CN114478043A - Connection method of silicon carbide ceramic based on liquid phase sintering - Google Patents
Connection method of silicon carbide ceramic based on liquid phase sintering Download PDFInfo
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- CN114478043A CN114478043A CN202210033547.6A CN202210033547A CN114478043A CN 114478043 A CN114478043 A CN 114478043A CN 202210033547 A CN202210033547 A CN 202210033547A CN 114478043 A CN114478043 A CN 114478043A
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- C04B37/00—Joining burned ceramic articles with other burned ceramic articles or other articles by heating
- C04B37/003—Joining burned ceramic articles with other burned ceramic articles or other articles by heating by means of an interlayer consisting of a combination of materials selected from glass, or ceramic material with metals, metal oxides or metal salts
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2237/00—Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
- C04B2237/02—Aspects relating to interlayers, e.g. used to join ceramic articles with other articles by heating
- C04B2237/04—Ceramic interlayers
- C04B2237/08—Non-oxidic interlayers
- C04B2237/083—Carbide interlayers, e.g. silicon carbide interlayers
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
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Abstract
The invention relates to a method for connecting silicon carbide ceramics based on liquid phase sintering, which comprises the following steps: (1) mixing silicon carbide powder, a sintering aid, a dispersing agent, a binder and a solvent to obtain suspension slurry; the sintering aid is AlN powder and Y2O3Pulverizing; (2) uniformly spreading the obtained suspension slurry on the surface to be connected of the first silicon carbide ceramic to obtain a slurry layer, attaching the surface to be connected of the second silicon carbide ceramic to the slurry layer, fixing the surface to be connected of the second silicon carbide ceramic by using a clamp, and finally realizing the connection of the silicon carbide ceramic in a normal-pressure sintering furnace; preferably, the temperature of the liquid phase sintering is 1600-2000 ℃, the heat preservation time is 0.5-5 hours, and the atmosphere is inert atmosphere, more preferably argon; wherein the pressure applied by the clamp is 1-10 MPa.
Description
Technical Field
The invention relates to a silicon carbide ceramic connection method based on a liquid phase sintering technology, wherein a connection layer is a silicon carbide component, and the silicon carbide ceramic connection method has the advantages of low connection interface stress, strong acid corrosion resistance, excellent high-temperature mechanics and the like, and belongs to the field of ceramic connection.
Background
The silicon carbide ceramic is a structural material with excellent performance, has good high-temperature mechanical property, high thermal conductivity, low density and thermal expansion coefficient, excellent wear resistance, corrosion resistance and other properties, and is widely applied to the fields of aerospace, chemical engineering, electronics, transportation, nuclear energy and the like. However, the high brittleness, high hardness, and difficult post-processing of silicon carbide ceramic limit further applications in these fields. One effective solution is to use ceramic joining techniques, i.e., ceramic parts of relatively simple shape or relatively small size are first prepared and then physically or chemically joined to the desired size and shape.
In the existing silicon carbide ceramic connection technology, the silicon carbide ceramic connection technology can be divided into a metal connection layer, a glass connection layer and a ceramic connection layer according to different intermediate layer material systems. In the metal connecting layer, huge physical and chemical property difference exists between the base material and the solder, so that the reliability of the joint can be reduced to a certain extent, and the application range and the application field of the silicon carbide ceramic are greatly limited. The glass connecting layer can generate crystallization phenomenon after being used for a long time, and has poor hot corrosion resistance and high temperature resistance. The performance of the ceramic connecting layer is matched with that of the base material, and the residual stress is the lowest. However, ceramic bond coats are typically constructed primarily by reactive bonding techniques, and the amount and distribution of residual silicon in the resulting bond coat affects bond strength and service temperature.
Disclosure of Invention
In order to solve the defects of the technology, the invention aims to provide a method for realizing the connection of silicon carbide ceramics based on a liquid phase sintering technology, and the silicon carbide ceramics connected by the method can resist the corrosion of concentrated sulfuric acid and concentrated nitric acid and have excellent high-temperature mechanical properties.
In one aspect, the present invention provides a method for joining silicon carbide ceramics based on liquid phase sintering, comprising:
(1) mixing silicon carbide powder, a sintering aid, a dispersing agent, a binder and a solvent to obtain suspension slurry; the sintering aid is AlN powder and Y2O3Pulverizing;
(2) uniformly spreading the obtained suspension slurry on the surface to be connected of the first silicon carbide ceramic to obtain a slurry layer, attaching the surface to be connected of the second silicon carbide ceramic to the slurry layer and fixing the surface to be connected of the second silicon carbide ceramic by using a clamp, so that the two silicon carbide ceramics to be connected are in close contact with each other, and finally, the connection of the silicon carbide ceramics is realized in a normal-pressure sintering furnace; preferably, the temperature of the liquid phase sintering is 1600-2000 ℃, the heat preservation time is 0.5-5 hours, and the atmosphere is inert atmosphere, more preferably argon; wherein the pressure applied by the clamp is 1-10 MPa.
