CN105347799A - Preparation method of large-particle-diameter Diamond/SiC composite - Google Patents
Preparation method of large-particle-diameter Diamond/SiC composite Download PDFInfo
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Abstract
The invention relates to a preparation method of a large-particle-diameter Diamond/SiC composite. The Diamond/SiC composite is prepared by adopting a method of combining a one-time formed large-particle-diameter diamond precast body with a CVI technology. By means of the method, the particle diameter and the volume content of diamond in the composite are increased, and the thermal conductivity of the composite is effectively increased. The thermal conductivity of the composite is increased by about 30 percent compared with a composite prepared through a method of combining flow casting with the CVI method. In addition, the method is simple in production technology, controllable and capable of being used for industrial production.
Description
Technical field
The invention belongs to the preparation method of Diamond/SiC matrix material, be specifically related to a kind of preparation method of Large stone Diamond/SiC matrix material, is the matrix material utilizing chemical vapor infiltration (CVI) to prepare the diamond doped SiC of Large stone.
Background technology
Diamond/SiC matrix material has the advantages such as high rigidity, high-wearing feature, low density, high heat conductance, low thermal coefficient of expansion, good high-temperature stability because of it and is widely applied in the middle of felt at the bottom of PDC high-abrasive material, resistance to compression, petroleum machinery drill bit, mirror substrate and electronic package material.The characteristics such as this high thermal conductance, low heat expansion property and low density of wherein having due to Diamond/SiC matrix material make it can as forth generation electronic package material, thus adapt to the use of current high performance chips and extensive and super large-scale integration and the high integration of electronic device chip, high packaging density and high operate frequency to the requirement of packaged material.
The main technique of current preparation Diamond/SiC matrix material mainly contains: High Temperature High Pressure sintering (HPHT), reactive melt infiltration gas-phase silicon (RMI), HIP sintering (HIP), precursor synthesis method conversion method (PIP) and discharge plasma sintering (SPS) etc.But these methods otherwise be to the requirement of equipment and hazard level high, be difficult to obtained large-sized Diamond/SiC sheet material.Be have residual silicon in obtained sample, make the mechanical properties decrease of product.In addition, the preparation temperature due to above method is general higher, and this makes diamond very easily greying occur, and has a strong impact on mechanical property and the heat physical properties of matrix material.
In order to solve above-mentioned problem, have employed curtain coating first in document " YongshengLiuandChenghaoHuMicrostructureandpropertiesofdi amond/SiCcompositespreparedbytape-castingandchemicalvapo rinfiltrationprocess [J] .J.Eur.Ceram.Soc.; 34,3489-3498 (2014). " and patent No. ZL201310739082.7 and obtain Diamond/SiC matrix material in conjunction with chemical vapor infiltration (CVI).The method requires that the diamond slurry first configuring different-grain diameter (7 ~ 27 μm) carries out curtain coating experiment, then substrate drying good for curtain coating is placed in CVI cvd furnace and deposits SiC matrix, obtain Diamond/SiC thin slice, thin slice is taken out on its surface curtain coating and deposition repeatedly.Finally, the diamond/silicon carbide composite sample that thickness is about 2mm is obtained.
Because chemical vapor infiltration reaction conditions is gentleer, and the SiC of deposition is generated in-situ, avoiding problems the problem of diamond graphitization and residual silicon in matrix material.Preparation-obtained Diamond/SiC/ matrix material is diamond and silicon carbide two-phase, without other impurity, diamond is evenly distributed in the composite and is combined well with matrix diamond.In addition, CVI, as a kind of technique of comparative maturity preparing ceramic matric composite, can realize suitability for industrialized production.
But in curtain coating in conjunction with in CVI method, due to the limitation of casting method itself, the particle diameter of the diadust adopted can not be too large, which limits the raising of diamond intrinsic thermal conductivity, thus limit the raising of Diamond/SiC heat conductivity, make thermal conductivity the highest the 110W/ that has an appointment (mk) of the matrix material prepared.
Summary of the invention
The technical problem solved
In order to avoid the deficiencies in the prior art part, the present invention proposes a kind of preparation method of Large stone Diamond/SiC matrix material, solves curtain coating and prepares in conjunction with CVI the technical barrier that diamond particle diameter in Diamond/SiC matrix material can not be too large.
