CN109516814B - Si3N4/SiC complex phase ceramic material and preparation method thereof - Google Patents

Si3N4/SiC complex phase ceramic material and preparation method thereof Download PDF

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CN109516814B
CN109516814B CN201811469392.0A CN201811469392A CN109516814B CN 109516814 B CN109516814 B CN 109516814B CN 201811469392 A CN201811469392 A CN 201811469392A CN 109516814 B CN109516814 B CN 109516814B
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曾宇平
梁汉琴
左开慧
夏咏锋
姚冬旭
尹金伟
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Jiangxi Zhongke Shangyu Technology Co.,Ltd.
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Shanghai Institute of Ceramics of CAS
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Abstract

The invention relates to Si3N4a/SiC complex phase ceramic material and a preparation method thereof, wherein Si is3N4the/SiC complex phase ceramic material is Si3N4And SiC as a raw material powder, Tm2O3And MgO as a sintering aid, and is prepared by hot-pressing sintering; the total mass of the raw material powder and the sintering aid is 100wt%, the content of SiC is 1-20 wt%, the content of the sintering aid is 6.94wt%, and the balance is Si3N4。

Description

Si3N4/SiC complex phase ceramic material and preparation method thereof
Technical Field
The invention relates to Si3N4A/SiC complex phase ceramic material and a preparation method thereof belong to the field of preparation of complex phase ceramics.
Background
The silicon nitride ceramic is an all-round ceramic material and has a plurality of excellent performances such as high strength, high toughness, high thermal conductivity, oxidation resistance, corrosion resistance, thermal shock resistance and the like. However, silicon nitride has strong covalent bonding properties and is therefore difficult to sinter. Hot press sintering is an effective method for preparing high performance structural ceramics, and densification of ceramic materials can be effectively promoted by applying axial pressure. However, the thermal conductivity of silicon nitride is anisotropic in character, i.e., the thermal conductivity along the a and b axes is low and the thermal conductivity along the c axis is high. During the hot press sintering, the growth of the c-axis of the silicon nitride ceramic crystal grains in the direction parallel to the hot press direction is inhibited due to the presence of the axial pressure, thereby resulting in a decrease in the thermal conductivity parallel to the hot press direction.
Disclosure of Invention
In view of the above problems, it is an object of the present invention to provide Si3N4a/SiC complex phase ceramic material and a preparation method thereof.
In one aspect, the present invention provides Si3N4a/SiC complex phase ceramic material, the Si3N4the/SiC complex phase ceramic material is Si3N4And SiC as a raw material powder, Tm2O3And MgO as a sintering aid, and is prepared by hot-pressing sintering;
the total mass of the raw material powder and the sintering aid is 100wt%, the content of SiC is 1-20 wt%, the content of the sintering aid is 6.94wt%, and the balance is Si3N4。
In the disclosure, silicon carbide is also a high-performance ceramic material, and has high thermal conductivity while having excellent mechanical properties, and the thermal conductivity has no obvious anisotropic characteristic. Because the silicon carbide particles are introduced into the silicon nitride ceramic matrix, the characteristic that the silicon carbide has higher thermal conductivity in all directions is utilized, the reduction of the thermal conductivity of the silicon nitride in the direction parallel to the hot pressing direction in the hot pressing sintering process is compensated, and the Si with higher thermal conductivity is prepared3N4the/SiC complex phase ceramic. On the other hand, because the silicon carbide has higher Vickers hardness, the introduction of the silicon carbide can improve Si3N4Hardness of the/SiC complex phase ceramic. The pinning of silicon carbide in a silicon nitride matrix also enhances Si3N4Fracture toughness of the/SiC complex phase ceramic. With Si3N4And SiC as a raw material powder, Tm2O3And MgO as a sintering aid (for example, 100wt% of the total mass of the raw material powder and the sintering aid, 1 to 20wt% of SiC, 6.94wt% of the sintering aid, and the balance of Si3N4) Preparing Si by hot-pressing sintering3N4the/SiC complex phase ceramic material. In summary, silicon carbide was introduced and Tm was used2O3And MgO as sintering aid, and is prepared by hot-pressing sinteringPreparing Si with high strength, high toughness and high thermal conductivity3N4the/SiC complex phase ceramic can effectively prepare Si with excellent comprehensive performance3N4the/SiC complex phase ceramic.
