CN116969764A - Method for preparing Diamond/SiC composite material by combining hot die pressing with CVI - Google Patents
Method for preparing Diamond/SiC composite material by combining hot die pressing with CVI Download PDFInfo
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- 239000010432 diamond Substances 0.000 title claims abstract description 163
- 229910003460 diamond Inorganic materials 0.000 title claims abstract description 162
- 239000002131 composite material Substances 0.000 title claims abstract description 63
- 238000000034 method Methods 0.000 title claims abstract description 47
- 238000007723 die pressing method Methods 0.000 title claims abstract description 14
- 239000000843 powder Substances 0.000 claims abstract description 49
- 238000000151 deposition Methods 0.000 claims abstract description 31
- 238000001764 infiltration Methods 0.000 claims abstract description 29
- 230000008595 infiltration Effects 0.000 claims abstract description 29
- 239000000126 substance Substances 0.000 claims abstract description 29
- 239000002245 particle Substances 0.000 claims abstract description 28
- 230000008021 deposition Effects 0.000 claims abstract description 23
- 239000011159 matrix material Substances 0.000 claims abstract description 16
- 229920002037 poly(vinyl butyral) polymer Polymers 0.000 claims abstract description 15
- 238000000498 ball milling Methods 0.000 claims abstract description 12
- 230000001680 brushing effect Effects 0.000 claims abstract description 8
- 239000000463 material Substances 0.000 claims abstract description 8
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 7
- 238000010438 heat treatment Methods 0.000 claims abstract description 5
- 238000003825 pressing Methods 0.000 claims abstract description 4
- 238000002156 mixing Methods 0.000 claims abstract description 3
- 229910000831 Steel Inorganic materials 0.000 claims description 36
- 239000010959 steel Substances 0.000 claims description 36
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 26
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 13
- 229910052786 argon Inorganic materials 0.000 claims description 13
- 230000006835 compression Effects 0.000 claims description 13
- 238000007906 compression Methods 0.000 claims description 13
- 239000001257 hydrogen Substances 0.000 claims description 13
- 229910052739 hydrogen Inorganic materials 0.000 claims description 13
- 239000007789 gas Substances 0.000 claims description 9
- 239000012159 carrier gas Substances 0.000 claims description 7
- 239000003085 diluting agent Substances 0.000 claims description 7
- 125000000118 dimethyl group Chemical group [H]C([H])([H])* 0.000 claims description 7
- 239000011812 mixed powder Substances 0.000 claims description 7
- -1 polytetrafluoroethylene Polymers 0.000 claims description 7
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 7
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 7
- 239000002243 precursor Substances 0.000 claims description 7
- 229920002545 silicone oil Polymers 0.000 claims description 7
- 238000003892 spreading Methods 0.000 claims description 7
- DWAWYEUJUWLESO-UHFFFAOYSA-N trichloromethylsilane Chemical compound [SiH3]C(Cl)(Cl)Cl DWAWYEUJUWLESO-UHFFFAOYSA-N 0.000 claims description 7
- 238000000465 moulding Methods 0.000 claims description 4
- 239000011248 coating agent Substances 0.000 claims description 3
- 238000000576 coating method Methods 0.000 claims description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 2
- 229910002804 graphite Inorganic materials 0.000 claims description 2
- 239000010439 graphite Substances 0.000 claims description 2
- 238000005266 casting Methods 0.000 abstract description 7
- 238000003475 lamination Methods 0.000 abstract description 2
- 239000011800 void material Substances 0.000 abstract description 2
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 66
- 229910010271 silicon carbide Inorganic materials 0.000 description 65
- 238000002360 preparation method Methods 0.000 description 9
- 239000000758 substrate Substances 0.000 description 9
- ZDHXKXAHOVTTAH-UHFFFAOYSA-N trichlorosilane Chemical compound Cl[SiH](Cl)Cl ZDHXKXAHOVTTAH-UHFFFAOYSA-N 0.000 description 7
- 239000005052 trichlorosilane Substances 0.000 description 7
- 238000010586 diagram Methods 0.000 description 4
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 3
- 229910052710 silicon Inorganic materials 0.000 description 3
- 239000010703 silicon Substances 0.000 description 3
- 238000004100 electronic packaging Methods 0.000 description 2
- 238000001513 hot isostatic pressing Methods 0.000 description 2
- 238000009776 industrial production Methods 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000005022 packaging material Substances 0.000 description 2
- 238000001878 scanning electron micrograph Methods 0.000 description 2
- 238000005245 sintering Methods 0.000 description 2
