CN117532002A - Preparation method of high-thermal conductivity high-surface-finish lamellar diamond metal matrix composite - Google Patents
Preparation method of high-thermal conductivity high-surface-finish lamellar diamond metal matrix composite Download PDFInfo
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- CN117532002A CN117532002A CN202311522400.4A CN202311522400A CN117532002A CN 117532002 A CN117532002 A CN 117532002A CN 202311522400 A CN202311522400 A CN 202311522400A CN 117532002 A CN117532002 A CN 117532002A
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- 239000010432 diamond Substances 0.000 title claims abstract description 319
- 229910003460 diamond Inorganic materials 0.000 title claims abstract description 317
- 238000002360 preparation method Methods 0.000 title claims abstract description 34
- 239000011156 metal matrix composite Substances 0.000 title abstract description 19
- 229910052751 metal Inorganic materials 0.000 claims abstract description 342
- 239000002184 metal Substances 0.000 claims abstract description 342
- 239000002245 particle Substances 0.000 claims abstract description 211
- 238000000034 method Methods 0.000 claims abstract description 108
- 239000002131 composite material Substances 0.000 claims abstract description 77
- 230000008569 process Effects 0.000 claims abstract description 55
- 239000000843 powder Substances 0.000 claims description 159
- 239000011888 foil Substances 0.000 claims description 71
- 239000010949 copper Substances 0.000 claims description 66
- 239000011248 coating agent Substances 0.000 claims description 65
- 238000000576 coating method Methods 0.000 claims description 65
- 239000013078 crystal Substances 0.000 claims description 64
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 61
- 229910052802 copper Inorganic materials 0.000 claims description 58
- 238000005245 sintering Methods 0.000 claims description 53
- 239000011159 matrix material Substances 0.000 claims description 38
- 238000002844 melting Methods 0.000 claims description 30
- 230000008018 melting Effects 0.000 claims description 30
- 238000003892 spreading Methods 0.000 claims description 28
- 230000007480 spreading Effects 0.000 claims description 28
- 238000005406 washing Methods 0.000 claims description 27
- 238000010438 heat treatment Methods 0.000 claims description 23
- 238000001816 cooling Methods 0.000 claims description 19
- 238000013329 compounding Methods 0.000 claims description 16
- 238000007747 plating Methods 0.000 claims description 16
- 230000003746 surface roughness Effects 0.000 claims description 15
- 238000007599 discharging Methods 0.000 claims description 12
- 238000011049 filling Methods 0.000 claims description 11
- 238000001755 magnetron sputter deposition Methods 0.000 claims description 11
- 238000004321 preservation Methods 0.000 claims description 10
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 9
- 239000002253 acid Substances 0.000 claims description 9
- 239000003513 alkali Substances 0.000 claims description 9
- 238000001035 drying Methods 0.000 claims description 9
- 238000012216 screening Methods 0.000 claims description 9
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 7
- 229910052709 silver Inorganic materials 0.000 claims description 7
- 239000004332 silver Substances 0.000 claims description 7
- 239000011863 silicon-based powder Substances 0.000 claims description 4
- 229910052721 tungsten Inorganic materials 0.000 claims description 4
- 229910000881 Cu alloy Inorganic materials 0.000 claims description 3
- 229910001316 Ag alloy Inorganic materials 0.000 claims description 2
- 229910000838 Al alloy Inorganic materials 0.000 claims description 2
- 229910052726 zirconium Inorganic materials 0.000 claims description 2
- 238000000227 grinding Methods 0.000 abstract description 12
- 230000001105 regulatory effect Effects 0.000 abstract description 12
- 238000005498 polishing Methods 0.000 abstract description 9
- 238000003466 welding Methods 0.000 abstract description 8
- 238000009713 electroplating Methods 0.000 abstract description 4
- 230000006872 improvement Effects 0.000 abstract description 4
- 239000010410 layer Substances 0.000 description 55
- 239000000463 material Substances 0.000 description 53
- 230000033228 biological regulation Effects 0.000 description 9
- 239000000956 alloy Substances 0.000 description 8
- 229910045601 alloy Inorganic materials 0.000 description 8
- 230000001276 controlling effect Effects 0.000 description 8
- 238000003825 pressing Methods 0.000 description 8
- 239000002356 single layer Substances 0.000 description 8
- 229910052782 aluminium Inorganic materials 0.000 description 6
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 6
- 238000005219 brazing Methods 0.000 description 6
- 239000002390 adhesive tape Substances 0.000 description 5
- 239000006260 foam Substances 0.000 description 5
- 239000002344 surface layer Substances 0.000 description 5
- 239000000758 substrate Substances 0.000 description 4
- 239000006061 abrasive grain Substances 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- 238000000137 annealing Methods 0.000 description 2
- 239000010953 base metal Substances 0.000 description 2
- 238000010288 cold spraying Methods 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 238000007731 hot pressing Methods 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 239000007769 metal material Substances 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 230000035484 reaction time Effects 0.000 description 2
- 238000005096 rolling process Methods 0.000 description 2
- 239000007790 solid phase Substances 0.000 description 2
- 238000002490 spark plasma sintering Methods 0.000 description 2
- 230000003685 thermal hair damage Effects 0.000 description 2
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 2
- 239000010937 tungsten Substances 0.000 description 2
- 239000002585 base Substances 0.000 description 1
- 238000010923 batch production Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000007664 blowing Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- 230000008595 infiltration Effects 0.000 description 1
- 238000001764 infiltration Methods 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 239000000155 melt Substances 0.000 description 1
- 238000004377 microelectronic Methods 0.000 description 1
- 230000008520 organization Effects 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 238000009715 pressure infiltration Methods 0.000 description 1
- 238000009736 wetting Methods 0.000 description 1
- 238000004857 zone melting Methods 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F7/00—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression
- B22F7/02—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression of composite layers
- B22F7/04—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression of composite layers with one or more layers not made from powder, e.g. made from solid metal
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F1/00—Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
- B22F1/06—Metallic powder characterised by the shape of the particles
- B22F1/065—Spherical particles
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F3/00—Manufacture of workpieces or articles from metallic powder characterised by the manner of compacting or sintering; Apparatus specially adapted therefor ; Presses and furnaces
- B22F3/10—Sintering only
- B22F3/105—Sintering only by using electric current other than for infrared radiant energy, laser radiation or plasma ; by ultrasonic bonding
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F3/00—Manufacture of workpieces or articles from metallic powder characterised by the manner of compacting or sintering; Apparatus specially adapted therefor ; Presses and furnaces
- B22F3/10—Sintering only
- B22F3/105—Sintering only by using electric current other than for infrared radiant energy, laser radiation or plasma ; by ultrasonic bonding
- B22F2003/1051—Sintering only by using electric current other than for infrared radiant energy, laser radiation or plasma ; by ultrasonic bonding by electric discharge
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Mechanical Engineering (AREA)
- Composite Materials (AREA)
- Materials Engineering (AREA)
- Physics & Mathematics (AREA)
- Optics & Photonics (AREA)
- Nanotechnology (AREA)
- Powder Metallurgy (AREA)
- Polishing Bodies And Polishing Tools (AREA)
- Cooling Or The Like Of Semiconductors Or Solid State Devices (AREA)
Abstract
A preparation method of a lamellar diamond metal-based composite material with high thermal conductivity and high surface finish relates to a preparation method of a diamond metal-based composite material. In order to solve the problem that the existing high-heat-conductivity lamellar diamond metal matrix composite is difficult to process. According to the invention, the arrangement direction of the monocrystalline diamond particles is regulated and controlled through the layering process, so that a good surface state is provided for subsequent precise grinding and polishing, and higher surface finish can be achieved. The upper and lower surfaces of the obtained diamond metal matrix composite are metal layers with specific thickness, so that the diamond metal matrix composite is easy to process, and provides convenience for subsequent processing, forming, precise grinding, electroplating and welding. And the overall heat conductivity of the obtained diamond metal matrix composite is higher due to the improvement of the process method, and the process is simple. The preparation period is short.