Preferably, Tm is in the sintering aid2O3The molar mass ratio of (1) to MgO is 2: 5. Namely, the Tm2O3Is 5.50 wt%, and the MgO content is 1.44 wt%.
Preferably, said Si3N4The thermal conductivity of the/SiC complex phase ceramic material is 50.2-72.8W/(m.K), the bending strength is 513.7-825.6 MPa, and the fracture toughness is 6.03-8.54 MPa.m1/2The Vickers hardness is 15.3-18.7 GPa.
On the other hand, the invention also provides the Si3N4The preparation method of the/SiC complex phase ceramic material comprises the following steps: selecting Si3N4Powder, SiC powder, Tm2O3Mixing and pressing the powder and MgO powder serving as initial raw materials to obtain a biscuit;
placing the obtained element body in a nitrogen atmosphere, and carrying out hot-pressing sintering at the temperature of 1700-1800 ℃ under the pressure of 20-60MPa for 120-240 minutes to obtain the Si3N4the/SiC complex phase ceramic material.
Preferably, said Si3N4The powder is alpha-Si3N4And (3) powder.
Preferably, the mixing mode is ball milling mixing; the ball milling mixing comprises: preparing the initial raw materials into slurry with solid content of 50wt%, and taking Si3N4The ball is used as a grinding medium, the ball milling speed is 200-400 rpm, the ball milling mode is that the ball milling device rotates clockwise and anticlockwise alternately for half an hour, and the total ball milling time is 3-6 hours.
Preferably, after ball milling and mixing, drying, grinding and sieving are carried out, wherein the sieving mesh number is 100-400 meshes.
Preferably, the compression molding mode is dry compression molding, and the pressure of the dry compression molding is 5MPa to 20 MPa.
The present invention uses Tm2O3And MgO as a sintering aid, by addingSintering the SiC powder with the same content for 240min at the temperature of 1700-1800 ℃ under the pressure of 20-60MPa to obtain Si with high thermal conductivity, high strength and high toughness3N4The thermal conductivity of the/SiC complex phase ceramic is 50.2-72.8W/(m.K), the bending strength is 513.7-825.6 MPa, and the fracture toughness is 6.03-8.54 MPa.m1/2The Vickers hardness is 15.3-18.7 GPa, and the comprehensive performance is excellent.
Compared with the prior art, the invention has the beneficial effects that: by adding SiC powder, the high thermal conductivity and isotropy of SiC can be utilized to compensate for Si in the hot pressing sintering process3N4The heat conductivity in the direction parallel to the hot pressing direction is insufficient, the fracture toughness and the Vickers hardness are improved simultaneously, and Si with excellent comprehensive performance is obtained3N4the/SiC complex phase ceramic.
Drawings
FIG. 1 shows Si with SiC powder content of 1 wt% at 1700 ℃/60MPa/2h in example 13N4The section microstructure topography of the/SiC complex phase ceramic;
FIG. 2 shows Si with SiC powder content of 1 wt% at 1800 ℃/60MPa/4h in example 23N4The section microstructure topography of the/SiC complex phase ceramic;
FIG. 3 shows Si with SiC powder content of 2 wt% at 1700 ℃/60MPa/2h in example 33N4A polished surface microstructure topography of the/SiC complex phase ceramic;
FIG. 4 shows Si with SiC powder content of 10 wt% at 1750 ℃/60MPa/2h3N4Phase analysis diagram of/SiC complex phase ceramic.
Detailed Description
The present invention is further illustrated by the following examples, which are to be understood as merely illustrative and not restrictive.
In the present disclosure, Si is selected3N4And SiC as the main phase, Tm being selected2O3And MgO as sintering aid to prepare Si with high heat conductivity3N4The thermal conductivity of the SiC complex phase ceramic material is higher than 50W/(m.K), and the fracture toughness is higher than 6.0 MPa.m1/2. Wherein the total mass of the raw material powder (main phase) and the sintering aid is 100wt%, the content of SiC can be 1-20 wt%, the content of the sintering aid can be 6.94wt%, and the balance is Si3N4. Wherein, Tm is2O3The molar mass ratio of (1) to MgO may be 2: 5. I.e., Tm2O3Is 5.50 wt%, and the MgO content is 1.44 wt%.
