, a compound layer (not shown) of Al (aluminum) and O (oxygen) and a compound layer (not shown) of Al (aluminum), O (oxygen), and C (carbon) are formed at the interface 4 between the aluminum substrate 2 and the carbon particles 3.
Hereinafter, the interface 4 between the aluminum matrix 2 and the carbon particles 3 is referred to as "Al/C interface 4", the compound layer of Al and O is referred to as "Al — O compound layer", and the compound layer of Al, O, and C is referred to as "Al — O — C compound layer".
The Al-O compound layer is different from the Al-O-C compound layer. That is, the Al — O compound layer means an Al — O compound layer not combined with C or an Al — O compound layer not substantially combined with C.
Both the Al-O compound layer and the Al-O-C compound layer function as barrier layers to suppress the formation of aluminum carbide (Al) by the combination of aluminum in the aluminum matrix 2 and carbon particles 3 4 C 3 )。
Therefore, by forming the Al-O compound layer at the Al/C interface 4, the generation of aluminum carbide at the Al/C interface 4 is suppressed. Therefore, the composite material 1 has high thermal conductivity. Further, by forming the Al-O-C compound layer at the Al/C interface 4, the formation of aluminum carbide at the Al/C interface 4 is further suppressed. Therefore, the composite material 1 has a higher thermal conductivity.
The thickness of the Al-O compound layer is preferably 20nm or less. In this case, the occurrence of cracks in the compound layer can be reliably suppressed. A preferred lower limit of the thickness of the compound layer is 1nm. When the thickness of the compound layer is 1nm or more, the formation of aluminum carbide at the Al/C interface 4 can be reliably suppressed. A more preferable lower limit of the thickness of the compound layer is 5nm.
The thickness of the Al-O-C compound layer is preferably 20nm or less. In this case, the generation of cracks in the compound layer can be reliably suppressed. A preferred lower limit of the thickness of the compound layer is 1nm. When the thickness of the compound layer is 1nm or more, the formation of aluminum carbide at the Al/C interface 4 can be reliably suppressed. A more preferable lower limit of the thickness of the compound layer is 5nm.
In addition, in the Al/C interface 4, aluminum substrate 2, al-O compound layer the Al-O-C compound layer and the carbon particles 3 are arranged in the order Al (aluminum matrix 2)/Al-O compound layer/Al-O-C compound layer/C (carbon particles 3).
It is desirable that both the Al-O compound layer and the Al-O-C compound layer have an amorphous structure. This is because the strength of the Al/C interface 4 is high, and therefore, when a large load is applied to the composite material 1, the possibility that the fracture mode of the composite material 1 becomes the base material fracture rather than the interface fracture increases.
The structure of the Al/C interface 4 of the aluminum-carbon particle composite material 1 will be described in detail below with reference to fig. 6.
As shown in the figure, at the Al/C interface 4 of the composite material 1, aluminum substrate 2, al-O compound layer 23 the Al-O-C compound layer 24 and the carbon particles 3 are arranged in the order of Al (aluminum matrix 2)/Al-O compound layer 23/Al-O-C compound layer 24/C (carbon particles 3) as described above.
Hereinafter, in the Al/C interface 4, a region of the aluminum matrix 2 is referred to as an aluminum matrix region 21, and a region of the carbon particles 3 is referred to as a carbon region 22.
In the Al/C interface 4, an Al-O compound layer 23 and an Al-OC compound layer 24 are present in the form of an intermediate layer 25 between the aluminum matrix region 21 and the carbon region 22. The intermediate layer 25 is assumed to have an amorphous structure (amorphous form).
Mg in the composite material 1 is present in enriched form at the Al/C interface 4. This can be confirmed by cross-sectional TEM analysis or the like of the Al/C interface 4. In detail, it is presumed that the Mg of the composite material 1 is mostly present in the Al-O compound layer 23 or the Al-O-C compound layer 24 among the aluminum matrix region 21, the Al-O compound layer 23, the Al-O-C compound layer 24, and the carbon region 22, or mostly present in two layers 23, 24 of the Al-O compound layer 23 and the Al-O-C compound layer 24 across the two layers 23, 24. Further, the meaning of "most" includes about half or more.