Technical scheme
A preparation method for Large stone Diamond/SiC matrix material, is characterized in that step is as follows:
Step 1: obtain slurry by after the solvent ball milling of the anti-settling thickening material of the diamond powder of 56% ~ 66% massfraction, 0.35% ~ 1.38% mass fraction, the polyvinyl butyral acetal of 3.5% ~ 4.2% mass fraction and 30.3% ~ 38.3% mass fraction; Described solvent is the dehydrated alcohol of 1: 1 mass ratio and the mixed solvent of butanone; The quality summation of described each component is absolutely;
Step 2: the slurry mixed is poured in mould, until it after seasoning under air ambient, after the demoulding, obtained thickness is about the diamond precast body of 2-3mm; The internal surface brushing releasing agent of described mould;
Step 3: adopted after graphite fixture by diamond precast body, puts into chemical vapor infiltration poke CVI stove and carries out chemical vapor infiltration and prepare Diamond/SiC matrix material; After SiC shell appears in Diamond/SiC composite material surface, proceed deposition after being polished off by the SiC shell on its surface, until the density of Diamond/SiC matrix material reaches about 3.1g/cm
3.
The ball milling of described step 1 is: ball milling cylinder speed is 50-300r/min, and the time is 5-15h.
The technique of the CVI method generation SiC matrix of described step 3 is: using trichloromethyl silane MTS as precursor, and hydrogen is as carrier gas, and argon gas is as diluent gas, and its flow rate is than being 1:5 ~ 50:2 ~ 20, and total gas pressure is 0.5 ~ 5kPa, and depositing temperature is 873 ~ 1773K.
The particle diameter of described diamond powder is 50 ~ 500um.
Beneficial effect
The preparation method of a kind of Large stone Diamond/SiC matrix material that the present invention proposes, adopts the method that once shaped Large stone diamond precast body is combined with CVI technique, obtained Diamond/SiC matrix material.Employing the method increases adamantine particle diameter and volume content in matrix material, thus effectively raises the thermal conductivity of matrix material.The matrix material that thermal conductivity is prepared than curtain coating in conjunction with CVI method improves about 30%.Moreover, the method production technique is simple, controlled, can be used for suitability for industrialized production.
Accompanying drawing explanation
Fig. 1: the schematic flow sheet of the inventive method
Fig. 2: the fracture apperance figure of Diamond/SiC matrix material prepared by the inventive method
Fig. 3: the present invention adopts the thermal conductivity figure of the matrix material of different diamond particle diameter
Embodiment
Now in conjunction with the embodiments, the invention will be further described for accompanying drawing:
Embodiment one
Step 1. by mass percentage, by the bortz powder of the 50um of 62.3%, the polyvinyl butyral acetal of 4.2%, the anti-settling thickening material of 0.3%, ball milling is carried out after solvent (ethanol and butanone add according to the mass ratio 1:1) mixing of 33.2%, Ball-milling Time is 10h, and ball milling cylinder speed is 120r/min.
Floorage is internal surface even brushing one deck silicone oil in advance of the mould of 55 × 55 by step 2., is then taken out by slurry good for aforementioned ball milling, evenly pours among mould.Make it in atmosphere after complete drying, carry out the demoulding of diamond precast body, the diamond precast body that thickness is about 2mm can be obtained.
Diamond preform deposition SiC matrix is obtained Diamond/SiC matrix material by step 3.: the diamond precast body obtained is carried out chemical vapor infiltration deposition SiC matrix, utilize MTS (CH3SiCl3) as precursor, hydrogen as carrier gas, argon gas as diluent gas, its flow rate is than being 1:40:40, wherein the flow rate of argon gas is 350mL/min, total gas pressure is 5000Pa, and depositing temperature is 1273K.
Step 4., after SiC shell appears in Diamond/SiC composite material surface, can affect reactant gases and enter the densification that material internal affects material, proceeds deposition after now needing the SiC shell of composite material surface to polish off.Finally obtain thickness and be about the thick Diamond/SiC matrix material of 2mm, density is 3.03g/cm
3, ventilate rate is 8.8%.
Embodiment two
Step 1. by mass percentage, by the bortz powder of the 104um of 57.4%, the polyvinyl butyral acetal of 3.8%, the anti-settling thickening material of 0.5%, ball milling is carried out after solvent (ethanol and butanone add according to the mass ratio 1:1) mixing of 38.3%, Ball-milling Time is 10h, and ball milling cylinder speed is 120r/min.
Floorage is internal surface even brushing one deck silicone oil in advance of the mould of 55 × 55 by step 2., is then taken out by slurry good for aforementioned ball milling, evenly pours among mould.Make it in atmosphere after complete drying, carry out the demoulding of diamond precast body, the diamond precast body that thickness is about 2mm can be obtained.