Preferably, the purity of the silicon carbide powder is more than or equal to 99%, the oxygen content is less than 1%, and the particle size is 0.1-1 μm;
the AlN powder has the purity of more than or equal to 99 percent and the particle size of 0.1-1 mu m;
said Y is2O3The purity of the powder is more than or equal to 99 percent, and the particle size is 0.5-5 mu m.
Preferably, the mass ratio of the SiC to the sintering aid is (95-85): (5-15); preferably, AlN and Y are contained in the sintering aid2O3The mass ratio of (1): (0.1 to 10), more preferably 1: 4;
preferably, the solvent is absolute ethyl alcohol or/and acetone; the dispersant is castor oil phosphate and/or castor oil; the binder is polyvinyl butyral and/or phenolic resin.
Preferably, the solid content of the suspension slurry is 40-60 wt%;
the dispersing agent accounts for 3-8% of the total mass of the powder;
the binder accounts for 1-5% of the total mass of the powder.
Preferably, the mixing mode is ball milling mixing; the rotation speed of ball milling mixing is 200-300 r/min, and the ball milling time is 12-24 hours;
the viscosity of the suspension slurry at a shear rate of 20/S is 200-1000 mPa & S.
Preferably, the spreading mode is centrifugal spin coating or screen printing;
the centrifugal spin coating speed is 1000-1500 rpm, and the time is 0.5-1 min;
the screen mesh number of the screen printing is 200-325 meshes;
the thickness of the slurry layer (solder layer) prepared by centrifugal spin coating or screen printing is 50-150 μm.
Preferably, the surface to be joined of the first silicon carbide ceramic and the surface to be joined of the second silicon carbide ceramic are subjected to surface grinding treatment to ensure a roughness Ra of less than 0.5 μm before spreading the slurry.
In another aspect, the present invention provides a silicon carbide ceramic connecting member prepared according to the above connecting method of a silicon carbide ceramic based on liquid phase sintering, the connecting strength of the silicon carbide ceramic connecting member at room temperature being 200 to 300MPa, and the bending strength at 1400 ℃ being 100 to 150 MPa; the connecting layer of the silicon carbide ceramic connecting piece is subjected to corrosion of concentrated sulfuric acid for 48 hours and corrosion of concentrated nitric acid for 48 hours without change.
On the other hand, the invention also provides application of the silicon carbide ceramic connecting piece in the fields of pharmaceutical chemicals and nuclear energy in extreme service environments.
Has the advantages that:
in the invention, the connection of SiC ceramics is realized based on a liquid phase sintering technology, and a normal pressure sintering furnace is used for the first time, which is beneficial to realizing the connection of SiC ceramics with complex shapes and large sizes; the obtained connecting layer is compact and has no hole defects. Because the connecting layer is mainly of SiC phase and basically consistent with the base material in property, huge interface welding stress caused by mismatching of the base material and the connecting layer due to thermal expansion coefficients can be effectively relieved. Because the intermediate layer is a SiC phase, the excellent performances of corrosion resistance, high temperature resistance, wear resistance and the like of the silicon carbide ceramic can be fully exerted, and the application field and the application range of the silicon carbide ceramic can be greatly widened. The invention can realize connection by fixing through a simple graphite clamp, can realize connection of large-size SiC ceramics, and is more beneficial to industrial application.
Drawings
FIG. 1 is an SEM image of a typical silicon carbide joint as embodied by this patent;
FIG. 2 is an SEM photograph of a silicon carbide joint obtained in example 1 by holding 1900 ℃ for 1h in a pressureless sintering furnace;
FIG. 3 is a photograph of a silicon carbide joint obtained in example 1 after etching in concentrated sulfuric acid for 48 hours;
FIG. 4 is a photograph of a silicon carbide joint obtained in example 1 after 48 hours of etching in concentrated nitric acid;
FIG. 5 is a graph of a successfully unconnected silicon carbide ceramic assembled without the use of a graphite jig in comparative example 1;
FIG. 6 is a graph showing cracks appearing on the surface of the SiC ceramic in comparative example 2 after applying a pressure of 20MPa to the ceramic;
FIG. 7 shows that the slurry of comparative example 3 has too low a solid content and voids appear in the connecting layer;
FIG. 8 shows that the slurry of comparative example 4 has too high a solid content and the slurry is not uniformly applied to the surface.