Description
Technical Field
The invention relates to a preparation method of a diamond metal matrix composite.
Background
With the continuous improvement of the power and the integration level of various devices, the traditional heat conduction and dissipation materials are difficult to meet the demands gradually, and the high heat conduction diamond/copper composite material is used as a new generation of heat management material, is widely applied to fields of integrated radiating fins, laser diode radiating substrates, solid-state laser heat sinks, CPU heat sinks or radiating fins, high-power electronic device substrates (such as IGBT (insulated gate bipolar transistor) substrates), LED and HB-LED radiating fins, radio frequency and microwave package heat sinks, microelectronic package heat sinks, high-heat-carrying electronic device heat management materials and the like, and can be upgraded to replace the traditional heat conduction materials, so that the temperature rise of the devices is greatly reduced.
The existing lamellar diamond metal-based composite material has the defects of high volume fraction of diamond and large particle size, so that the need of processing monocrystalline diamond particles is unavoidable during processing. Because the single crystal diamond particles are extremely hard and copper is very soft, such materials cannot be tapped, ground, polished as conventional metallic materials. Not only is it difficult to achieve the surface finish of conventional metallic materials during grinding and polishing, but the thermal conductivity of the material is lost.
The existing lamellar diamond metal-based composite material with high thermal conductivity is easier to process due to the fact that copper is coated on the surface of the diamond metal-based composite material, and the diamond metal-based composite material is a metal layer without monocrystalline diamond particles, but the method requires two devices, namely air pressure infiltration equipment and plasma discharge sintering equipment, to finish preparation of raw materials, so that the method is unfavorable for development into a batch low-cost raw material preparation method. The patent CN112974809B melts the whole matrix metal or alloy, then flows around the single crystal diamond particles, uses a specific device to carry out air-entraining pressure to compound the matrix metal or alloy, and makes the diamond copper composite, then makes the surface of the diamond copper composite and the copper layer generate discharge micro-area melting and pressurizing force to combine together, the discharge of the method only occurs between the composite and the surface layer, and the surface finish of the composite prepared by the method is better than 0.8 μm, which can not meet the requirement. If the surface finish of the prepared composite material can be improved, the subsequent grinding and polishing are facilitated, so that development of a preparation method capable of maintaining the high thermal conductivity of the lamellar diamond metal-based composite material and maintaining the high surface finish of the lamellar diamond metal-based composite material is needed.
Disclosure of Invention
The invention provides a method for preparing a high-heat-conductivity high-surface-finish lamellar diamond metal matrix composite in single equipment, which aims to solve the problem that the existing high-heat-conductivity lamellar diamond metal matrix composite is difficult to process. The surface finish of the prepared flaky diamond metal-based composite is 0.012 μm to 0.04 μm.
The preparation method of the high-heat conductivity high-surface-finish lamellar diamond metal matrix composite material comprises the following steps:
1. screening monocrystalline diamond particles, sequentially carrying out acid washing, alkali washing and absolute ethyl alcohol washing, and drying;
2. uniformly plating a metal coating with the thickness of 10-100 nanometers on the surface of the monocrystalline diamond particles, wherein the surface roughness of the metal coating is 1-10 nanometers;
3. paving a metal foil on the bottom of the die;
4. paving metal powder on the metal foil;
5. spreading monocrystalline diamond particles on the metal powder, and adjusting the arrangement of the monocrystalline diamond particles under a split microscope in the spreading process to enable one (100) crystal face of the monocrystalline diamond particles to face upwards and the inclination angle of the (100) crystal face relative to the metal foil to be 0-15 degrees; gaps between adjacent single crystal diamond particles do not exceed 50 μm, while no stacking of particles occurs;
6. Filling metal powder in the gaps of the monocrystalline diamond particles until the metal powder is level with the highest point of the monocrystalline diamond particles;
7. spreading metal foils which are the same as those in the third step on the surfaces of the monocrystalline diamond particles and the metal powder;
8. placing the mold in a plasma discharge sintering device;
9. vacuumizing the plasma discharge sintering equipment, heating to 100-200 ℃ below the melting point of the metal foil at the speed of 50-60K/min, and preserving heat for 10-60 min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide;
10. then heating the plasma discharge sintering equipment to 20-50 ℃ below the melting point of the matrix metal at the speed of 10-20K/min, applying the pressure of 10-50 MPa after reaching the temperature, and carrying out heat preservation and pressure maintaining for 10-60 min to realize pressurized compounding;
11. and cooling the plasma discharge sintering equipment to room temperature, releasing pressure, discharging vacuum and demoulding.
The principle and beneficial effects of the invention are as follows:
1. the invention provides a method for preparing a high-heat-conductivity lamellar diamond metal-based composite material in single equipment, wherein the upper surface and the lower surface of the obtained diamond metal-based composite material are metal layers with specific thickness, so that the diamond metal-based composite material is easy to process, and provides convenience for subsequent processing, forming, precise grinding, electroplating and welding. And the overall heat conductivity of the obtained diamond metal matrix composite is higher due to the improvement of the process method, and the process is simple.
2. The invention adopts the spark plasma sintering method to make the monocrystal diamond particles plated with the metal film form metallurgical bonding with the metal powder and the metal foil, the reaction time is short, the organization structure of the interface layer can be regulated and controlled, the heat damage of the monocrystal diamond particles is small, and the invention can realize the regulation and control of the arrangement direction of the monocrystal diamond particles.
3. The invention has the advantages of short preparation period, simple process flow, and suitability for mass production, and can be completed in 3 hours from die filling to die stripping.
4. The invention can realize finer regulation and control on the heat conductivity and the thermal expansion coefficient of the whole material through regulation and control on the volume fraction of the diamond and the components and the thickness of the same layer (surface layer).
5. According to the invention, the arrangement direction of the monocrystalline diamond particles is regulated and controlled through the layering process, so that a good surface state is provided for subsequent precise grinding and polishing, and higher surface finish can be achieved.
6. The invention can realize the preparation of the ultra-thin high heat conductivity diamond metal-based composite material with the thickness of 0.12mm, wherein the middle layer of the composite material is monocrystalline diamond particles, the upper layer and the lower layer are metal matrixes or alloys of the metal matrixes, the heat conductivity of the composite material is 700-1000W/(m.K), the surface finish is 0.012 mu m-0.04 mu m, and the thickness is 0.12-6 mm.