Therefore, when Mg is present in the composite material 1, the content of Mg in the aluminum alloy of the aluminum material used as the aluminum matrix 2 in the production of the composite material 1 is a ratio of the amount of Mg to the total area of the aluminum matrix region 21, the Al — O compound layer 23, and the Al — O — C compound layer 24 in the composite material 1, and the ratio is in the range of 20 to 300 mass ppm, whereby the formation of aluminum carbide at the Al/C interface 4 can be suppressed.
When Mg is present in the Al — O compound layer 23, it is presumed that Mg is present in the Al — O compound layer 23 in the form of a compound of Mg and O (oxygen) (which is referred to as "Mg — O compound"). In addition, in the case where Mg is present in the Al-O-C compound layer 24, it is presumed that Mg is present in the form of an Mg-O compound in the Al-O-C compound layer 24.
The presence of Mg in the composite material 1 enriched at the Al/C interface 4 can suppress the formation of aluminum carbide at the Al/C interface 4. Further, it is considered that the interface bonding between the Al — O compound layer 23 and the Al — O — C compound layer 24 at the Al/C interface 4, the interface bonding between the Al — O — C compound layer 24 and the carbon region 22, or both of them is strengthened, and as a result, the bonding between the aluminum matrix 2 and the carbon particles 3 at the Al/C interface 4 is strengthened.
The composite material 1 of the present embodiment has high thermal conductivity, and is therefore suitable as a material for a cooler or a heat sink. Therefore, when the composite material 1 is used as a material for a cooler or a radiator, the cooler or the radiator having high cooling performance or high heat dissipation performance can be obtained.
In detail, the composite material 1 is suitably used as a material for coolers, radiators, power modules, heat exchangers, batteries, vehicles, automobiles, engines, communication equipment, power generation equipment, and the like.
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While the embodiments of the present invention have been described above, the present invention is not limited to the above embodiments, and various modifications can be made without departing from the scope of the present invention.
Examples
Specific examples of the present invention and comparative examples are shown below. However, the present invention is not limited to the following examples.
TABLE 1
< example 1>
In example 1, an aluminum-carbon particle composite was produced substantially in accordance with the method 1 for producing an aluminum-carbon particle composite described in the above embodiment. The specific manufacturing method is as follows.
A specific aluminum alloy (specifically, a melt of a specific aluminum alloy or a molten specific aluminum alloy) having an Mg content of 50 mass ppm (0.005 mass%) was prepared by adding a predetermined amount of Mg powder to a melt of pure aluminum (alloy No. A1N 99) having a purity of 99.99 mass%. Then, a specific aluminum alloy casting is produced by casting a specific aluminum alloy.
The chemical composition of the specific aluminum alloy was quantitatively analyzed by ICP emission spectrometry. The results are shown in the column "chemical composition" in table 1. In the column, "-" means not more than the detection limit (i.e., not more than 0.001 mass% (10 mass ppm)).
Next, a specific aluminum alloy casting was used as a material of the aluminum foil, and a strip of the aluminum foil was produced by cold rolling. Thereafter, the strip of aluminum foil was annealed. The annealing temperature was 400 ℃. The thickness of the strip of aluminum foil was 20 μm.
Further, scale-like graphite particles as carbon particles were mixed with a binder liquid and stirred to prepare a coating material. The average length of the flaky graphite particles in the longest axis direction was 300 μm, and the aspect ratio was 30. The average length of the flaky graphite particles in the longest axis direction was calculated by the following method. That is, 100 flaky graphite particles arbitrarily selected from a large number of flaky graphite particles dispersed on a glass plate were observed with an optical microscope, and the length of each flaky graphite particle in the longest direction was measured. Then, the arithmetic average of these values was defined as the average length of the flaky graphite particles in the longest axis direction.
The binder liquid is prepared by dissolving a binder resin in a solvent. A mixture of polyethylene oxide and polyvinyl alcohol was used as the binder resin, and a mixture of water and isopropyl alcohol was used as the solvent.
Next, the coating material was applied to the bar of aluminum foil using a three-roll coater and dried at 150 ℃, thereby obtaining a bar of scaly graphite particle-coated foil as a bar of carbon particle-coated foil.