- 230000002411 adverse Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000011153 ceramic matrix composite Substances 0.000 description 1
- 238000005229 chemical vapour deposition Methods 0.000 description 1
- 238000000280 densification Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000005087 graphitization Methods 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 238000000626 liquid-phase infiltration Methods 0.000 description 1
- 238000004806 packaging method and process Methods 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000005475 siliconizing Methods 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 238000002490 spark plasma sintering Methods 0.000 description 1
- 238000010345 tape casting Methods 0.000 description 1
- 238000009827 uniform distribution Methods 0.000 description 1
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/515—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
- C04B35/56—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides
- C04B35/565—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide
- C04B35/573—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide obtained by reaction sintering or recrystallisation
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/42—Non metallic elements added as constituents or additives, e.g. sulfur, phosphor, selenium or tellurium
- C04B2235/422—Carbon
- C04B2235/427—Diamond
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/48—Organic compounds becoming part of a ceramic after heat treatment, e.g. carbonising phenol resins
- C04B2235/483—Si-containing organic compounds, e.g. silicone resins, (poly)silanes, (poly)siloxanes or (poly)silazanes
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Abstract
The invention particularly relates to a method for preparing a Diamond/SiC composite material by combining hot die pressing with CVI, which solves the technical problems of low heat conductivity, high porosity and high void size of the Diamond/SiC composite material caused by large grain size of Diamond and large heat resistance between cast laminations in a casting method. The method for preparing the Diamond/SiC composite material by combining hot die pressing with CVI comprises the following steps: step 1: mixing a plurality of diamond powder materials with different particle sizes and polyvinyl butyral, and performing ball milling to obtain powder materials; step 2: brushing a release agent on the inner surface of a die, flatly laying the powder obtained in the step 1, pouring the powder into the die, heating and preserving heat of the die, applying pressure to the die, and demolding to obtain a diamond preform after the die is cooled; step 3: and (3) fixing the Diamond preform prepared in the step (2), and putting the Diamond preform into a chemical vapor infiltration furnace to perform chemical vapor infiltration deposition on the SiC matrix to obtain the Diamond/SiC composite material so as to improve the thermal conductivity of the Diamond/SiC composite material.
Description
Technical Field
The invention particularly relates to a method for preparing a Diamond/SiC composite material by combining hot die pressing and CVI.
Background
The Diamond/SiC composite material has the advantages of high hardness, high wear resistance, low density, high heat conductivity, low thermal expansion coefficient, good high-temperature stability and the like, and is widely used for PDC wear-resistant materials, compression-resistant base felts, petroleum mechanical drill bits, reflector substrates and electronic packaging materials. And the Diamond/SiC composite material has the characteristics of high heat conductivity, low thermal expansibility, low density and the like, meets the characteristics of high integration level, high packaging density and high working frequency of the current electronic device chip, and can be used as a fourth-generation electronic packaging material.
The main methods for preparing the Diamond/SiC composite material at present are as follows: high temperature high pressure sintering (HPHT), reactive melt infiltration gas phase silicon (RMI), hot isostatic pressing sintering (HIP), reactive gas phase siliconizing (RVI), spark Plasma Sintering (SPS), and the like. The method has the advantages of high efficiency, higher density of the prepared Diamond/SiC composite material, high equipment requirement, difficulty in preparing Diamond/SiC plates with large-size complex structures, residual silicon in prepared samples, and the like. In addition, due to the high preparation temperature of HPHT, the Diamond is extremely easy to graphitize, and the mechanical property and the thermophysical property of the Diamond/SiC composite material are seriously affected. In summary, it is difficult to fully meet the use requirements of the products produced by these methods.