The difference of the application with respect to the method for coating copper on the surface of the diamond/copper composite material is that: (1) the equipment used is different. The preparation of the material can be completed by only using one plasma discharge sintering device, namely the integral material with the middle layer of diamond particles and the upper and lower surfaces of copper or copper alloy is obtained. CN112974809a requires two devices, pneumatic infiltration and plasma discharge sintering, to achieve copper coating on the surface of the diamond copper composite. (2) The compounding process of the materials is different. The application is that the whole discharge micro-area of the surface coating of the diamond particles and the surrounding copper powder is melted and formed into a sheet material by pressurizing. CN112974809a is a method of forming a diamond copper composite material by melting a matrix alloy integrally, flowing the matrix alloy around diamond particles, and compounding the matrix alloy by pressurizing the diamond particles with a specific apparatus, and then bonding the surface of the diamond copper composite material and the copper layer by applying a pressure and a discharge micro-area melting. I.e. the extent of the area in which the discharge occurs is different. The discharge of the present application occurs throughout the material. The discharge of CN112974809a only occurs between the composite and the surface layer. The metal powder is melted in the discharging micro-area and then pressurized and compounded, so that the whole preparation period is short, and the working time is saved. CN112974809a is prepared by melting a bulk metal, and the whole process is very long. (3) The properties of the prepared materials are different. The surface finish of the composite material prepared by CN112974809A is better than 0.8 mu m, the surface finish of the composite material prepared by the method is 0.012-0.04 mu m, and the surface finish is improved by one order of magnitude. The (100) crystal face of the diamond particles is parallel to the surface of the material in the layering process, so that the corner exposure of the diamond particles is reduced, and higher surface finish can be realized in subsequent processing. CN112974809a does not control the arrangement of diamond particles. The exposed edges and corners of the diamond particles can be embedded into the copper layer, which is equivalent to embedding hard particles in a soft substrate, and brings difficulty for subsequent grinding and polishing.
The difference of the present application with respect to the "near net shape forming method of ultra-thin thickness diamond/copper composite material", CN114147223a ", is: (1) the properties of the prepared materials are different. The thermal conductivity of the material prepared by CN114147223A is 434W/mK at the highest. The thermal conductivity of the material prepared by the method is 700-1000W/mK. (2) According to the method, the thickness and the surface roughness of the surface coating of the diamond particles are regulated, so that the discharge degree is regulated, and an ideal interface and good heat conductivity are obtained. CN114147223a defines the plating element as tungsten, but there is no limitation on the plating thickness and surface roughness. In addition to precise control of process parameters, surface roughness needs to be defined if a higher quality interface bond is to be achieved. The surface roughness affects the current distribution, temperature distribution, and tissue structure of the sample during plasma discharge. The thickness of the plating layer on the surface of the diamond particles is 10-100 nanometers, and the roughness of the plating layer surface is 1-10 nanometers. The method ensures uniform discharge in the material preparation process to a certain extent, ensures that current and temperature are nearly uniformly distributed in the composite material block in the plasma discharge process, reduces the temperature gradient and also reduces the non-uniformity of tissues and components. CN114147223a only limits the particle size of diamond particles and copper powder, and does not limit the thickness and surface roughness of the tungsten plating. The thermal conductivity of the flaky diamond metal-based composite material obtained by the application is 700-1000W/mK, and the thermal conductivity of the CN114147223A preparation material is 434W/mK at most. (example 1 of CN114147223 a), the lowest thermal conductivity of the present application is 266W/mK higher than the highest thermal conductivity of CN114147223 a. After the heat conducting performance of the material prepared by the method is improved, the application range of the material is enlarged, mass production is easier to realize, and the heat dissipation effect of the prepared heat sink device is better. (3) The arrangement of the diamond particles is regulated and controlled. CN114147223a does not regulate the arrangement of diamond particles. The (100) crystal face of the diamond particles is parallel to the surface of the material in the layering process, so that the corner exposure of the diamond particles is reduced, and higher surface finish can be realized in subsequent processing.
The differences of the present application with respect to "a metal-based diamond product and a preparation method thereof, CN115365505a" are: (1) the material is prepared by the hot press sintering method, CN115365505A is different in preparation process, and the material preform is densified by applying pressure at high temperature without discharge process. The plasma discharge sintering method is used for preparing the material, and the discharge micro-area melting and pressurizing of the material preform are carried out in a vacuum environment, so that the method is simpler and more convenient to implement. (2) The arrangement of the diamond particles is regulated and controlled, and CN115365505A does not regulate and control the arrangement of the diamond particles. The (100) crystal face of the diamond particles is parallel to the surface of the material in the layering process, so that the corner exposure of the diamond particles is reduced, and higher surface finish can be realized in subsequent processing. The subsequent grinding and polishing of the material is performed on the metal matrix, and the grinding and polishing of the material by CN115365505A is performed on the basis of coexistence of the outcrop of diamond particles and two phases of the metal matrix, so that the grinding and polishing difficulty of CN115365505A is higher. CN115365505a example 1 "the diamond is selected from 12/14 mesh uncoated diamond", mesh number and size of the screen corresponds to 12 mesh: 1397 μm,14 mesh: 1165 μm. I.e. diamond particle sizes exceeding 1.1mm. After a series of steps the "thickness of the diamond article was reduced from 3.25mm to 1mm" indicated that the corners or edges of the diamond particles were worn away. And the surface of the resulting material should be composed of diamond particles and metal. The present application does not destroy the diamond particles. And the upper and lower surfaces of the material obtained in the application are homogeneous surfaces. Only the metal matrix is provided, and no diamond particles are exposed, which brings great convenience for subsequent electroplating and the like. (3) CN115365505a example 1 "the outer matrix is selected from copper flakes having a thickness of 1mm, the inner matrix is selected from silver-based alloys having a thickness of 0.5mm, and the diamond is selected from 12/14 mesh uncoated diamond. Since diamond is non-wetting with copper and silver, the interface layer of diamond particles with the surrounding matrix is not an interface layer of carbide. The magnetron sputtering method is used for uniformly plating the metal coating with the thickness of 50-100 nanometers on the surface of the diamond particles, the surface roughness of the coating is 1-10 nanometers, and in the subsequent plasma discharge sintering process, the metal coating reacts with the diamond particles to generate metal carbide, so that the diamond particles and the boundary layer of the surrounding matrix are mutually reacted to generate the carbide boundary layer, and the binding force is stronger.
