CN111635233A - In-situ generated AlN/SiC combined C composite material and preparation method thereof - Google Patents
In-situ generated AlN/SiC combined C composite material and preparation method thereof Download PDFInfo
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Abstract
The invention relates to an in-situ generated AlN/SiC combined C composite material and a preparation method thereof. The technical scheme is as follows: mixing Al4SiC4Mixing the powder and a binder to obtain a mixture I; or mixing Al4SiC4Mixing the powder with the material containing C and then mixing with a binder to obtain a mixture II; the mixture is mixture I or mixture II. Pre-pressing and forming the mixture, performing isostatic pressing and drying at 110 ℃ to obtain a prefabricated blank; placing the graphite crucible with the prefabricated blank body in a gas pressure sintering furnace, and heating the graphite crucible to 1000-1200 ℃ from room temperature under the condition that the mbar is less than or equal to 0.1 mbar; heat preservationFilling N under the condition2And (3) heating to 1600-1800 ℃ under the pressure maintaining condition at the pressure of 1-5 MPa, maintaining the pressure and preserving the heat, and naturally cooling to room temperature to prepare the AlN/SiC combined C composite material generated in situ. The AlN/SiC combined C composite material prepared by the method has the advantages of low density, light weight, uniform phase distribution, high strength, good thermal shock resistance and excellent oxidation resistance.
Description
Technical Field
The invention belongs to the technical field of AlN/SiC combined C composite materials. In particular to an in-situ generated AlN/SiC combined C composite material and a preparation method thereof.
Background
The oxide-carbon composite material has excellent erosion resistance and thermal shock stability due to the introduction of graphite, and is widely applied to high-temperature systems in the metallurgical industry. With the continuous development of smelting technology, the carbon composite material develops towards low carbonization, and the contradiction of low carbonization and the synergistic improvement of thermal shock stability and slag penetration resistance appears, so that the application of the carbon composite material is severely restricted. In recent years, non-oxides and composite materials thereof become a new generation of high-quality composite materials with excellent high-temperature strength, oxidation resistance, erosion resistance and other performances, and are applied to key parts of many high-temperature industries. Especially, the AlN/SiC composite material has attracted great attention in the electronic field and the high temperature ceramic field due to the characteristics of excellent mechanical property, high temperature resistance, erosion resistance and the like. However, as the non-oxide and the composite material thereof are studied more deeply, it is found that the thermal shock resistance and toughness thereof are gradually difficult to satisfy the practical application, and further improvement is urgently needed.
Since the 21 st century, the rapid development of novel carbon materials such as carbon fibers, expanded graphite, carbon nanotubes, graphene and fullerene has attracted extensive attention of global researchers, and the carbon materials are increasingly used as reinforcement materials for various composite materials due to excellent properties such as good high temperature resistance, erosion resistance, high temperature oxidation resistance and high fracture toughness. Therefore, the AlN/SiC is combined with a novel carbon material to prepare a non-oxide-bonded carbon composite material, and an advanced refractory material with long service life, high temperature resistance, high erosion resistance and high mechanical property is expected to be developed so as to solve the problems of the contradiction of the synergistic improvement of low carbonization and thermal shock stability and slag penetration resistance, the low fracture toughness of the non-oxide composite material and the like.
In recent years, in the preparation of AlN-SiC composite materials, XRD and NMR studies of SiC-AlN solid solutions have been carried out by people such as Tatan shogao and the like (Tatan shogao, Yueyuan; [ J ]]The silicate science report 1997 (3) 345 and 349) adopts a pressureless sintering method, 6H-SiC is taken as a raw material, a small amount of A1N is doped, and the pressureless sintering is carried out at 2050 ℃ under Ar atmosphere to prepare the single-phase 4H type SiC-AlN solid solution. Also in the preparation of carbon material-bonded non-oxide composite materials, e.g., Chen et al (Chen W, Tojo T, Miyamoto Y. SiCERAMIC-bonded carbon composite with Si3N4and carbon powders[J]International Journal of Applied Ceramic Technology,2012,9(2):313-3N4And carbon powder is taken as a raw material, a discharge plasma sintering method is adopted, the SiC/CBC composite material is prepared in situ at the temperature of 1700-1900 ℃, silicon carbide grains grow up along with the increase of the sintering temperature, the physical combination with the carbon grains is enhanced, and the mechanical property and the thermal conductivity of the obtained material are effectively improved. He et al (He X, Gong Q, Du Y, et al preparation, microstructures and properties of AlN/CBC compositions [ J]Materials characterization,2018,136: 417-.