Diamond preform deposition SiC matrix is obtained Diamond/SiC matrix material by step 3.: the diamond precast body obtained is carried out chemical vapor infiltration deposition SiC matrix, utilize MTS (CH3SiCl3) as precursor, hydrogen as carrier gas, argon gas as diluent gas, its flow rate is than being 1:40:40, wherein the flow rate of argon gas is 350mL/min, total gas pressure is 5000Pa, and depositing temperature is 1273K.
Step 4., after SiC shell appears in Diamond/SiC composite material surface, can affect reactant gases and enter the densification that material internal affects material, proceeds deposition after now needing the SiC shell of composite material surface to polish off.Finally obtain thickness and be about the thick Diamond/SiC matrix material of 2mm, density is 3.04g/cm3, and ventilate rate is 7.6%.
Embodiment three
Step 1. by mass percentage, by the bortz powder of the 250um of 61.5%, the polyvinyl butyral acetal of 4.2%, the anti-settling thickening material of 0.5%, ball milling is carried out after solvent (ethanol and butanone add according to the mass ratio 1:1) mixing of 33.8%, Ball-milling Time is 10h, and ball milling cylinder speed is 120r/min.
Floorage is internal surface even brushing one deck silicone oil in advance of the mould of 55 × 55 by step 2., is then taken out by slurry good for aforementioned ball milling, evenly pours among mould.Make it in atmosphere after complete drying, carry out the demoulding of diamond precast body, the diamond precast body that thickness is about 2.5mm can be obtained.
Diamond preform deposition SiC matrix is obtained Diamond/SiC matrix material by step 3.: the diamond precast body obtained is carried out chemical vapor infiltration deposition SiC matrix, utilize MTS (CH3SiCl3) as precursor, hydrogen as carrier gas, argon gas as diluent gas, its flow rate is than being 1:40:40, wherein the flow rate of argon gas is 350mL/min, total gas pressure is 5000Pa, and depositing temperature is 1273K.
Step 4., after SiC shell appears in Diamond/SiC composite material surface, can affect reactant gases and enter the densification that material internal affects material, proceeds deposition after now needing the SiC shell of composite material surface to polish off.Finally obtain thickness and be about the thick Diamond/SiC matrix material of 2.5mm, density is 3.17g/cm
3, ventilate rate is 3.1%.
Embodiment four
Step 1. by mass percentage, by the bortz powder of the 350um of 64.9%, the polyvinyl butyral acetal of 3.93%, the anti-settling thickening material of 0.87%, ball milling is carried out after solvent (ethanol and butanone add according to the mass ratio 1:1) mixing of 30.3%, Ball-milling Time is 10h, and ball milling cylinder speed is 120r/min.
Floorage is internal surface even brushing one deck silicone oil in advance of the mould of 55 × 55 by step 2., is then taken out by slurry good for aforementioned ball milling, evenly pours among mould.Make it in atmosphere after complete drying, carry out the demoulding of diamond precast body, the diamond precast body that thickness is about 2.5mm can be obtained.
Diamond preform deposition SiC matrix is obtained Diamond/SiC matrix material by step 3.: the diamond precast body obtained is carried out chemical vapor infiltration deposition SiC matrix, utilize MTS (CH3SiCl3) as precursor, hydrogen as carrier gas, argon gas as diluent gas, its flow rate is than being 1:40:40, wherein the flow rate of argon gas is 350mL/min, total gas pressure is 5000Pa, and depositing temperature is 1273K.
Step 4., after SiC shell appears in Diamond/SiC composite material surface, can affect reactant gases and enter the densification that material internal affects material, proceeds deposition after now needing the SiC shell of composite material surface to polish off.Finally obtain thickness and be about the thick Diamond/SiC matrix material of 2.5mm, density is 3.14g/cm
3, ventilate rate is 5.6%.
Embodiment five
Step 1. by mass percentage, by the bortz powder of the 500um of 60.6%, the polyvinyl butyral acetal of 3.5%, the anti-settling thickening material of 1.3%, ball milling is carried out after solvent (ethanol and butanone add according to the mass ratio 1:1) mixing of 34.6%, Ball-milling Time is 10h, and ball milling cylinder speed is 120r/min.