The following exemplary illustrations of Si provided by the present invention3N4A preparation method of a/SiC complex phase ceramic material.
Selecting Si3N4Powder, SiC powder, Tm2O3The powder and MgO powder are used as initial raw materials and are mixed to obtain mixed powder. Wherein, Si3N4The powder is alpha-Si3N4And (3) powder. Wherein, the mixing mode can be ball milling mixing. The ball milling and mixing comprises the following steps: preparing the initial raw materials into slurry with solid content of 50wt%, and taking Si3N4The ball is used as a grinding medium, the ball milling speed is 200-400 rpm, the ball milling mode is that the ball milling device alternately rotates clockwise and anticlockwise for half an hour, and the total ball milling time can be 3-6 hours. Preferably, after ball milling and mixing, the slurry is dried (dried), ground and sieved to obtain mixed powder. Wherein the number of the sieving meshes can be 100-400 meshes. In an alternative embodiment, Si3N4The particle size of the powder can be 0.3-0.8 μm. The grain diameter of the SiC powder can be 0.3nm-0.8 μm. Tm is2O3The particle size of the powder can be 1.0-5.0 μm. The particle size of the MgO powder can be 0.1 μm to 0.3. mu.m.
And pressing and molding the mixed powder to obtain a ceramic biscuit (biscuit). Wherein, the pressing and forming mode can be dry pressing and forming. The pressure of the dry pressing molding can be 5MPa to 20 MPa.
Placing the element body in a graphite hot-pressing mold, placing the element body in a sintering furnace, carrying out hot-pressing sintering for 120-240 minutes at 20-60MPa and at the temperature of 1700-1800 ℃ in the nitrogen atmosphere, and then cooling the element body along with the furnace to obtain the Si3N4the/SiC complex phase ceramic material.
In the present invention, Si is measured by using a laser thermal conductivity meter (LFA427)3N4Parallel heat of/SiC complex phase ceramic materialThe thermal conductivity in the pressing direction can be 50.2-72.8W/(m.K). Si measurement Using Universal tester (INSTRON-1195)3N4The bending strength of the/SiC complex phase ceramic material can be 513.7-825.6 MPa. Si measurement with a Vickers hardness tester (TUKON-2100B)3N4The fracture toughness of the/SiC complex phase ceramic material can be 6.03-8.54 MPa-m1/2. Si measurement with a Vickers hardness tester (TUKON-2100B)3N4The Vickers hardness of the/SiC complex phase ceramic material can be 15.3-18.7 GPa.
The present invention will be described in detail by way of examples. It is also to be understood that the following examples are illustrative of the present invention and are not to be construed as limiting the scope of the invention, and that certain insubstantial modifications and adaptations of the invention by those skilled in the art may be made in light of the above teachings. The specific process parameters and the like of the following examples are also only one example of suitable ranges, i.e., those skilled in the art can select the appropriate ranges through the description herein, and are not limited to the specific values exemplified below. In the following examples, unless otherwise specified, Si3N4The particle size of the powder can be 0.3-0.8 μm. The grain diameter of the SiC powder can be 0.3nm-0.8 μm. Tm is2O3The particle size of the powder can be 1.0-5.0 μm. The particle size of the MgO powder can be 0.1 μm to 0.3. mu.m.
Example 1
Hot-pressed sintered Si3N4The preparation method of the/SiC complex phase ceramic comprises the following steps:
s1 weighing 92.06g of Si3N4，1.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 6 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 200 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 100-mesh sieve, and performing dry pressing preforming (dry pressing forming) under the pressure of 5 MPa;
s4, placing the ceramic biscuit (biscuit) obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1700 deg.C under 60MPa for 120 min to obtain the final product with relative density of 98.5%, bending strength of 747.5 + -45.5 MPa, and fracture toughness of 7.85 + -0.25 MPa-m1/2The Vickers hardness is 15.45 +/-0.14 GPa, and the thermal conductivity is 56.3 w/(m.k) of Si3N4the/SiC complex phase ceramic.