Compared with a single-layer diamond abrasive particle orderly arrangement brazing method for template-free furnace brazing, the difference of CN113524058B is that: (1) the compounding process of the materials is different. CN113524058B 'putting the above obtained matrix to be welded with uniformly arranged diamonds into a vacuum annealing furnace for brazing, taking out the sample to obtain a brazing tool product with uniformly and densely arranged diamonds', and controlling the air pressure in the vacuum annealing furnace to be 5×10 during brazing -3 The brazing temperature is 900 or 920 ℃ below Pa, and the heat preservation time is 5 min. CN113524058B has no discharge process. The method adopts a plasma discharge sintering method to prepare the material, and the material preform is subjected to discharge micro-zone melting and pressurizing in a vacuum environment. The metal powder is melted in the discharging microcell, pressurized and compounded, so that the temperature is low, the time is short, and the thermal damage to diamond particles is small. (2) The regulation and control requirements on the arrangement of diamond particles are different. CN113524058B sequentially arranging abrasive grains, firstly cutting an appropriate amount of adhesive tape, sticking it on the lower part of screen, then spreading a certain amount of diamond abrasive grains on the area with adhesive tape on the lower part of screen, dispersing the stacked diamond grains with brush, then blowing off the diamond abrasive grains on the surface layer of adhesive tape which is not stuck by adhesive tape with compressed air, finally Slowly removing the arranged adhesive tape from the screen. The whole process does not regulate that a certain crystal plane of the diamond particles is parallel to the surface, but only ensures that the diamond particles are not stacked. The arrangement of diamond particles is regulated and controlled in the layering process, so that the (100) crystal faces of the diamond particles are parallel to the upper surface and the lower surface of the integral material; ". The (100) crystal face of the diamond particles is parallel to the upper surface and the lower surface of the integral material, so that the corner outcrop of the diamond particles is reduced, and higher surface finish can be realized in subsequent processing. (3) The performance requirements of the prepared materials are different. CN113524058B is to obtain a composite material with high hardness, high strength and good wear resistance, and the purpose of the present application is to obtain a composite material with high thermal conductivity. (4) The interface bonding state between the diamond particles and the matrix is different. CN113524058B does not have a step of regulating the interface, nor does the diamond particle surface undergo a plating treatment. If the base metal is a metal such as aluminum or iron that reacts with diamond to form carbide, the interface bond will be strong, and if the base metal is a metal such as copper or silver that does not wet with diamond, the interface bond will be very weak. The scheme adopted by the application is that firstly, the temperature is raised to 100-200 ℃ below the melting point of the matrix metal at the speed of 50-60K/min, and the temperature is kept for 10-60 min, so that interface regulation and control are carried out; heating to 20-50 ℃ below the melting point of the matrix metal at the speed of 10-20K/min, then applying the pressure of 10-50 MPa, and preserving heat and pressure for 10-60 min to realize pressurized compounding; heating to 100-200 ℃ below the melting point of the metal foil at the speed of 50-60K/min, and preserving heat for 10-60 min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide; then heating to 20-50 ℃ below the melting point of the matrix metal at a speed of 10-20K/min, applying pressure of 10-50 MPa after reaching the temperature, and preserving heat and pressure for 10-60 min to realize pressurized compounding; by controlling the interface layer of the diamond particles and the metal matrix, a higher thermal conductivity can be achieved.
Compared with the diamond layer copper-paved-base high-heat-conductivity composite material and the preparation method thereof, the difference of CN109808258A is that: (1) the compounding process of the materials is different. CN109808258A was prepared by upsetting, welding, hot-pressing, without the process of discharge sintering. The whole process is carried out at 200 ℃ below the melting point. The metal powder is melted in the discharging micro-area and then pressurized and compounded, so that the whole preparation process has few procedures, short period and labor hour saving. According to the technical scheme, the metal foil, the diamond particles and the metal foil are manually assembled; the preparation is then completed in a plasma discharge sintering apparatus. The technical proposal of CN109808258A is that a metal foil, a copper net or foam copper, diamond particles and a metal foil are subjected to cold press assembly; then carrying out ultrasonic rolling solid phase welding on the cold-pressed assembled material; and then performing hot-press diffusion welding under a vacuum state. The whole working procedures are multiple, the period is long, and the working time is long. (2) CN109808258A does not give the surface finish of the prepared material. CN109808258A describes: the diamond particles are uniformly dispersed on the copper net or the copper foam, the mesh number of the copper net is 35-150 meshes, according to a mesh size comparison table, the mesh number of the copper net is 0.425mm, the mesh number of the copper net is 0.106mm, and the diamond particles are simply dispersed on the copper net or the copper foam, and no requirement is made on the direction of the diamond particles, so that the diamond particles are likely to be exposed in the final obtained material because the edges or the tips of the diamond particles are propped against the copper foils at the upper layer and the lower layer, and even in the subsequent pressurizing process. Severely affecting the surface quality of the material. The diamond particles with the metal coating are paved on the surface of a metal sheet; the arrangement of the diamond particles is regulated and controlled in the layering process, so that the (100) crystal faces of the diamond particles are parallel to the upper surface and the lower surface of the integral material, and the (100) crystal faces of the diamond particles are parallel to the surface of the material in the layering process, so that the exposure of the edges and corners of the diamond particles is reduced, and higher surface finish can be realized in subsequent processing. (3) The interface bonding state between the diamond particles and the matrix is different. CN109808258A does not give the thermal conductivity of the prepared material. The diamond particle of claim 5 of CN109808258A is coated with a thin metal layer, having a thickness of between 1 and 20 μm, in embodiments 15 μm and 16 μm, by magnetron sputtering or cold spraying. Sequentially placing a metal foil, a copper mesh or foam copper, diamond particles and a metal foil in claim 6 to complete cold press assembly of the material; carrying out ultrasonic rolling solid-phase welding on the cold-pressed assembled material; and (3) performing hot-pressing diffusion welding under a vacuum state to finish the preparation of the diamond layer copper-paving-based high-heat-conductivity composite material without the steps and the processes of interface regulation. At present, the cold spraying cannot uniformly coat the surface of the granular powder material, but can only uniformly coat the surface of the block material. The application adopts a magnetron sputtering method to uniformly plate a metal coating with the thickness of 50-100 nanometers on the surface of diamond particles, and the roughness of the surface of the coating is 1-10 nanometers. Simultaneously heating to 100-200 ℃ below the melting point of the metal foil at the speed of 50-60K/min and preserving heat for 10-60 min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide; then heating to 20-50 ℃ below the melting point of the matrix metal at a speed of 10-20K/min, applying pressure of 10-50 MPa after reaching the temperature, and performing heat preservation and pressure maintaining for 10-60 min to realize the technical scheme of pressurized compounding, so that the interface layer of the diamond particles and the metal matrix (the metal coating on the diamond surface reacts with the diamond particles to generate metal carbide, and the metal powder reacts with the diamond particles to generate metal carbide) can be controlled to obtain higher heat conductivity. The thickness of the diamond particle surface coating is different from that of CN109808258A by more than 1 order of magnitude, and the interface thermal resistance can be increased by excessively thick interface layer, so that the thermal conductivity of the material is reduced. (4) The diamond composite material is single-layer diamond particles, and thermal short circuit is easier to realize in principle, namely, interface thermal resistance among multiple layers does not exist, so that the overall thermal conductivity of the material can be greatly improved. CN109808258A is a multilayer diamond particle. Copper mesh or copper foam can remain in the matrix, introducing new interfaces, reducing the thermal conductivity of the copper matrix.
Drawings
FIG. 1 is a photograph showing a cross section of a flaky diamond metal-based composite of example 1, in which a is one (100) plane of single crystal diamond particles;
FIG. 2 is a surface morphology of single crystal diamond particles of the flaky diamond metal-based composite of example 1;
fig. 3 is a surface morphology of single crystal diamond particles of the flaky diamond metal-based composite of example 2.