The foil-coated strip was cut into a square shape, and a plurality of cut pieces (i.e., the scaly graphite particle-coated foils) were stacked to form a stacked body as a1 st sintered material, in which a plurality of scaly graphite particle-coated foils were stacked.
Next, the laminate was pressed and heated in a vacuum to perform sintering, thereby producing an aluminum-flaky graphite particle composite material as an aluminum-carbon composite material. The sintering temperature of the laminate was 600 ℃, the sintering time was 180 minutes, the direction of pressing the laminate was the thickness direction of the laminate, and the pressing force to the laminate was 20MPa. The thickness of the composite material was 0.5mm. The volume ratio of the flaky graphite particles to the aluminum matrix in the composite material was 30 (flaky graphite particles): 70 (aluminum matrix).
In order to examine the thermal conductivity of the composite material, the thermal diffusivity of the composite material was measured by a laser flash method, and the thermal conductivity of the composite material at 25 ℃ was calculated by multiplying the thermal diffusivity by the density and specific heat of the composite material. The results are shown in the column "thermal conductivity" in table 1.
In addition, after the distribution state of Mg in the composite material is investigated by using the cross-sectional TEM analysis of the Al/C interface of the composite material, the Mg in the composite material is enriched in the Al/C interface.
< example 2>
A specific aluminum alloy having an Mg content of 50 mass ppm (0.005 mass%) was prepared by adding a predetermined amount of Mg powder to a melt of pure aluminum (alloy designation: a 1100) having a purity of 99.00 mass%. Then, by casting the specific aluminum alloy, a specific aluminum alloy casting is produced.
The chemical composition of the specific aluminum alloy was quantitatively analyzed by ICP emission spectrometry. The results are shown in the column "chemical composition" in table 1.
Using this specific aluminum alloy casting, an aluminum-flaky graphite particle composite was produced in the same manner as in example 1 above.
The thermal conductivity of the composite material was calculated in the same manner as in example 1. The results are shown in the column "thermal conductivity" in table 1.
Further, the distribution state of Mg in the composite material was examined by the same method as in example 1, and it was found that Mg in the composite material was distributed in the same manner as in example 1.
< example 3>
A specific aluminum alloy having an Mg content of 200 mass ppm (0.020 mass%) was prepared by adding a predetermined amount of Mg powder to a melt of pure aluminum (alloy No. a 1100) having a purity of 99.00 mass%. Then, by casting the specific aluminum alloy, a specific aluminum alloy casting is produced.
The chemical composition of the specific aluminum alloy was quantitatively analyzed by ICP emission spectrometry. The results are shown in the column "chemical composition" in table 1.
Using this specific aluminum alloy casting, an aluminum-flaky graphite particle composite was produced in the same manner as in example 1 above.
The thermal conductivity of the composite material was calculated in the same manner as in example 1. The results are shown in the column "thermal conductivity" in table 1.
Further, the distribution state of Mg in the composite material was examined by the same method as in example 1, and it was found that Mg in the composite material was distributed in the same manner as in example 1.
< comparative example 1>
A strip of aluminum foil made of pure aluminum (alloy No. A1N 99) having a purity of 99.99 mass% was prepared. The thickness was 20 μm.
The chemical composition of pure aluminum was quantitatively analyzed by ICP emission spectrometry. The results are shown in the column "chemical composition" in table 1.
Using the aluminum foil strip, an aluminum-flaky graphite particle composite was produced in the same manner as in example 1.
The thermal conductivity of the composite material was calculated in the same manner as in example 1. The results are shown in the column "thermal conductivity" in table 1.
< comparative example 2>
A strip of aluminum foil made of pure aluminum (alloy No. A1100) having a purity of 99.00 mass% was prepared. The thickness was 20 μm.
The chemical composition of pure aluminum was quantitatively analyzed by ICP emission spectrometry. The results are shown in the column "chemical composition" in table 1.
Using the aluminum foil strip, an aluminum-flaky graphite particle composite was produced in the same manner as in example 1.
The thermal conductivity of the composite material was calculated by the same method as in example 1. The results are shown in the column "thermal conductivity" in table 1.
< comparative example 3>
A strip of aluminum foil made of aluminum alloy (alloy No. a 6063) was prepared instead of pure aluminum. The thickness was 20 μm.