The method adopts a plurality of raw materials to be mechanically mixed and then to be sintered at high temperature, the dispersibility and uniformity of phases in the obtained composite material are not easy to control, the material performance is difficult to regulate and control, and meanwhile, the novel composite material of the honeycomb microstructure, such as non-oxide combined carbon, is only widely applied to the fields of high-power semiconductor equipment, heat dissipation substrates, high-temperature parts and the like, and is less applied to the field of refractory materials.
In addition, "a foaming-based AlN-SiC porous composite ceramic and a preparation method thereof" (CN01811229600.X) adopts a single ternary carbide Al4SiC4Preparing AlN/SiC porous composite ceramic from the raw material, and preparing the material into a porous structure under normal pressure to enable Al to be in a porous structure4SiC4Completely nitridizing to obtain the porous material with SiC as a framework and whisker-shaped AlN as a reinforcing phaseCeramic with a layered structure, but is only suitable for use in the field of filters.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides an in-situ generated AlN/SiC combined C composite material which has the advantages of light weight, uniform phase distribution, high fracture toughness, good thermal shock resistance and excellent oxidation resistance and erosion resistance.
In order to achieve the purpose, the invention adopts the technical scheme that:
step 1, prefabrication of mixture
The mixture is mixture I or mixture II.
The mixture I is as follows: 95 to 97 weight percent of Al4SiC4And mixing the powder with 3-5 wt% of a binder to obtain a mixture I.
The mixture II comprises: firstly, 85-95 wt% of Al4SiC4Mixing the powder with 5-15 wt% of a C-containing material to obtain a premix; and mixing 95-97 wt% of the premix with 3-5 wt% of a binder to obtain a mixture II.
The Al is4SiC4The purity of the powder is more than or equal to 98.0 wt%, and Al4SiC4The particle size of the powder is less than or equal to 150 mu m.
Step 2, prefabricating a blank
The mixture is pre-pressed and molded under the condition of 5-100 MPa, then is subjected to isostatic pressing under the condition of 50-300 MPa, and then is placed in a constant-temperature drying box and is dried for 1-5 hours under the condition of 110 ℃ to obtain a prefabricated blank body.
Step 3, in-situ generation of AlN/SiC combined C composite material
Placing the prefabricated blank into a graphite crucible, then placing the graphite crucible into a pneumatic sintering furnace, and heating the graphite crucible to 1000-1200 ℃ from room temperature at the speed of 5-10 ℃/min under the condition that the pressure is less than or equal to 0.1 mbar; n is filled for 10-20 min under the condition of heat preservation2Heating to 1600-1800 ℃ at the speed of 1-5 ℃/min under the pressure maintaining condition, maintaining the pressure and keeping the temperature for 1-5 h, and naturally cooling to room temperature to prepare the AlN/SiC combined C composite material generated in situ.
The C-containing material is more than one of graphite, coke and carbon black.
The binder is more than one of phenolic resin, epoxy resin and asphalt; the binder used for mix I was the same as the binder used for mix II.
The purity of the nitrogen is more than or equal to 99.999 percent.
Due to the adoption of the scheme, compared with the prior art, the invention has the following advantages:
the invention adopts single Al4SiC4The powder is used as a raw material, and the raw material has excellent oxidation resistance and hydration resistance, so that the oxidation resistance of the AlN/SiC combined C composite material generated in situ can be obviously improved.
Al used in the invention4SiC4The nitridation reaction can occur along with the increase of the sintering temperature, the generated AlN, SiC and C are uniformly distributed in the in-situ generated AlN/SiC combined C composite material, and as the evaporation and diffusion mass transfer rates of all phases in the C composite material are different, a honeycomb structure of AlN/SiC ceramic phase wrapping the C phase is gradually formed in the system; meanwhile, AlN and SiC have similarity in atomic size, molecular weight and crystal structure, so that the two phases are tightly combined without obvious interfaces; the C phase generated in situ is detected to be vermicular graphite, and the special structure of the C phase is used as a reinforcing phase to further improve the strength and the thermal shock resistance of the product. The prepared in-situ generated AlN/SiC combined C composite material has the advantages of uniform phase distribution, high strength and good thermal shock resistance.