Detailed Description
The technical scheme of the invention is not limited to the specific embodiments listed below, and also comprises any reasonable combination of the specific embodiments.
The first embodiment is as follows: the preparation method of the lamellar diamond metal matrix composite with high thermal conductivity and high surface finish of the embodiment comprises the following steps:
1. screening monocrystalline diamond particles, sequentially carrying out acid washing, alkali washing and absolute ethyl alcohol washing, and drying;
2. uniformly plating a metal coating with the thickness of 10-100 nanometers on the surface of the monocrystalline diamond particles, wherein the surface roughness of the metal coating is 1-10 nanometers;
3. paving a metal foil on the bottom of the die;
4. paving metal powder on the metal foil;
5. spreading monocrystalline diamond particles on the metal powder, and adjusting the arrangement of the monocrystalline diamond particles under a split microscope in the spreading process to enable one (100) crystal face of the monocrystalline diamond particles to face upwards and the inclination angle of the (100) crystal face relative to the metal foil to be 0-15 degrees; gaps between adjacent single crystal diamond particles do not exceed 50 μm, while no stacking of particles occurs;
6. Filling metal powder in the gaps of the monocrystalline diamond particles until the metal powder is level with the highest point of the monocrystalline diamond particles;
7. spreading metal foils which are the same as those in the third step on the surfaces of the monocrystalline diamond particles and the metal powder;
8. placing the mold in a plasma discharge sintering device;
9. vacuumizing the plasma discharge sintering equipment, heating to 100-200 ℃ below the melting point of the metal foil at the speed of 50-60K/min, and preserving heat for 10-60 min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide;
10. then heating the plasma discharge sintering equipment to 20-50 ℃ below the melting point of the matrix metal at the speed of 10-20K/min, applying the pressure of 10-50 MPa after reaching the temperature, and carrying out heat preservation and pressure maintaining for 10-60 min to realize pressurized compounding;
11. and cooling the plasma discharge sintering equipment to room temperature, releasing pressure, discharging vacuum and demoulding.
1. The embodiment provides a method for preparing a high-heat-conductivity lamellar diamond metal-based composite material in single equipment, wherein the upper surface and the lower surface of the obtained diamond metal-based composite material are metal layers with specific thickness, the diamond metal-based composite material is easy to process, and convenience is provided for subsequent processing, forming, precise grinding, electroplating and welding. And the overall heat conductivity of the obtained diamond metal matrix composite is higher due to the improvement of the process method, and the process is simple.
2. The method adopts a spark plasma sintering method to form metallurgical bonding between the monocrystalline diamond particles coated with the metal film, the metal powder and the metal foil, the reaction time is short, the structure of the interface layer can be regulated and controlled, the thermal damage of the monocrystalline diamond particles is small, and the method can realize the regulation and control of the arrangement direction of the monocrystalline diamond particles.
3. The preparation period of the embodiment is short, the process flow is simple, and the process can be completed from die filling to die stripping for 3 hours, so that the method is suitable for batch production.
4. The embodiment can realize finer regulation and control on the heat conductivity and the thermal expansion coefficient of the whole material through regulation and control on the volume fraction of the diamond and the components and the thickness of the same layer (surface layer).
5. According to the method, the arrangement direction of the monocrystalline diamond particles is regulated and controlled through the layering process, so that a good surface state is provided for subsequent precise grinding and polishing, and higher surface finish can be achieved.
6. The preparation of the ultra-thin high-heat-conductivity diamond metal-based composite material with the thickness of 0.12mm can be realized, the middle layer of the composite material is monocrystalline diamond particles, the upper layer and the lower layer are metal matrixes or alloys of the metal matrixes, the heat conductivity of the composite material is 700-1000W/(m.K), the surface smoothness is 0.012 mu m-0.04 mu m, and the thickness is 0.12-6 mm.
The second embodiment is as follows: the first difference between this embodiment and the specific embodiment is that: the grain size of the single crystal diamond in the step one is 100-1200 mu m.
And a third specific embodiment: this embodiment differs from the first or second embodiment in that: and in the second step, the metal coating is W, cr, mo, ti or Zr.
The specific embodiment IV is as follows: this embodiment differs from one of the first to third embodiments in that: and step two, preparing the metal coating by adopting a magnetron sputtering process, wherein the temperature is 300-400 ℃, the current is 0.5-1.5A, and the obtained metal coating is in a polycrystalline state.
Fifth embodiment: this embodiment differs from one to four embodiments in that: and step three, the thickness of the metal foil is 0.01-3 mm.
Specific embodiment six: this embodiment differs from one of the first to fifth embodiments in that: and step three, the metal foil is made of copper, copper alloy, aluminum alloy, silver or silver alloy.
Seventh embodiment: this embodiment differs from one of the first to sixth embodiments in that: the metal powder is one or more of Cu powder, al powder, ag powder, ti powder, cr powder, B powder, si powder, zr powder, W powder and Mo powder; the diameter of the metal powder is not more than 100 mu m, and the shape of the metal powder is spherical.
Eighth embodiment: this embodiment differs from one of the first to seventh embodiments in that: the metal powder is one or more of Cu powder, al powder, ag powder, ti powder, cr powder, B powder, si powder, zr powder, W powder and Mo powder; the diameter of the metal powder is not more than 100 mu m, and the shape of the metal powder is spherical.
Detailed description nine: this embodiment differs from one to eight of the embodiments in that: and step nine, vacuumizing the plasma discharge sintering equipment to a vacuum degree of 10-100 Pa.
Detailed description ten: this embodiment differs from one of the embodiments one to nine in that: in the eleventh step, the cooling speed is 20-40K/min when cooling to room temperature.
Example 1
The preparation method of the lamellar diamond metal matrix composite with high thermal conductivity and high surface finish comprises the following steps:
1. screening monocrystalline diamond particles, sequentially carrying out acid washing, alkali washing and absolute ethyl alcohol washing, and drying;
the grain size of the single crystal diamond is 700 mu m;
2. uniformly plating a metal coating with the thickness of 100 nanometers on the surface of the monocrystalline diamond particles, wherein the surface roughness of the metal coating is 10 nanometers;
The metal coating is made of Ti;
the metal coating is prepared by a magnetron sputtering process, the temperature is 300 ℃, the current is 0.5A, and the obtained metal coating is in a polycrystalline state;
3. paving a metal foil on the bottom of the die;
the thickness of the metal foil is 0.2mm;
the metal foil is made of pure copper;
4. paving metal powder on the metal foil;
the metal powder is Cu powder; the diameter of the metal powder is 15 mu m, and the shape of the metal powder is spherical;
5. spreading monocrystalline diamond particles on the metal powder, and adjusting the arrangement of the monocrystalline diamond particles under a split microscope in the spreading process to enable one (100) crystal face of the monocrystalline diamond particles to face upwards and the inclination angle of the (100) crystal face relative to the metal foil to be 0-15 degrees; gaps between adjacent single crystal diamond particles do not exceed 50 μm, while no stacking of particles occurs;
6. filling metal powder in the gaps of the monocrystalline diamond particles until the metal powder is level with the highest point of the monocrystalline diamond particles;
the metal powder is Cu powder; the diameter of the metal powder is 15 mu m, and the shape of the metal powder is spherical;
7. spreading metal foils which are the same as those in the third step on the surfaces of the monocrystalline diamond particles and the metal powder;
8. Placing the mold in a plasma discharge sintering device;
9. vacuumizing the plasma discharge sintering equipment, heating to 100 ℃ below the melting point of the metal foil at the speed of 50K/min, and preserving heat for 10min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide;
step nine, vacuumizing plasma discharge sintering equipment until the vacuum degree is 10Pa;
10. then heating plasma discharge sintering equipment to 20 ℃ below the melting point of the matrix metal at a speed of 20K/min, applying pressure of 10MPa after reaching the temperature, and preserving heat and pressure for 20min to realize pressurized compounding;
11. cooling the plasma discharge sintering equipment to room temperature, releasing pressure, discharging vacuum and demoulding;
in the eleventh step, the cooling speed is 20K/min when the temperature is reduced to the room temperature.