For Si obtained in example 13N4The fracture morphology of the/SiC complex phase ceramic is observed, the result is shown in figure 1, and no obvious pore exists in the sample, which shows that the densification can be realized by adding 1 wt% of SiC powder under the condition of hot-pressing sintering.
Example 2
Hot-pressed sintered Si3N4The preparation method of the/SiC complex phase ceramic comprises the following steps:
s1 weighing 92.06g of Si3N4，1.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 4 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 300 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 100-mesh sieve, and performing dry pressing preforming under the pressure of 5 MPa;
s4, placing the ceramic biscuit obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1800 deg.C and 60MPa for 240min to obtain the final product with relative density of 99.2%, bending strength of 799.3 + -26.3 MPa and fracture toughness of 8.32 + -0.22 MPa-m1/2The Vickers hardness is 15.53 +/-0.23 GPa, and the thermal conductivity is 72.8W/(m.k) of Si3N4the/SiC complex phase ceramic.
For the hot-pressed sintered Si obtained in example 23N4/SiC complex phase ceramicThe fracture morphology of (A) was observed, and the results are shown in FIG. 2, and no obvious pores are still present in the sample, which indicates that Si is added with 1 wt% of SiC3N4the/SiC complex phase ceramic is highly compact. In addition, as can be seen from the figure, the longer holding time in this example makes the crystal grain size larger and the thermal conductivity is improved accordingly, compared to example 1.
Example 3
Hot-pressed sintered Si3N4The preparation method of the/SiC complex phase ceramic comprises the following steps:
s1 weighing 91.06g Si3N4，2.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 5 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 350 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 200-mesh sieve, and performing dry pressing preforming under the pressure of 10 MPa;
s4, placing the ceramic biscuit (biscuit) obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1700 deg.C under 60MPa for 120 min to obtain the final product with relative density of 98.6%, bending strength of 733.8 + -65.5 MPa, and fracture toughness of 7.56 + -0.08 MPa-m1/2Si with Vickers hardness of 15.97 +/-0.23 GPa and thermal conductivity of 53.4W/(m.k)3N4the/SiC complex phase ceramic.
For Si obtained in example 33N4The polished surface morphology of the/SiC complex phase ceramic is observed, and the result is shown in figure 3, and no obvious pore exists in the sample, which shows that under the condition of hot-pressing sintering, the densification can be realized by adding 2 wt% of SiC powder.
Example 4
Hot-pressed sintered Si3N4The preparation method of the/SiC complex phase ceramic comprises the following steps:
s1 weighing 90.06g of Si3N4，3.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 4 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 300 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 400-mesh sieve, and performing dry pressing preforming under the pressure of 15 MPa;
s4, placing the ceramic biscuit obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1800 deg.C and 30MPa for 240min to obtain the final product with relative density of 99.1%, bending strength of 763.9 + -49.0 MPa, and fracture toughness of 7.17 + -0.40 MPa-m1/2Si with Vickers hardness of 16.21 +/-0.16 GPa and thermal conductivity of 66.1W/(m.k)3N4the/SiC complex phase ceramic.
Example 5
Hot-pressed sintered Si3N4The preparation method of the/SiC complex phase ceramic comprises the following steps:
s1 weighing 89.06g of Si3N4，4.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 2 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 400 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 100-mesh sieve, and performing dry pressing preforming under the pressure of 20 MPa;
s4, placing the ceramic biscuit obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1800 deg.C and 40MPa for 180 min to obtain the final product with relative density of 99.1% and bending strength of 658.7 + -4.7MPa, and fracture toughness of 7.01 +/-0.09 MPa.m1/2Si with Vickers hardness of 16.24 +/-0.00 GPa and thermal conductivity of 65.3 w/(m.k)3N4the/SiC complex phase ceramic.