In order to solve the above-mentioned problems, a Diamond/SiC composite material was prepared by a casting-combined Chemical Vapor Infiltration (CVI) method for the first time in chinese patent CN103724014a, "a preparation method of a highly thermally conductive Diamond doped SiC ceramic", and literature "Yongsheng Liu and Chenghao Hu Microstructure and properties of Diamond/SiC composites prepared by tape-casting and chemical vapor infiltration process J. Firstly preparing Diamond slurry with different particle sizes (7-27 mu m) for casting experiments, then drying the cast substrate, placing the dried substrate in a CVI (chemical vapor deposition) deposition furnace to deposit a SiC matrix to obtain a Diamond/SiC sheet, and taking out the sheet to repeatedly cast and deposit on the surface of the sheet. Finally, a diamond/silicon carbide composite sample having a thickness of about 2mm was obtained.
The Chemical Vapor Infiltration (CVI) method has mild preparation conditions, and SiC generated by in-situ deposition has high purity, so that the problems of diamond graphitization, residual silicon and the like in other preparation methods are avoided. The Diamond/SiC composite material prepared is biphase of Diamond and silicon carbide, has no other impurities, and has uniform distribution in the Diamond/SiC composite material and good combination with matrix Diamond. In addition, CVI is used as a relatively mature process for preparing the ceramic matrix composite material, and can realize industrial production. However, in the casting combined CVI method, due to the limitation of the casting method, the grain size of the adopted Diamond micro powder cannot be too large, so that the improvement of the effective heat conductivity of Diamond is limited, and in addition, larger heat resistance exists between the laminated layers prepared by the casting method, so that the improvement of the heat conductivity of the Diamond/SiC composite material is limited, and the heat conductivity of the prepared Diamond/SiC composite material is only about 110W/(m.k) at most.
Disclosure of Invention
The invention aims to solve the technical problems that Diamond particle size cannot be too large, and Diamond/SiC composite material has low heat conductivity and high porosity and void size due to larger heat resistance between casting lamination layers in a casting method, and provides a method for preparing the Diamond/SiC composite material by combining hot die pressing with CVI.
The conception of the invention is as follows:
in order to improve the compactness of the Diamond/SiC composite material, the Diamond preform is prepared by adopting a method of preparing a SiC matrix by adopting hot die pressing and grain composition, and the Diamond/SiC composite material is prepared by adopting a Chemical Vapor Infiltration (CVI) method. The grain grading of the diamond powder adopts a three-level grading method, namely three kinds of diamond powder with large grain size, medium grain size and small grain size. In this way, during the forming process of the diamond preform, the diamond particles with medium particle size will fill the gaps between the diamond particles with large particle size, and the diamond particles with small particle size will further fill the gaps between the diamond particles with large particle size and the diamond particles with medium particle size. The method and the hot molding process can effectively improve the density of the Dianned/SiC composite material and the volume content of diamond thereof, thereby improving the heat conductivity thereof.
In order to solve the technical problems and complete the conception, the invention adopts the following technical scheme:
the method for preparing the Diamond/SiC composite material by combining hot die pressing and CVI is characterized by comprising the following steps of:
step 1: mixing a plurality of diamond powder materials with different particle sizes and polyvinyl butyral, and performing ball milling to obtain powder materials;
step 2: brushing a release agent on the inner surface of a die, flatly laying the powder obtained in the step 1, pouring the powder into the die, heating and preserving heat of the die, applying pressure to the die, and demolding to obtain a diamond preform after the die is cooled;
step 3: and (3) fixing the Diamond preform prepared in the step (2), and putting the Diamond preform into a chemical vapor infiltration furnace to perform chemical vapor infiltration deposition on the SiC matrix to obtain the Diamond/SiC composite material.
Further, in the step 1, the number of the diamond powder is three, and the diameter ratio of the three diamond powder is D Big size :D In (a) :D Small size = (4-7): (2-3): 1, mass ratio m Big size :m In (a) :m Small size =(17~25):(7~12):1;
The proportion of the total mass of the diamond powder to the total mass of the polyvinyl butyral is (6-9): 1.
further, the step 2 specifically comprises:
uniformly coating a release agent on the inner surface of a die, then spreading and pouring the mixed powder into the die, heating the die to 80-350 ℃, keeping the temperature for 0.5-3h, finally applying a pressure of 5-40MPa to the die, and demoulding after the die is cooled to obtain the diamond preform with the thickness of 2-3 mm.