The thermal conductivity of the flaky diamond copper-based composite obtained by the method of example 1 was 900W/mK. Preparation of a single-layer diamond copper-based composite material with high thermal conductivity by controlling the arrangement of the single-crystal diamond particles of the intermediate layer and the interface bonding of the single-crystal diamond particles and the metal matrix, fig. 1 is a photograph of a cross section of a flaky diamond metal-based composite material in example 1, in which a is a (100) crystal plane of the single-crystal diamond particles; FIG. 2 is a surface morphology of single crystal diamond particles of the flaky diamond metal-based composite of example 1; the thickness of the composite material is 1.1mm, the thickness of the diamond layer is 0.7mm, and the sum of the thicknesses of the upper copper layer and the lower copper layer is 0.4mm.
Example 2
The preparation method of the lamellar diamond metal matrix composite with high thermal conductivity and high surface finish comprises the following steps:
1. screening monocrystalline diamond particles, sequentially carrying out acid washing, alkali washing and absolute ethyl alcohol washing, and drying;
the grain size of the single crystal diamond is 100 mu m;
2. uniformly plating a metal coating with the thickness of 50 nanometers on the surface of the monocrystalline diamond particles, wherein the surface roughness of the metal coating is 10 nanometers;
the metal coating is made of W;
the metal coating is prepared by a magnetron sputtering process, the temperature is 400 ℃, the current is 1.5A, and the obtained metal coating is in a polycrystalline state;
3. paving a metal foil on the bottom of the die;
the thickness of the metal foil is 0.01mm;
the metal foil is made of pure copper;
4. paving metal powder on the metal foil;
the metal powder is Cu powder; the diameter of the metal powder is not more than 100 mu m, and the shape of the metal powder is spherical;
5. spreading monocrystalline diamond particles on the metal powder, and adjusting the arrangement of the monocrystalline diamond particles under a split microscope in the spreading process to enable one (100) crystal face of the monocrystalline diamond particles to face upwards and the inclination angle of the (100) crystal face relative to the metal foil to be 0-15 degrees; gaps between adjacent single crystal diamond particles do not exceed 50 μm, while no stacking of particles occurs;
6. Filling metal powder in the gaps of the monocrystalline diamond particles until the metal powder is level with the highest point of the monocrystalline diamond particles;
the metal powder is Cu powder; the diameter of the metal powder is not more than 100 mu m, and the shape of the metal powder is spherical;
7. spreading metal foils which are the same as those in the third step on the surfaces of the monocrystalline diamond particles and the metal powder;
8. placing the mold in a plasma discharge sintering device;
9. vacuumizing the plasma discharge sintering equipment, heating to 100 ℃ below the melting point of the metal foil at the speed of 50K/min, and preserving heat for 20min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide;
step nine, vacuumizing plasma discharge sintering equipment until the vacuum degree is 10Pa;
10. then heating the plasma discharge sintering equipment to 25 ℃ below the melting point of the matrix metal at the speed of 20K/min, applying the pressure of 15MPa after reaching the temperature, and carrying out heat preservation and pressure maintaining for 60min to realize pressurized compounding;
11. cooling the plasma discharge sintering equipment to room temperature, releasing pressure, discharging vacuum and demoulding;
In the eleventh step, the cooling speed is 20K/min when the temperature is reduced to the room temperature.
Fig. 3 is a surface morphology of single crystal diamond particles of the flaky diamond metal-based composite of example 2. The sheet-like diamond copper-based composite material obtained in example 2 had a thermal conductivity of 750W/mK. The single-layer diamond copper-based composite material with high thermal conductivity is obtained by controlling the arrangement of the single-crystal diamond particles of the intermediate layer and the interface combination of the single-crystal diamond particles and the metal matrix. The thickness of the composite material is 0.12mm, the thickness of the diamond layer is 0.1mm, the thickness of the upper copper layer and the lower copper layer is 0.01mm, and the surface finish is better than 0.012 mu m.
Example 3
The preparation method of the lamellar diamond metal matrix composite with high thermal conductivity and high surface finish comprises the following steps:
1. screening monocrystalline diamond particles, sequentially carrying out acid washing, alkali washing and absolute ethyl alcohol washing, and drying;
the grain size of the single crystal diamond is 425 mu m;
2. uniformly plating a metal coating with the thickness of 10 nanometers on the surface of the monocrystalline diamond particles, wherein the surface roughness of the metal coating is 1 nanometer;
the metal coating is made of Ti;
the metal coating is prepared by a magnetron sputtering process, the temperature is 320 ℃, the current is 0.7A, and the obtained metal coating is in a polycrystalline state;
3. Paving a metal foil on the bottom of the die;
the thickness of the metal foil is 3mm;
the metal foil is made of pure copper;
4. paving metal powder on the metal foil;
the metal powder is Ti powder; the diameter of the metal powder is not more than 30 mu m, and the shape of the metal powder is spherical;
5. spreading monocrystalline diamond particles on the metal powder, and adjusting the arrangement of the monocrystalline diamond particles under a split microscope in the spreading process to enable one (100) crystal face of the monocrystalline diamond particles to face upwards and the inclination angle of the (100) crystal face relative to the metal foil to be 0-15 degrees; gaps between adjacent single crystal diamond particles do not exceed 50 μm, while no stacking of particles occurs;
6. filling metal powder in the gaps of the monocrystalline diamond particles until the metal powder is level with the highest point of the monocrystalline diamond particles;
the metal powder is Ti powder; the diameter of the metal powder is not more than 30 mu m, and the shape of the metal powder is spherical;
7. spreading metal foils which are the same as those in the third step on the surfaces of the monocrystalline diamond particles and the metal powder;
8. placing the mold in a plasma discharge sintering device;
9. vacuumizing the plasma discharge sintering equipment, heating to 120 ℃ below the melting point of the metal foil at the speed of 55K/min, and preserving heat for 20min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide;
Step nine, vacuumizing plasma discharge sintering equipment until the vacuum degree is 100Pa;
10. then heating plasma discharge sintering equipment to 50 ℃ below the melting point of the matrix metal at the speed of 10K/min, applying pressure of 10MPa after reaching the temperature, and carrying out heat preservation and pressure maintaining for 60min to realize pressurized compounding;
11. cooling the plasma discharge sintering equipment to room temperature, releasing pressure, discharging vacuum and demoulding;
in the eleventh step, the cooling speed is 40K/min when the temperature is reduced to the room temperature.