The invention adopts a gas pressure sintering method, which can not only promote the sintering of products, but also lead Al to be4SiC4And (4) fully nitriding. The prepared AlN/SiC combined C composite material generated in situ has the characteristics of low density and light weight.
Therefore, the in-situ generated AlN/SiC combined C composite material prepared by the invention has the advantages of low density, light weight, uniform phase distribution, high strength, good thermal shock resistance and excellent oxidation resistance.
Drawings
FIG. 1 is an XRD pattern of an in situ-grown AlN/SiC-bonded C composite material synthesized in accordance with the present invention;
FIG. 2 is a BSE plot of the cross-section of the in-situ grown AlN/SiC-bonded C composite shown in FIG. 1 after polishing.
Detailed Description
The invention will be further described and illustrated with reference to the accompanying drawings and specific embodiments, it being understood that the following specific examples are intended to illustrate the invention and are not intended to limit the scope thereof.
In this embodiment:
the Al is4SiC4The purity of the powder is more than or equal to 98.0 wt%, and Al4SiC4The particle size of the powder is less than or equal to 150 mu m;
the purity of the nitrogen is more than or equal to 99.999 percent.
The C-containing material is more than one of graphite, coke and carbon black.
The binder is more than one of phenolic resin, epoxy resin and asphalt; the binder used for mix I was the same as the binder used for mix II.
The detailed description is omitted in the embodiments.
Example 1
An in-situ generated AlN/SiC combined C composite material and a preparation method thereof.
Step 1, prefabrication of mixture
The mixture is as follows: mixing 95 wt% of Al4SiC4Mixing the powder with 5 wt% of binder to obtain the mixture.
Step 2, prefabricating a blank
The mixture is pre-pressed and formed under the condition of 10MPa, then is subjected to isostatic pressing and forming under the condition of 180MPa, and then is placed in a constant-temperature drying box and is dried for 1 hour under the condition of 110 ℃ to obtain a prefabricated blank body.
Step 3, in-situ generation of AlN/SiC combined C composite material
Placing the prefabricated blank into a graphite crucible, then placing the graphite crucible into a gas pressure sintering furnace, and heating the graphite crucible to 1200 ℃ from room temperature at the speed of 10 ℃/min under the condition that the pressure is less than or equal to 0.1 mbar; charging N for 10min under the condition of heat preservation2Heating to 1700 ℃ at the speed of 5 ℃/min under the pressure maintaining condition, maintaining the pressure and preserving the heat for 2h, and naturally cooling to room temperature to prepare the AlN/SiC combined C composite material generated in situ.
Example 2
An in-situ generated AlN/SiC combined C composite material and a preparation method thereof.
Step 1, prefabrication of mixture
The mixture is as follows: 97 wt% of Al4SiC4Mixing the powder with 3 wt% of binder to obtain a mixture.
Step 2, prefabricating a blank
The mixture is pre-pressed and formed under the condition of 5MPa, then is formed under the condition of 50MPa in an isostatic pressing mode, and then is placed in a constant-temperature drying box and is dried for 5 hours under the condition of 110 ℃ to obtain a prefabricated blank body.
Step 3, in-situ generation of AlN/SiC combined C composite material
Placing the prefabricated blank into a graphite crucible, then placing the graphite crucible into a pneumatic sintering furnace, and heating the graphite crucible to 1000 ℃ from room temperature at the speed of 5 ℃/min under the condition that the pressure is less than or equal to 0.1 mbar; charging N for 20min under the condition of heat preservation2Heating to 1600 ℃ at the speed of 4 ℃/min under the pressure maintaining condition, maintaining the pressure and preserving the heat for 1h, and naturally cooling to room temperature to prepare the AlN/SiC combined C composite material generated in situ.
Example 3
An in-situ generated AlN/SiC combined C composite material and a preparation method thereof.
Step 1, prefabrication of mixture
The mixture is as follows: mixing 96 wt% of Al4SiC4Mixing the powder with 4 wt% of binder to obtain the mixture.
Step 2, prefabricating a blank
The mixture is pre-pressed and formed under the condition of 30MPa, then is formed under the condition of isostatic pressing under the condition of 200MPa, and then is placed in a constant-temperature drying box and is dried for 3 hours under the condition of 110 ℃ to obtain a prefabricated blank body.