Further, in the step 3, the chemical vapor infiltration SiC substrate specifically includes:
the method comprises the steps of using trichloromethylsilane as a precursor, hydrogen as a carrier gas, the flow rate ratio of the trichloromethylsilane to the hydrogen is 1:10, argon as a diluent gas, the flow rate of the argon is 200-400mL/min, the total air pressure of a chemical vapor infiltration furnace is 0.5-5 kPa, the deposition temperature is 873-1773K, the time for depositing a SiC matrix is 500-700h, and the density of a Diamond/SiC composite material reaches 2.9-3.1g/cm 3 。
Further, in the step 1, the ball milling time is 5-15h, and the ball milling roller speed is 50-300r/min.
Further, in step 2, the mold is a steel mold.
Further, in step 3, the fixing adopts a graphite fixture.
Further, in the step 2, the step of coating the inner surface of the mold with a release agent specifically includes:
a layer of polytetrafluoroethylene paper is stuck on the working surface of the steel mold, and then the inner surface of the steel mold is uniformly coated with dimethyl silicone oil.
Further, in the step 1, the number of the diamond powder is three, and the diameter ratio of the three diamond powder is D Big size :D In (a) :D Small size =4: 3:1 mass ratio m Big size :m In (a) :m Small size =17:7:1。
Compared with the prior art, the technical scheme of the invention has the beneficial effects that:
the invention adopts a method of thermal molding and grain composition combining and is combined with a CVI process to prepare the Diamond/SiC composite material. The method can effectively solve the problem of difficult molding of the large-grain-diameter diamond preform, and can effectively improve the density of the composite material and the volume content of diamond, thereby effectively improving the thermal conductivity and the mechanical property of the composite material. Moreover, the method has simple production process and convenient operation, and is suitable for industrial production.
Drawings
FIG. 1 is a flow chart of a method of preparing a Diamond/SiC composite material by thermal compression bonding CVI according to the present invention;
FIG. 2 is a schematic diagram of fracture morphology of a 100 μm graded Diamond preform in a second embodiment of a method for preparing a Diamond/SiC composite material by thermal compression and CVI in accordance with the present invention;
FIG. 3 is a schematic diagram of fracture morphology of a 250 μm graded Diamond preform in example III of a method for preparing a Diamond/SiC composite material by thermal compression and CVI according to the present invention;
FIG. 4 is a schematic diagram of fracture morphology of a 350 μm graded Diamond preform in example IV of a method of preparing a Diamond/SiC composite material by thermal compression and CVI according to the present invention;
FIG. 5 is a schematic diagram of fracture morphology of a 500 μm graded Diamond preform in a fifth embodiment of a method of preparing a Diamond/SiC composite material by thermal compression and CVI according to the present invention;
FIG. 6 is a SEM image of a fracture of a Diamond/SiC composite in example one of the method of preparing a Diamond/SiC composite by thermal compression bonding CVI according to the present invention.
Detailed Description
Example 1
As shown in FIG. 1, diamond powder with 100 mu m grading is subjected to hot die pressing and CVI (chemical vapor infiltration) preparation, and the density of the Diamond/SiC composite material reaches 3.0g/cm 3 :
Step 1: 63.6% of 100 μm diamond powder, 26.8% of 75 μm diamond powder, 3.7% of 25 μm diamond powder and 7.9% of polyvinyl butyral (PVB) are mixed and then ball-milled for 12 hours at a ball-milling roller speed of 120r/min.
Step 2: sticking a layer of polytetrafluoroethylene paper on the working surface of a steel mold, uniformly brushing dimethyl silicone oil on the inner surface of the steel mold, and then spreading and pouring the mixed powder into the steel mold; and then the steel mould is placed in an oven to be heated for 2.5 hours at the temperature of 100 ℃, and finally the pressure of 25MPa is applied to the steel mould on a press. And after the steel mold is cooled, demolding to obtain the diamond preform with the thickness of 2.2 mm.