The sheet-like diamond aluminum-based composite material obtained in example 4 had a thermal conductivity of 710W/mK, and a single-layer diamond copper-based composite material having a high thermal conductivity was obtained by controlling the arrangement of single-crystal diamond particles of the intermediate layer, and the interface bonding of the single-crystal diamond particles with the metal matrix. The thickness of the composite material is 0.2mm, the thickness of the diamond layer is 0.1mm, the thickness of the upper copper layer and the lower copper layer is 0.05mm, and the surface finish is better than 0.012 mu m.
Example 4
The preparation method of the lamellar diamond metal matrix composite with high thermal conductivity and high surface finish comprises the following steps:
1. screening monocrystalline diamond particles, sequentially carrying out acid washing, alkali washing and absolute ethyl alcohol washing, and drying;
The grain size of the single crystal diamond is 100 mu m;
2. uniformly plating a metal coating with the thickness of 50 nanometers on the surface of the monocrystalline diamond particles, wherein the surface roughness of the metal coating is 10 nanometers;
the metal coating is made of W;
the metal coating is prepared by a magnetron sputtering process, the temperature is 380 ℃, the current is 1.2A, and the obtained metal coating is in a polycrystalline state;
3. paving a metal foil on the bottom of the die;
the thickness of the metal foil is 0.05mm;
the metal foil is made of pure aluminum;
4. paving metal powder on the metal foil;
the metal powder is Al powder; the diameter of the metal powder is not more than 50 mu m, and the shape of the metal powder is spherical;
5. spreading monocrystalline diamond particles on the metal powder, and adjusting the arrangement of the monocrystalline diamond particles under a split microscope in the spreading process to enable one (100) crystal face of the monocrystalline diamond particles to face upwards and the inclination angle of the (100) crystal face relative to the metal foil to be 0-15 degrees; gaps between adjacent single crystal diamond particles do not exceed 50 μm, while no stacking of particles occurs;
6. filling metal powder in the gaps of the monocrystalline diamond particles until the metal powder is level with the highest point of the monocrystalline diamond particles;
The metal powder is Al powder; the diameter of the metal powder is not more than 50 mu m, and the shape of the metal powder is spherical;
7. spreading metal foils which are the same as those in the third step on the surfaces of the monocrystalline diamond particles and the metal powder;
8. placing the mold in a plasma discharge sintering device;
9. vacuumizing the plasma discharge sintering equipment, heating to 100 ℃ below the melting point of the metal foil at the speed of 60K/min, and preserving heat for 60min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide;
step nine, vacuumizing plasma discharge sintering equipment until the vacuum degree is 50Pa;
10. then heating the plasma discharge sintering equipment to 30 ℃ below the melting point of the matrix metal at a speed of 15K/min, applying pressure of 25MPa after reaching the temperature, and carrying out heat preservation and pressure maintaining for 30min to realize pressurized compounding;
11. cooling the plasma discharge sintering equipment to room temperature, releasing pressure, discharging vacuum and demoulding;
in the eleventh step, the cooling speed is 30K/min when the temperature is reduced to the room temperature.
The thermal conductivity of the flaky diamond aluminum-based composite obtained in example 4 was 710W/mK. The single-layer diamond copper-based composite material with high heat conductivity is obtained by controlling the arrangement of the single-crystal diamond particles in the middle layer and the interface combination of the single-crystal diamond particles and the metal matrix, the thickness of the composite material is 0.2mm, the thickness of the diamond layer is 0.1mm, the thicknesses of the upper copper layer and the lower copper layer are both 0.05mm, and the surface finish is better than 0.012 mu m.
Example 5
The preparation method of the lamellar diamond metal matrix composite with high thermal conductivity and high surface finish comprises the following steps:
1. screening monocrystalline diamond particles, sequentially carrying out acid washing, alkali washing and absolute ethyl alcohol washing, and drying;
the grain size of the single crystal diamond is 700 mu m;
2. uniformly plating a metal coating with the thickness of 30 nanometers on the surface of the monocrystalline diamond particles, wherein the surface roughness of the metal coating is 10 nanometers;
the metal coating is made of W;
the metal coating is prepared by a magnetron sputtering process, the temperature is 350 ℃, the current is 1A, and the obtained metal coating is in a polycrystalline state;
3. paving a metal foil on the bottom of the die;
the thickness of the metal foil is 3mm;
the metal foil is made of pure aluminum;
4. paving metal powder on the metal foil;
the metal powder is Al powder; the diameter of the metal powder is not more than 100 mu m, and the shape of the metal powder is spherical;
5. spreading monocrystalline diamond particles on the metal powder, and adjusting the arrangement of the monocrystalline diamond particles under a split microscope in the spreading process to enable one (100) crystal face of the monocrystalline diamond particles to face upwards and the inclination angle of the (100) crystal face relative to the metal foil to be 0-15 degrees; gaps between adjacent single crystal diamond particles do not exceed 50 μm, while no stacking of particles occurs;
6. Filling metal powder in the gaps of the monocrystalline diamond particles until the metal powder is level with the highest point of the monocrystalline diamond particles;
the metal powder is Al powder; the diameter of the metal powder is not more than 100 mu m, and the shape of the metal powder is spherical;
7. spreading metal foils which are the same as those in the third step on the surfaces of the monocrystalline diamond particles and the metal powder;
8. placing the mold in a plasma discharge sintering device;
9. vacuumizing the plasma discharge sintering equipment, heating to 200 ℃ below the melting point of the metal foil at the speed of 58K/min, and preserving heat for 30min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide;
step nine, vacuumizing plasma discharge sintering equipment until the vacuum degree is 30Pa;
10. then heating plasma discharge sintering equipment to 40 ℃ below the melting point of the matrix metal at the speed of 18K/min, applying pressure of 50MPa after reaching the temperature, and carrying out heat preservation and pressure maintaining for 10min to realize pressurized compounding;
11. cooling the plasma discharge sintering equipment to room temperature, releasing pressure, discharging vacuum and demoulding;
In the eleventh step, the cooling speed is 25K/min when the temperature is reduced to the room temperature.
The thermal conductivity of the flaky diamond aluminum-based composite obtained in example 5 was 850W/mK. The single-layer diamond copper-based composite material with high heat conductivity is obtained by controlling the arrangement of the single-crystal diamond particles in the middle layer and the interface combination of the single-crystal diamond particles and the metal matrix, the thickness of the composite material is 6.7mm, the thickness of the diamond layer is 0.7mm, the thicknesses of the upper copper layer and the lower copper layer are 3mm, and the surface finish is better than 0.012 mu m.