The chemical components of the aluminum alloy are quantitatively analyzed by adopting an ICP emission spectrometry. The results are shown in the column "chemical composition" in table 1.
Using the aluminum foil strip, an aluminum-flaky graphite particle composite was produced in the same manner as in example 1.
The thermal conductivity of the composite material was calculated by the same method as in example 1. The results are shown in the column "thermal conductivity" in table 1.
Evaluation
As shown in table 1, the thermal conductivity of the composite materials of examples 1 to 3 and the thermal conductivity of the composite materials of comparative examples 1 to 2 were both higher than that of the composite material of comparative example 3.
Further, the thermal conductivity of the composite material of example 1 was higher than that of the composite material of comparative example 1.
In addition, the thermal conductivity of the composites of examples 2 and 3 was compared with that of the composite of comparative example 2, the former being higher than the latter.
The present application claims priority based on japanese patent application No. 2018-218031 filed on 21/11/2018, the disclosure of which directly forms part of the present application.
It must be understood that the words and expressions used herein have been used for the purpose of illustration and not of limitation, and there is no intention, in the use of such words and expressions, of excluding any equivalents of the features shown and described or portions thereof, but it is recognized that various modifications are possible within the scope of the invention claimed.
The present invention can be embodied in a number of different forms and this disclosure should be considered as providing a disclosure of embodiments of the principles of the present invention which are not intended to limit the invention to the preferred embodiments described and/or illustrated herein, with the understanding that the various illustrated embodiments are described herein.
Industrial applicability
The present invention can be used for an aluminum-carbon particle composite material and a method for producing the same.
Description of the reference numerals
1: aluminum-carbon particle composite material
2: aluminum matrix
3: carbon particles
4: interface of aluminum matrix and carbon particles (Al/C interface)
6: aluminum foil
7: foil coated with carbon particles
8: aluminum particles
11: 1 st sintered compact
12: laminated body
13: 2 nd sintered compact
14: mixing body
21: region of aluminum matrix (aluminum matrix region)
22: region of carbon particles (carbon region)
23: compound layer of Al and O (Al-O compound layer)
24: compound layer of Al, O and C (Al-O-C compound layer)
Claims (6)
1. An aluminum-carbon particle composite comprising an aluminum matrix and carbon particles dispersed in the aluminum matrix,
as the aluminum material for the aluminum matrix, an aluminum alloy obtained by adding Mg to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm is used,
the carbon particles are at least one selected from the group consisting of graphite particles, graphene and carbon fibers,
at the interface between the aluminum matrix and the carbon particles, there are formed:
a compound layer of Al and O having a thickness of 20nm or less, and/or
A compound layer of Al, O and C having a thickness of 20nm or less.
2. An aluminum-carbon particle composite comprising an aluminum matrix and carbon particles dispersed in the aluminum matrix, the aluminum-carbon particle composite being obtained by subjecting,
a step of adding Mg to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm, thereby preparing an aluminum alloy; and
a step of sintering a sintered compact containing an aluminum material made of the aluminum alloy and carbon particles,
at least one carbon particle selected from the group consisting of graphite particles, graphene and carbon fibers is used as the carbon particle,
at the interface between the aluminum matrix and the carbon particles, there are formed:
a compound layer of Al and O having a thickness of 20nm or less, and/or
A compound layer of Al, O and C having a thickness of 20nm or less.
3. The aluminum-carbon particle composite of claim 1 or 2, wherein Mg is concentrated at the interface of the aluminum matrix and the carbon particles.
4. The aluminum-carbon particle composite material according to claim 1 or 2, which is used as a material for a cooler or a heat sink.
5. A method for producing an aluminum-carbon particle composite material, comprising:
a step for preparing an aluminum alloy by adding Mg to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm; and
a step of sintering the first sintered compact 1,
the step of sintering the 1 st sintered compact includes: a step for producing an aluminum foil made of the aluminum alloy, and a step for producing a carbon particle-coated foil by coating a coating material containing carbon particles on the aluminum foil and drying the coating material,
at least one carbon particle selected from the group consisting of graphite particles, graphene and carbon fibers is used as the carbon particle,
and a step of sintering the 1 st sintered material, wherein a laminate obtained by laminating a plurality of the carbon particle-coated foils is sintered as the 1 st sintered material to obtain an aluminum-carbon particle composite material in which a compound layer of Al and O having a thickness of 20nm or less and/or a compound layer of Al, O and C having a thickness of 20nm or less is formed at the interface between the aluminum foil and the carbon particles.