Step 3: depositing a diamond preform into a SiC substrate: the obtained diamond preform was subjected to chemical vapor infiltration deposition of SiC matrix using trichlorosilane (CH 3 SiCl 3, MTS) as a precursor, hydrogen as a carrier gas, and a stream of trichlorosilane and hydrogenThe ratio of the deposition temperature is 1:10, the argon is taken as diluent gas, the flow rate of the argon is 350mL/min, the total air pressure of the chemical vapor infiltration furnace is 1.5kPa, the deposition temperature is 1500K, the deposition time is 640h, and the density of the obtained Diamond/SiC composite material reaches 3.0g/cm 3 . As shown in fig. 6, in the SEM image of the Diamond/SiC composite fracture in the first embodiment, it can be seen from fig. 6 that Diamond is uniformly distributed in the SiC matrix, the pore size is smaller, and the density of the Diamond/SiC composite is higher.
Because larger gaps exist among large-grain-size diamonds in the Diamond preform, densification of the Diamond/SiC composite material can be influenced in the process of depositing the SiC matrix, and the porosity and the gap size of the prepared Diamond/SiC composite material are higher, the thermal conductivity and the mechanical property of the composite material are adversely affected, and therefore, a method of adopting three-level Diamond powder particles is selected.
Example two
Carrying out hot die pressing and CVI (chemical vapor infiltration) preparation on Diamond powder with 100 mu m grading to obtain Diamond powder/SiC composite material with density reaching 3.1g/cm 3 :
Step 1: 51.3% of 85 μm diamond powder, 23.9% of 26 μm diamond powder, 2.3% of 12 μm diamond powder and 7.9% of polyvinyl butyral are mixed and then ball-milled for 8 hours at a ball-milling roller speed of 120r/min.
Step 2: sticking a layer of polytetrafluoroethylene paper on the working surface of a steel mold, uniformly brushing dimethyl silicone oil on the inner surface of the steel mold, and then spreading and pouring the mixed powder into the steel mold; and then the steel mould is put into an oven to be heated for 1h at 180 ℃, and finally the pressure of 15MPa is applied to the steel mould on a press. And after the steel mold is cooled, demolding to obtain the diamond preform with the thickness of 2.5 mm.
Step 3: depositing a diamond preform into a SiC substrate: the obtained diamond preform was subjected to chemical vapor infiltration deposition of SiC matrix using trichlorosilane (CH 3 SiCl 3, MTS) as a precursor, hydrogen as a carrier gas, a flow rate ratio of trichlorosilane to hydrogen of 1:10, argon as a diluent gas, and argonThe flow rate of the catalyst is 200mL/min, the total air pressure of the chemical vapor infiltration furnace is 1.5kPa, the deposition temperature is 1500K, and the deposition time is 500h until the density of the obtained Diamond/SiC composite material reaches 3.1g/cm 3 . As can be seen from fig. 2, the small particles in the diamond preform are well filled between the gaps of the large particles, the internal structure of the diamond preform is also relatively uniform, and the surface of the diamond particles is uniformly coated by PVB.
Example III
Carrying out hot die pressing and CVI (chemical vapor infiltration) preparation on Diamond powder with 250 mu m grading to obtain Diamond powder/SiC composite material with density reaching 2.9g/cm 3 :
Step 1: 62.9% of 260 μm diamond powder, 26.6% of 188 μm diamond powder, 3.7% of 63 μm diamond powder and 7.8% of polyvinyl butyral are mixed and then ball-milled for 5 hours at a ball-milling roller speed of 300r/min.
Step 2: sticking a layer of polytetrafluoroethylene paper on the working surface of a steel mold, uniformly brushing dimethyl silicone oil on the inner surface of the steel mold, and then spreading and pouring the mixed powder into the steel mold; and then the steel mould is put into an oven to be heated for 3 hours at 80 ℃, and finally the pressure of 5MPa is applied to the steel mould on a press. And after the steel mold is cooled, demolding to obtain the diamond preform with the thickness of 2 mm.