Step 3, in-situ generation of AlN/SiC combined C composite material
Placing the prefabricated blank into a graphite crucible, then placing the graphite crucible into a pneumatic sintering furnace, and heating the graphite crucible to 1100 ℃ from room temperature at the speed of 8 ℃/min under the condition that the pressure is less than or equal to 0.1 mbar; charging N for 15min under the condition of heat preservation2Heating to 1800 ℃ at the speed of 3 ℃/min under the pressure maintaining condition until the pressure reaches 3MPa, maintaining the pressure and preserving the heat for 4h, and naturally cooling to room temperature to prepare the AlN/SiC combined C composite material generated in situ.
Example 4
An in-situ generated AlN/SiC combined C composite material and a preparation method thereof.
Step 1, prefabrication of mixture
The mixture is as follows: firstly 85 wt% of Al4SiC4Mixing the powder with 15 wt% of material containing C to obtain premix; then 97 wt% of the premix and 3 wt% of the binder are mixed to obtain a mixture.
Step 2, prefabricating a blank
The mixture is pre-pressed and formed under the condition of 100MPa, then is subjected to isostatic pressing and forming under the condition of 300MPa, and then is placed in a constant-temperature drying box and is dried for 4 hours under the condition of 110 ℃ to obtain a prefabricated blank body.
Step 3, in-situ generation of AlN/SiC combined C composite material
Placing the prefabricated blank into a graphite crucible, then placing the graphite crucible into a gas pressure sintering furnace, and heating the graphite crucible to 1100 ℃ from room temperature at the speed of 6 ℃/min under the condition that the pressure is less than or equal to 0.1 mbar; charging N for 16min under the condition of heat preservation2Heating to 1800 ℃ at the speed of 1 ℃/min under the pressure maintaining condition, maintaining the pressure and preserving the heat for 5 hours, and naturally cooling to room temperature to prepare the AlN/SiC combined C composite material generated in situ.
Example 5
An in-situ generated AlN/SiC combined C composite material and a preparation method thereof.
Step 1, prefabrication of mixture
The mixture is as follows: first 90 wt% of Al4SiC4Mixing the powder with 10 wt% of material containing C to obtain premix; and mixing 96 wt% of the premix and 4 wt% of a binder to obtain a mixture.
Step 2, prefabricating a blank
The mixture is pre-pressed and formed under the condition of 60MPa, then is subjected to isostatic pressing and forming under the condition of 240MPa, and then is placed in a constant-temperature drying box and is dried for 2 hours under the condition of 110 ℃ to obtain a prefabricated blank body.
Step 3, in-situ generation of AlN/SiC combined C composite material
Putting the prefabricated blank into a graphite crucible, then putting the graphite crucible into a pneumatic sintering furnace, and heating the graphite crucible to 1200 ℃ from room temperature at the speed of 4 ℃/min under the condition that the pressure is less than or equal to 0.1 mbar; charging N for 10min under the condition of heat preservation2Heating to 1700 ℃ at the speed of 4 ℃/min under the pressure maintaining condition, maintaining the pressure and preserving the heat for 3h, and naturally cooling to room temperature to prepare the AlN/SiC combined C composite material generated in situ.
Example 6
An in-situ generated AlN/SiC combined C composite material and a preparation method thereof.
Step 1, prefabrication of mixture
The mixture is as follows: firstly 95 wt% of Al4SiC4Mixing the powder with 5 wt% of material containing C to obtain premix; and mixing 95 wt% of the premix and 5 wt% of a binder to obtain a mixture.
Step 2, prefabricating a blank
The mixture is pre-pressed and formed under the condition of 70MPa, then is subjected to isostatic pressing and forming under the condition of 160MPa, and then is placed in a constant-temperature drying box and is dried for 3 hours under the condition of 110 ℃ to obtain a prefabricated blank body.
Step 3, in-situ generation of AlN/SiC combined C composite material
Placing the prefabricated blank into a graphite crucible, then placing the graphite crucible into a gas pressure sintering furnace, and heating the graphite crucible to 1050 ℃ from room temperature at the speed of 7 ℃/min under the condition that the pressure is less than or equal to 0.1 mbar; charging N for 14min under the condition of heat preservation2Heating to 1800 ℃ at the speed of 3 ℃/min under the pressure maintaining condition, maintaining the pressure and preserving the heat for 2h, and naturally cooling to room temperature to prepare the AlN/SiC combined C composite material generated in situ.
Compared with the prior art, the specific implementation mode has the following advantages:
this embodiment uses a single Al4SiC4The powder is used as a raw material, and the raw material has excellent oxidation resistance and hydration resistance, so that the oxidation resistance of the AlN/SiC combined C composite material generated in situ can be obviously improved.