Floorage is internal surface even brushing one deck silicone oil in advance of the mould of 55 × 55 by step 2., is then taken out by slurry good for aforementioned ball milling, evenly pours among mould.Make it in atmosphere after complete drying, carry out the demoulding of diamond precast body, the diamond precast body that thickness is about 2.5mm can be obtained.
Diamond preform deposition SiC matrix is obtained Diamond/SiC matrix material by step 3.: the diamond precast body obtained is carried out chemical vapor infiltration deposition SiC matrix, utilize MTS (CH3SiCl3) as precursor, hydrogen as carrier gas, argon gas as diluent gas, its flow rate is than being 1:40:40, wherein the flow rate of argon gas is 350mL/min, total gas pressure is 5000Pa, and depositing temperature is 1273K.
Step 4., after SiC shell appears in Diamond/SiC composite material surface, can affect reactant gases and enter the densification that material internal affects material, proceeds deposition after now needing the SiC shell of composite material surface to polish off.Finally obtain thickness and be about the thick Diamond/SiC matrix material of 2.5mm, density is 3.18g/cm
3, ventilate rate is 3.9%.
Claims (4)
1. a preparation method for Large stone Diamond/SiC matrix material, is characterized in that step is as follows:
Step 1: obtain slurry by after the solvent ball milling of the anti-settling thickening material of the diamond powder of 56% ~ 66% massfraction, 0.35% ~ 1.38% mass fraction, the polyvinyl butyral acetal of 3.5% ~ 4.2% mass fraction and 30.3% ~ 38.3% mass fraction; Described solvent is the dehydrated alcohol of 1: 1 mass ratio and the mixed solvent of butanone; The quality summation of described each component is absolutely;
Step 2: the slurry mixed is poured in mould, until it after seasoning under air ambient, after the demoulding, obtained thickness is about the diamond precast body of 2-3mm; The internal surface brushing releasing agent of described mould;
Step 3: adopted after graphite fixture by diamond precast body, puts into chemical vapor infiltration poke CVI stove and carries out chemical vapor infiltration and prepare Diamond/SiC matrix material; After SiC shell appears in Diamond/SiC composite material surface, proceed deposition after being polished off by the SiC shell on its surface, until the density of Diamond/SiC matrix material reaches about 3.1g/cm
3.
2. the preparation method of Large stone Diamond/SiC matrix material according to claim 1, it is characterized in that: the ball milling of described step 1 is: ball milling cylinder speed is 50-300r/min, the time is 5-15h.
3. the preparation method of Large stone Diamond/SiC matrix material according to claim 1, it is characterized in that: the technique of the CVI method generation SiC matrix of described step 3 is: using trichloromethyl silane MTS as precursor, hydrogen is as carrier gas, argon gas is as diluent gas, its flow rate is than being 1:5 ~ 50:2 ~ 20, total gas pressure is 0.5 ~ 5kPa, and depositing temperature is 873 ~ 1773K.
4. the preparation method of Large stone Diamond/SiC matrix material according to claim 1, is characterized in that: the particle diameter of described diamond powder is 50 ~ 500um.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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) |
| CN109704798A (en) * | 2019-01-09 | 2019-05-03 | 西北工业大学 | The method that vacuum impregnation association reaction melt infiltration RMI prepares C/SiC-Diamond composite material |
| CN111484330A (en) * | 2020-04-13 | 2020-08-04 | 北京科技大学广州新材料研究院 | Diamond-enhanced silicon carbide substrate, preparation method thereof and electronic product |
| CN114315354A (en) * | 2021-12-29 | 2022-04-12 | 武汉理工大学 | Diamond-B4Two-step sintering method of C-SiC three-phase composite ceramic |
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| US20060217258A1 (en) * | 2003-05-30 | 2006-09-28 | The Regents Of The University Of California | Diamond-silicon carbide composite and method |
| 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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| US20060217258A1 (en) * | 2003-05-30 | 2006-09-28 | The Regents Of The University Of California | Diamond-silicon carbide composite and method |
| 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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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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) |
| CN109704798A (en) * | 2019-01-09 | 2019-05-03 | 西北工业大学 | The method that vacuum impregnation association reaction melt infiltration RMI prepares C/SiC-Diamond composite material |
| CN111484330A (en) * | 2020-04-13 | 2020-08-04 | 北京科技大学广州新材料研究院 | Diamond-enhanced silicon carbide substrate, preparation method thereof and electronic product |
| CN114315354A (en) * | 2021-12-29 | 2022-04-12 | 武汉理工大学 | Diamond-B4Two-step sintering method of C-SiC three-phase composite ceramic |
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