Step 3: depositing a diamond preform into a SiC substrate: the obtained diamond preform was subjected to chemical vapor infiltration deposition of SiC matrix using trichlorosilane (CH 3 SiCl 3, MTS) is used as a precursor, hydrogen is used as carrier gas, the flow ratio of the trichloromethylsilane to the hydrogen is 1:10, argon is used as diluent gas, the flow rate of the argon is 250mL/min, the total air pressure of the chemical vapor infiltration furnace is 1.5kPa, the deposition temperature is 1500K, the deposition time is 550h, and the density of the obtained Diamond/SiC composite material reaches 2.9g/cm 3 . As can be seen from fig. 3, the small particles in the diamond preform are well filled between the gaps of the large particles, the internal structure of the diamond preform is also relatively uniform, and the surface of the diamond particles is uniformly coated by PVB.
Example IV
Carrying out hot die pressing and CVI (chemical vapor infiltration) preparation on Diamond powder with 350 mu m grading to obtain Diamond/SiC composite material with density reaching 3.05g/cm 3 :
Step 1: 70% of 360 μm diamond powder, 28.8% of 270 μm diamond powder, 3.7% of 88 μm diamond powder and 7.8% of polyvinyl butyral are mixed and then ball-milled for 15 hours at a ball-milling roller speed of 50r/min.
Step 2: and sticking a layer of polytetrafluoroethylene paper on the working surface of the steel mold, uniformly brushing the dimethyl silicone oil on the inner surface of the steel mold, and then spreading and pouring the mixed powder into the steel mold. And then placing the steel mold into an oven to heat for 0.5h at 350 ℃, and finally applying pressure of 40MPa to the steel mold on a press. And after the steel mold is cooled, demolding to obtain the diamond preform with the thickness of 3.0 mm.
Step 3: depositing a diamond preform into a SiC substrate: the obtained diamond preform was subjected to chemical vapor infiltration deposition of SiC matrix using trichlorosilane (CH 3 SiCl 3, MTS) is used as a precursor, hydrogen is used as carrier gas, the flow ratio of the trichloromethylsilane to the hydrogen is 1:10, argon is used as diluent gas, the flow rate of the argon is 300mL/min, the total air pressure of a chemical vapor infiltration furnace is 1.5kPa, the deposition temperature is 1500K, the deposition time is 600h, and the density of the obtained Diamond/SiC composite material reaches 3.05g/cm 3 . As can be seen from fig. 4, the small particles in the diamond preform are well filled between the gaps of the large particles, the internal structure of the diamond preform is also relatively uniform, and the surface of the diamond particles is uniformly coated by PVB.
Example five
Carrying out hot die pressing and CVI (chemical vapor infiltration) preparation on Diamond powder with 500 mu m grading to obtain Diamond powder/SiC composite material with density reaching 2.95g/cm 3 :
Step 1: 63.5% of 500 μm diamond powder, 26.1% of 350 μm diamond powder, 3.7% of 124 μm diamond powder and 6.7% of polyvinyl butyral are mixed and then ball-milled for 10 hours at a ball-milling roller speed of 200r/min.
Step 2: and sticking a layer of polytetrafluoroethylene paper on the working surface of the steel mold, uniformly brushing the dimethyl silicone oil on the inner surface of the steel mold, and then spreading and pouring the mixed powder into the steel mold. And then the steel mould is put into a baking oven to be heated for 2.0h at 220 ℃, and finally the pressure of 35MPa is applied to the steel mould on a press. And after the steel mold is cooled, demolding to obtain the diamond preform with the thickness of 2.7 mm.
Step 3: depositing a diamond preform into a SiC substrate: the obtained diamond preform was subjected to chemical vapor infiltration deposition of SiC matrix using trichlorosilane (CH 3 SiCl 3, MTS) is used as a precursor, hydrogen is used as carrier gas, the flow ratio of the trichloromethylsilane to the hydrogen is 1:10, argon is used as diluent gas, the flow rate of the argon is 400mL/min, the total air pressure of the chemical vapor infiltration furnace is 1.5kPa, the deposition temperature is 1500K, the deposition time is 700h, and the density of the obtained Diamond/SiC composite material reaches 2.95g/cm 3 . As can be seen from fig. 5, the small particles in the diamond preform are well filled between the gaps of the large particles, the internal structure of the diamond preform is also relatively uniform, and the surface of the diamond particles is uniformly coated by PVB.