6. A method for producing an aluminum-carbon particle composite material, comprising:
a step for preparing an aluminum alloy by adding Mg to pure aluminum having a purity of 99.00 mass% or more so that the Mg content is in the range of 20 to 300 mass ppm; and
a step of sintering the 2 nd sintered compact,
the step of sintering the 2 nd sintered compact includes a step of producing aluminum particles made of the aluminum alloy,
in the step of sintering the 2 nd sintered compact, a mixture of the aluminum particles and carbon particles is sintered as the 2 nd sintered compact to obtain an aluminum-carbon particle composite material in which a compound layer of Al and O having a thickness of 20nm or less and/or a compound layer of Al, O and C having a thickness of 20nm or less is formed at an interface between the aluminum particles and the carbon particles,
at least one selected from graphite particles, graphene, and carbon fibers is used as the carbon particles.
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| JP2018218031 | 2018-11-21 | ||
| JP2018-218031 | 2018-11-21 | ||
| PCT/JP2019/040872 WO2020105328A1 (en) | 2018-11-21 | 2019-10-17 | Aluminum-(carbon particle) composite material and method for producing same |
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| CN113699417B (en) * | 2021-08-30 | 2022-03-08 | 中北大学 | Al (aluminum)2O3/Fe3O4Preparation method of @ GNS hybrid reinforced aluminum-based composite material |
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| US5508120A (en) * | 1994-08-12 | 1996-04-16 | The Dow Chemical Company | Boron carbide cermet structural materials with high flexure strength at elevated temperatures |
| JP4597279B2 (en) | 1998-07-31 | 2010-12-15 | 弘治 大石橋 | Thermally conductive composite material |
| JP2000345254A (en) * | 1999-06-03 | 2000-12-12 | Toyota Motor Corp | Aluminum base composite material and its production |
| JP4711165B2 (en) * | 2004-06-21 | 2011-06-29 | 日立金属株式会社 | High thermal conductivity / low thermal expansion composite and method for producing the same |
| JP4279221B2 (en) * | 2004-09-10 | 2009-06-17 | 日信工業株式会社 | Composite metal material and manufacturing method thereof, caliper body, bracket, disk rotor, drum, and knuckle |
| CN1944698A (en) * | 2006-10-24 | 2007-04-11 | 北京科技大学 | Super high heat conduction, low heat expansion coefficient composite material and its preparing method |
| JP5229934B2 (en) * | 2007-07-05 | 2013-07-03 | 住友精密工業株式会社 | High thermal conductivity composite material |
| WO2010007974A1 (en) * | 2008-07-17 | 2010-01-21 | 電気化学工業株式会社 | Process for production of aluminum-diamond composite |
| KR20130000647A (en) * | 2011-06-23 | 2013-01-03 | 권한상 | Method for processing carbon nanotube-aluminum composite wire for electrical cable application and products produced thereby |
| CN103343265B (en) * | 2013-07-24 | 2015-12-02 | 上海交通大学 | Graphite/silicon hybrid buildup high-thermal-conductivity low-expansibility aluminum matrix composite |
| CN104264000B (en) * | 2014-09-03 | 2016-09-07 | 上海交通大学 | The high thermal conductivity aluminum matrix composite of Graphene modification and method for preparing powder metallurgy thereof |
| CN104630570B (en) * | 2014-12-11 | 2017-02-22 | 中车青岛四方机车车辆股份有限公司 | High-damping carbon nanotube/aluminum alloy composite material and preparation method thereof |
| JP6749087B2 (en) | 2015-10-30 | 2020-09-02 | 矢崎総業株式会社 | Fastening member |
| US20190001652A1 (en) * | 2015-12-24 | 2019-01-03 | Showa Denko K.K. | Method for producing metal-carbon fiber composite material |
| JP2016180185A (en) | 2016-05-09 | 2016-10-13 | デンカ株式会社 | Aluminum alloy-ceramic composite, production method of the composite and stress buffer composed of the composite |
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