Al used in the present embodiment4SiC4The nitridation reaction can occur along with the increase of the sintering temperature, the generated AlN, SiC and C are uniformly distributed in the in-situ generated AlN/SiC combined C composite material, and as the evaporation and diffusion mass transfer rates of all phases in the C composite material are different, a honeycomb structure of AlN/SiC ceramic phase wrapping the C phase is gradually formed in the system; meanwhile, AlN and SiC have similarity in atomic size, molecular weight and crystal structure, so that the two phases are tightly combined without obvious interfaces; the C phase generated in situ is detected to be vermicular graphite, and the special structure of the C phase is used as a reinforcing phase to further improve the strength and the thermal shock resistance of the product. The prepared in-situ generated AlN/SiC combined C composite material has the advantages of uniform phase distribution, high strength and good thermal shock resistance.
The in-situ generated AlN/SiC-bonded C composite material prepared by the embodiment is shown in the attached drawings. FIG. 1 is an XRD pattern of an in situ grown AlN/SiC bonded C composite prepared in example 1. FIG. 2 is a BSE plot of a polished cross-section of the in-situ grown AlN/SiC-bonded C composite shown in FIG. 1. As can be seen from FIG. 1, Al in the article produced4SiC4The raw material is completely nitrided, and the product does not contain any impurity except AlN, SiC and C; as can be seen from FIG. 2, the phases of the prepared products are uniformly and tightly combined, and a honeycomb structure with AlN/SiC ceramic phase wrapping C phase is presented.
The embodiment adopts a gas pressure sintering method, which can not only promote the sintering of the product but also enable Al4SiC4And the prepared AlN/SiC combined C composite material generated in situ has the characteristics of low density and light weight.
Therefore, the in-situ generated AlN/SiC combined C composite material prepared by the embodiment has the advantages of low density, light weight, uniform phase distribution, high strength, good thermal shock resistance and excellent oxidation resistance.
Claims (5)
1. A preparation method for in-situ generation of an AlN/SiC combined C composite material is characterized by comprising the following steps:
step 1, prefabrication of mixture
The mixture is a mixture I or a mixture II;
the mixture I is as follows: 95 to 97 weight percent of Al4SiC4Mixing the powder with 3-5 wt% of a binder to obtain a mixture I;
the mixture II comprises: firstly, 85-95 wt% of Al4SiC4Mixing the powder with 5-15 wt% of a C-containing material to obtain a premix; mixing 95-97 wt% of the premix and 3-5 wt% of a binder to obtain a mixture II;
the Al is4SiC4The purity of the powder is more than or equal to 98.0 wt%, and Al4SiC4The particle size of the powder is less than or equal to 150 mu m;
step 2, prefabricating a blank
The mixture is pre-pressed and molded under the condition of 5-100 MPa, then is subjected to isostatic pressing under the condition of 50-300 MPa, and then is placed in a constant-temperature drying box and is dried for 1-5 hours under the condition of 110 ℃ to obtain a prefabricated blank body;
step 3, in-situ generation of AlN/SiC combined C composite material
Placing the prefabricated blank into a graphite crucible, then placing the graphite crucible into a pneumatic sintering furnace, and heating the graphite crucible to 1000-1200 ℃ from room temperature at the speed of 5-10 ℃/min under the condition that the pressure is less than or equal to 0.1 mbar; n is filled for 10-20 min under the condition of heat preservation2Heating to 1600-1800 ℃ at the speed of 1-5 ℃/min under the pressure maintaining condition, maintaining the pressure and keeping the temperature for 1-5 h, and naturally cooling to room temperature to prepare the AlN/SiC combined C composite material generated in situ.
2. The method of claim 1, wherein the C-containing material is at least one of graphite, coke, and carbon black.
3. The method of claim 1, wherein the binder is one or more of phenolic resin, epoxy resin, and pitch; the binder used for mix I was the same as the binder used for mix II.
4. The method of claim 1, wherein the nitrogen has a purity of at least 99.999%.
5. An in-situ generated AlN/SiC combined C composite material, characterized in that the in-situ generated AlN/SiC combined C composite material is an in-situ generated AlN/SiC combined C composite material prepared by the preparation method of the in-situ generated AlN/SiC combined C composite material according to any one of claims 1 to 4.
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