Example 6
Hot-pressed sintered Si3N4The preparation method of the/SiC complex phase ceramic comprises the following steps:
s1 weighing 88.06g of Si3N4，5.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 4 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 250 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 200-mesh sieve, and performing dry pressing preforming under the pressure of 20 MPa;
s4, placing the ceramic biscuit obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1800 deg.C and 60MPa for 180 min to obtain the final product with relative density of 99.0%, bending strength of 584.9 + -12.5 MPa, and fracture toughness of 6.61 + -0.51 MPa.m1/2Si with Vickers hardness of 17.09 +/-1.65 GPa and thermal conductivity of 56.8W/(m.k)3N4the/SiC complex phase ceramic.
Example 7
Hot-pressed sintered Si3N4The preparation method of the/SiC complex phase ceramic comprises the following steps:
s1 weighing 83.06g Si3N4，10.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 5 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 350 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 200-mesh sieve, and performing dry pressing preforming under the pressure of 10 MPa;
s4, placing the ceramic biscuit obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1750 deg.C and 60MPa for 120 min to obtain final product with relative density of 98.8%, bending strength of 560.5 + -24.3 MPa, and fracture toughness of 6.43 + -0.23 MPa-m1/2Si with Vickers hardness of 17.29 +/-0.09 GPa and thermal conductivity of 51.8W/(m.k)3N4the/SiC complex phase ceramic.
Si obtained in example 73N4The phase of the/SiC complex phase ceramic is analyzed, and the result is shown in figure 4, wherein the main phase in the sample is beta-Si3N4Alpha phase, Si during sintering is not specified3N4The transition from the alpha phase to the beta phase is relatively complete. The second phase in the sample was 6H-SiC.
Example 8
Hot-pressed sintered Si3N4The preparation method of the/SiC complex phase ceramic comprises the following steps:
s1 weighing 78.06g of Si3N4，15.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 6 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 300 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 400-mesh sieve, and performing dry pressing preforming under the pressure of 20 MPa;
s4, placing the ceramic biscuit obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1700 deg.C under 60MPa for 120 min to obtain the final product with relative density of 98.2%, bending strength of 557.5 + -19.7 MPa and fracture toughness of 6.31 + -0.22 MPa-m1/2The Vickers hardness is 17.82 +/-0.18 GPa, and the thermal conductivity is 50.2W/(m.k)) Si of (2)3N4the/SiC complex phase ceramic.
Example 9
Hot-pressed sintered Si3N4The preparation method of the/SiC complex phase ceramic comprises the following steps:
s1 weighing 73.06g of Si3N4，20.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 4 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 400 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 200-mesh sieve, and performing dry pressing preforming under the pressure of 10 MPa;
s4, placing the ceramic biscuit (biscuit) obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1750 deg.C and 30MPa for 240min to obtain the final product with relative density of 98.7%, bending strength of 529.3 + -15.6 MPa, and fracture toughness of 6.21 + -0.20 MPa-m1/2Si with Vickers hardness of 18.51 +/-0.19 GPa and thermal conductivity of 53.2W/(m.k)3N4the/SiC complex phase ceramic.
Comparative example 1
Hot-pressed sintered Si3N4The ceramic and the preparation method thereof comprise the following steps:
s1 weighing 93.06g Si3N4，0.0g SiC，5.50g Tm2O3And 1.44g MgO for a total of 100 g;
s2 adding 100g of alcohol as a solvent and 100g of Si to the mixed powder obtained in the step S13N4The balls are ball milling media, and are subjected to planetary ball milling for 6 hours in a mode of alternately rotating anticlockwise and clockwise for half an hour, and the rotating speed is 200 rpm;
s3, placing the slurry obtained in the step S2 in an oven, setting the temperature of the oven at 80 ℃, drying for 24 hours, grinding, sieving by a 100-mesh sieve, and performing dry pressing preforming under the pressure of 5 MPa;
s4, placing the ceramic biscuit (biscuit) obtained in the step S3 into a graphite hot-pressing die, placing the sample into a carbon tube furnace, and filling N2Sintering at 1700 deg.C under 60MPa for 120 min to obtain the final product with relative density of 98.1%, bending strength of 741.5 + -35.3 MPa, and fracture toughness of 5.98 + -0.11 MPa-m1/2The Vickers hardness is 14.62 +/-0.13 GPa, and the thermal conductivity is 48.9 w/(m.k) of Si3N4A ceramic.