Example 6
The preparation method of the lamellar diamond metal matrix composite with high thermal conductivity and high surface finish comprises the following steps:
1. screening monocrystalline diamond particles, sequentially carrying out acid washing, alkali washing and absolute ethyl alcohol washing, and drying;
the grain size of the single crystal diamond is 100 mu m;
2. uniformly plating a metal coating with the thickness of 80 nanometers on the surface of the monocrystalline diamond particles, wherein the surface roughness of the metal coating is 10 nanometers;
the metal coating is made of Zr;
the metal coating is prepared by a magnetron sputtering process, the temperature is 300 ℃, the current is 1.2A, and the obtained metal coating is in a polycrystalline state;
3. paving a metal foil on the bottom of the die;
The thickness of the metal foil is 0.02mm;
the metal foil is made of pure silver;
4. paving metal powder on the metal foil;
the metal powder is Ag powder; the diameter of the metal powder is not more than 20 mu m, and the shape of the metal powder is spherical;
5. spreading monocrystalline diamond particles on the metal powder, and adjusting the arrangement of the monocrystalline diamond particles under a split microscope in the spreading process to enable one (100) crystal face of the monocrystalline diamond particles to face upwards and the inclination angle of the (100) crystal face relative to the metal foil to be 0-15 degrees; gaps between adjacent single crystal diamond particles do not exceed 50 μm, while no stacking of particles occurs;
6. filling metal powder in the gaps of the monocrystalline diamond particles until the metal powder is level with the highest point of the monocrystalline diamond particles;
the metal powder is Ag powder; the diameter of the metal powder is not more than 100 mu m, and the shape of the metal powder is spherical;
7. spreading metal foils which are the same as those in the third step on the surfaces of the monocrystalline diamond particles and the metal powder;
8. placing the mold in a plasma discharge sintering device;
9. vacuumizing the plasma discharge sintering equipment, heating to 100 ℃ below the melting point of the metal foil at the speed of 50K/min, and preserving heat for 20min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide;
Step nine, vacuumizing plasma discharge sintering equipment until the vacuum degree is 40Pa;
10. then heating the plasma discharge sintering equipment to 20 ℃ below the melting point of the matrix metal at a speed of 20K/min, applying pressure of 30MPa after reaching the temperature, and carrying out heat preservation and pressure maintaining for 20min to realize pressurized compounding;
11. cooling the plasma discharge sintering equipment to room temperature, releasing pressure, discharging vacuum and demoulding;
in the eleventh step, the cooling speed is 30K/min when the temperature is reduced to the room temperature.
The thermal conductivity of the flake-form diamond silver-based composite obtained in example 6 was 890W/mK. The single-layer diamond copper-based composite material with high heat conductivity is obtained by controlling the arrangement of the single-crystal diamond particles in the middle layer and the interface combination of the single-crystal diamond particles and the metal matrix, the thickness of the composite material is 0.14mm, the thickness of the diamond layer is 0.1mm, the thicknesses of the upper copper layer and the lower copper layer are both 0.02mm, and the surface finish is better than 0.012 mu m.
Claims (10)
1. A preparation method of a high-heat conductivity high-surface-finish lamellar diamond metal-based composite material is characterized by comprising the following steps of: the preparation method of the high-heat conductivity high-surface-finish lamellar diamond metal-based composite material comprises the following steps:
1. Screening monocrystalline diamond particles, sequentially carrying out acid washing, alkali washing and absolute ethyl alcohol washing, and drying;
2. uniformly plating a metal coating with the thickness of 10-100 nanometers on the surface of the monocrystalline diamond particles, wherein the surface roughness of the metal coating is 1-10 nanometers;
3. paving a metal foil on the bottom of the die;
4. paving metal powder on the metal foil;
5. spreading monocrystalline diamond particles on the metal powder, and adjusting the arrangement of the monocrystalline diamond particles under a split microscope in the spreading process to enable one (100) crystal face of the monocrystalline diamond particles to face upwards and the inclination angle of the (100) crystal face relative to the metal foil to be 0-15 degrees; gaps between adjacent single crystal diamond particles do not exceed 50 μm, while no stacking of particles occurs;
6. filling metal powder in the gaps of the monocrystalline diamond particles until the metal powder is level with the highest point of the monocrystalline diamond particles;
7. spreading metal foils which are the same as those in the third step on the surfaces of the monocrystalline diamond particles and the metal powder;
8. placing the mold in a plasma discharge sintering device;
9. vacuumizing the plasma discharge sintering equipment, heating to 100-200 ℃ below the melting point of the metal foil at the speed of 50-60K/min, and preserving heat for 10-60 min to enable the metal coating on the diamond surface to react with the monocrystalline diamond particles to generate metal carbide, and enabling the metal powder to react with the monocrystalline diamond particles to generate metal carbide;
10. Then heating the plasma discharge sintering equipment to 20-50 ℃ below the melting point of the matrix metal at the speed of 10-20K/min, applying the pressure of 10-50 MPa after reaching the temperature, and carrying out heat preservation and pressure maintaining for 10-60 min to realize pressurized compounding;
11. and cooling the plasma discharge sintering equipment to room temperature, releasing pressure, discharging vacuum and demoulding.
2. The method for preparing the high-thermal-conductivity high-surface-finish lamellar diamond metal-based composite material according to claim 1, wherein the method comprises the following steps of: the grain size of the single crystal diamond in the step one is 100-1200 mu m.
3. The method for preparing the high-thermal-conductivity high-surface-finish lamellar diamond metal-based composite material according to claim 1, wherein the method comprises the following steps of: and in the second step, the metal coating is W, cr, mo, ti or Zr.
4. The method for preparing the high-thermal-conductivity high-surface-finish lamellar diamond metal-based composite material according to claim 1, wherein the method comprises the following steps of: and step two, preparing the metal coating by adopting a magnetron sputtering process, wherein the temperature is 300-400 ℃, the current is 0.5-1.5A, and the obtained metal coating is in a polycrystalline state.
5. The method for preparing the high-thermal-conductivity high-surface-finish lamellar diamond metal-based composite material according to claim 1, wherein the method comprises the following steps of: and step three, the thickness of the metal foil is 0.01-3 mm.
6. The method for preparing the high-thermal-conductivity high-surface-finish lamellar diamond metal-based composite material according to claim 1, wherein the method comprises the following steps of: and step three, the metal foil is made of copper, copper alloy, aluminum alloy, silver or silver alloy.
7. The method for preparing the high-thermal-conductivity high-surface-finish lamellar diamond metal-based composite material according to claim 1, wherein the method comprises the following steps of: the metal powder is one or more of Cu powder, al powder, ag powder, ti powder, cr powder, B powder, si powder, zr powder, W powder and Mo powder; the diameter of the metal powder is not more than 100 mu m, and the shape of the metal powder is spherical.
8. The method for preparing the high-thermal-conductivity high-surface-finish lamellar diamond metal-based composite material according to claim 1, wherein the method comprises the following steps of: the metal powder is one or more of Cu powder, al powder, ag powder, ti powder, cr powder, B powder, si powder, zr powder, W powder and Mo powder; the diameter of the metal powder is not more than 100 mu m, and the shape of the metal powder is spherical.
9. The method for preparing the high-thermal-conductivity high-surface-finish lamellar diamond metal-based composite material according to claim 1, wherein the method comprises the following steps of: and step nine, vacuumizing the plasma discharge sintering equipment to a vacuum degree of 10-100 Pa.
10. The method for preparing the high-thermal-conductivity high-surface-finish lamellar diamond metal-based composite material according to claim 1, wherein the method comprises the following steps of: in the eleventh step, the cooling speed is 20-40K/min when cooling to room temperature.
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