Claims (9)
1. A method for preparing a Diamond/SiC composite material by thermal compression bonding with CVI, comprising the steps of:
step 1: mixing a plurality of diamond powder materials with different particle sizes and polyvinyl butyral, and performing ball milling to obtain powder materials;
step 2: brushing a release agent on the inner surface of a die, flatly laying the powder obtained in the step 1, pouring the powder into the die, heating and preserving heat of the die, applying pressure to the die, and demolding to obtain a diamond preform after the die is cooled;
step 3: and (3) fixing the Diamond preform prepared in the step (2), and putting the Diamond preform into a chemical vapor infiltration furnace to perform chemical vapor infiltration deposition on the SiC matrix to obtain the Diamond/SiC composite material.
2. A method of preparing a Diamond/SiC composite material by thermal compression bonding with CVI according to claim 1, wherein:
in the step 1, the number of the diamond powder is three, and the diameter ratio of the three diamond powder is D Big size :D In (a) :D Small size = (4-7): (2-3): 1, mass ratio m Big size :m In (a) :m Small size =(17~25):(7~12):1;
The total mass ratio of the diamond powder to the polyvinyl butyral is (6-9): 1.
3. the method for preparing the Diamond/SiC composite material by combining hot die pressing with CVI according to claim 2, wherein the step 2 is specifically as follows:
uniformly coating a release agent on the inner surface of a die, then spreading and pouring the mixed powder into the die, heating the die to 80-350 ℃, keeping the temperature for 0.5-3h, finally applying a pressure of 5-40MPa to the die, and demoulding after the die is cooled to obtain the diamond preform with the thickness of 2-3 mm.
4. A method for preparing a Diamond/SiC composite material according to claim 1, 2 or 3, wherein in step 3, the chemical vapor infiltration SiC matrix is specifically:
the method comprises the steps of using trichloromethylsilane as a precursor, hydrogen as a carrier gas, the flow rate ratio of the trichloromethylsilane to the hydrogen is 1:10, argon as a diluent gas, the flow rate of the argon is 200-400mL/min, the total air pressure of a chemical vapor infiltration furnace is 0.5-5 kPa, the deposition temperature is 873-1773K, the time for depositing a SiC matrix is 500-700h, and the density of a Diamond/SiC composite material reaches 2.9-3.1g/cm 3 。
5. A method of preparing a Diamond/SiC composite material by thermal compression bonding with CVI according to claim 4, wherein:
in the step 1, the ball milling time is 5-15h, and the ball milling roller speed is 50-300r/min.
6. A method of preparing a Diamond/SiC composite material by thermal compression bonding with CVI according to claim 5, wherein:
in the step 2, the die is a steel die.
7. A method of preparing a Diamond/SiC composite material by thermal compression bonding with CVI according to claim 6, wherein:
in the step 3, a graphite clamp is adopted for fixing.
8. The method for preparing Diamond/SiC composite material by thermal molding and CVI according to claim 7, wherein in step 2, the inner surface of the mold is coated with a release agent specifically comprises:
a layer of polytetrafluoroethylene paper is stuck on the working surface of the steel mold, and then the inner surface of the steel mold is uniformly coated with dimethyl silicone oil.
9. A method of preparing a Diamond/SiC composite material by thermal compression bonding with CVI according to claim 8, wherein:
in the step 1, the number of the diamond powder is three, and the diameter ratio of the three diamond powder is D Big size :D In (a) :D Small size =4: 3:1 mass ratio m Big size :m In (a) :m Small size =17:7:1。
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CN103724014A (en) * | 2013-12-26 | 2014-04-16 | 西北工业大学 | Preparation method of diamond doped silicon carbide (SiC) ceramics with high heat conductivity |
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CN105777172A (en) * | 2016-03-30 | 2016-07-20 | 西北工业大学 | Method for preparing Diamond/SiC composite material by combining thermally compression molding with chemical vapor infiltration (CVI) |
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CN103724014A (en) * | 2013-12-26 | 2014-04-16 | 西北工业大学 | Preparation method of diamond doped silicon carbide (SiC) ceramics with high heat conductivity |
CN105347799A (en) * | 2015-11-30 | 2016-02-24 | 西北工业大学 | Preparation method of large-particle-diameter Diamond/SiC composite |
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