Table 1 shows the composition and preparation parameters of the Si3N4/SiC composite ceramic material prepared in examples 1-9:
Si3N4/g SiC/g Tm2O3/g MgO/g sintering pressure/MPa Temperature/. degree.C Time/min
Example 1 92.06 1.0 5.50 1.44 60 1700 120
Example 2 92.06 1.0 5.50 1.44 60 1800 240
Example 3 91.06 2.0 5.50 1.44 60 1700 120
Example 4 90.06 3.0 5.50 1.44 30 1800 240
Example 5 89.06 4.0 5.50 1.44 40 1800 180
Example 6 88.06 5.0 5.50 1.44 60 1800 180
Example 7 83.06 10.0 5.50 1.44 60 1750 120
Example 8 78.06 15.0 5.50 1.44 60 1700 120
Example 9 73.06 20.0 5.50 1.44 30 1750 240
Comparative example 1 93.06 0.0 5.50 1.44 60 1700 120
Table 2 shows Si prepared in examples 1 to 93N4The performance parameters of the SiC complex phase ceramic material are as follows:
Figure BDA0001890562010000081
Figure BDA0001890562010000091
as can be seen from the above examples, the present invention is achieved by adding Si3N4Adding SiC particles to the matrix at Tm2O3And MgO as sintering aid, and Si with high strength, high toughness, high hardness and high thermal conductivity can be obtained by adopting a hot-pressing sintering mode3N4the/SiC complex phase ceramic realizes the adjustability.
Finally, it is necessary to mention that: the above embodiments are only used for further detailed description of the technical solutions of the present invention, and should not be understood as limiting the scope of the present invention, and the insubstantial modifications and adaptations made by those skilled in the art according to the above descriptions of the present invention are within the scope of the present invention.

Claims (6)

1. Si3N4the/SiC complex phase ceramic material is characterized in that the Si is3N4the/SiC complex phase ceramic material is Si3N4And SiC as a raw material powder, Tm2O3And MgO as sintering aid, and hot-pressed sintering is carried out for 120-240 minutes at 20-60MPa and 1700-1800 ℃ in nitrogen atmospherePreparing to obtain; the grain diameter of SiC is 0.3nm-0.8 μm;
the total mass of the raw material powder and the sintering aid is 100wt%, the content of SiC is 1-5 wt%, the content of the sintering aid is 6.94wt%, and the balance is Si3N4(ii) a Tm in the sintering aid2O3And MgO in a molar ratio of 2: 5;
said Si3N4The thermal conductivity of the/SiC complex phase ceramic material is 53.4-72.8W/(m.K), the bending strength is 572.4-825.6 MPa, and the fracture toughness is 6.1-8.54 MPa.m1/2The Vickers hardness is 15.3-18.7 GPa.
2. Si according to claim 13N4The preparation method of the/SiC complex phase ceramic material is characterized by comprising the following steps:
selecting Si3N4Powder, SiC powder, Tm2O3Mixing and pressing the powder and MgO powder serving as initial raw materials to obtain a biscuit;
placing the obtained biscuit in a nitrogen atmosphere, and carrying out hot-pressing sintering at the temperature of 1700-1800 ℃ under the pressure of 20-60MPa for 120-240 minutes to obtain the Si3N4the/SiC complex phase ceramic material.
3. The production method according to claim 2, wherein the Si is3N4The powder is alpha-Si3N4And (3) powder.
4. The method according to claim 2, wherein the mixing is performed by ball milling; the ball milling mixing comprises: preparing the initial raw materials into slurry with solid content of 50wt%, and taking Si3N4The ball is used as a grinding medium, the ball milling speed is 200-400 rpm, the ball milling mode is that the ball milling device rotates clockwise and anticlockwise alternately for half an hour, and the total ball milling time is 3-6 hours.
5. The preparation method according to claim 4, wherein the ball milling and mixing are followed by drying, grinding and sieving, and the sieving mesh number is 100-400 meshes.
6. The production method according to any one of claims 2 to 5, wherein the press molding is dry press molding, and the pressure of the dry press molding is 5MPa to 20 MPa.
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