Detailed Description
The present invention is further illustrated by the following examples, which are to be understood as merely illustrative and not restrictive.
The invention discloses suspension slurry for realizing high-strength connection of silicon carbide ceramics. According to the invention, an aluminum nitride-yttrium oxide system is selected for ceramic connection for the first time, compared with the method of single liquid phase sintering ceramic densification, the connection layer densification is realized, and the problem of a connection interface between the connection layer and a silicon carbide ceramic base material is also considered, and compared with the aluminum nitride-yttrium oxide system, the aluminum nitride-yttrium oxide system has better connection performance.
The suspended slurry mainly comprises the following components: solvent, dispersant, binder, silicon carbide powder and sintering aid. Preferably, the above substances are mixed with a ball milling medium and subjected to ball milling treatment to obtain a suspension slurry. More preferably, the ball milling time is 12-24 h, and the rotating speed is 200-300 r/min.
Wherein, the solvent can be absolute ethyl alcohol or/and acetone. The solid content in the suspension slurry is 40-60% by mass. According to the invention, the solid content of the slurry is regulated and controlled, so that the viscosity of the slurry can reach the viscosity capable of performing centrifugal spin coating or screen printing on the ceramic surface. If the solid content is too high: the paste viscosity is too high for centrifugal spin coating or screen printing. If the solid content is too low: the connection interface is perforated, resulting in a decrease in connection strength.
Wherein, the dispersant can be castor oil and/or castor oil phosphate; preferably, the dispersant is castor oil phosphate, and the dispersibility of the castor oil phosphate is better than that of castor oil; the mass fraction of the dispersant can be 3-8%. The invention can adjust the kind and content of the dispersant to optimize the dispersion effect of the slurry.
Wherein, the binder can be polyvinyl butyral and/or phenolic resin, and the mass fraction can be 1-5%. Preferably, the binder is polyvinyl butyral, and the mass fraction of the binder can be 1-5%. Preferably, the viscosity of the slurry is controlled to be 200 to 1000mPa.S (when the shear rate is 20/S). The invention controls the viscosity of the slurry so that the slurry is uniformly dispersed and can be centrifugally spin-coated or screen-printed on the surface of the ceramic. If the viscosity is too high: the slurry cannot be uniformly dispersed and cannot be centrifugally spin-coated or screen-printed. If the viscosity is too low: the connection interface is perforated, resulting in a decrease in connection strength.
In an optional embodiment, the purity of the silicon carbide powder is greater than or equal to 99%, the particle size is 0.1-1 μm, and the oxygen content is less than 1%. The sintering aid can be AlN-Y2O3(ii) a Wherein the AlN purity is more than or equal to 99 percent, and the grain diameter is 0.1-1 mu m; y is2O3The purity is more than or equal to 99 percent, and the grain diameter is 0.5-5 mu m. The SiC: (AlN + Y)2O3) The mass ratio of (95-85): (5-15). AlN and Y are preferred2O3The mass ratio is 1: (0.1 to 10), preferably 1: 4. if the ratio of the two is too high or too low, the liquid phase distribution during sintering is not uniform, and the bonding effect is reduced. In addition, the ratio between aluminum nitride and yttrium oxide is selected from 1: 4, the joint is comprehensively optimized on the basis of a large number of tests, and the joint prepared according to the proportion has the highest connection strength and the best strong acid corrosion resistance.
In the invention, suspension slurry containing ceramic powder and liquid phase sintering aid is coated on the surface of connected ceramics, and a compact connecting layer is generated by utilizing the liquid phase sintering principle and simultaneously the base materials are connected into a whole. The following exemplarily illustrates a method for realizing silicon carbide ceramic connection by using the above-mentioned suspension slurry.
And uniformly coating the suspension slurry on the surfaces of two pieces of SiC ceramics subjected to surface treatment, fixing by using a C-C clamp, placing in a normal pressure sintering furnace, and connecting at 1600-2000 ℃ under the protection of argon. The invention adopts optimized connection layer component design and reasonable connection process, and can meet the use requirement only by one-step sintering without secondary auxiliary process. The coating method is centrifugal spin coating or screen printing, preferably, the speed of the centrifugal spin coating is 1000-1500 rpm, the time is 0.5-1 min, and the thickness of the finally obtained spin coating slurry layer can be 50-150 μm. The screen mesh number of the screen printing is 200-325 meshes, and the thickness of the obtained slurry layer (solder layer) is 50-150 μm. In this case, the thicker the slurry layer is, the lower the bonding strength is, and the thinner the bonding layer is, the less the bonding strength is.
In order to achieve a good bonding effect, the surface roughness Ra of the SiC ceramics to be bonded should be low, preferably Ra 0.5 μm.
In alternative embodiments, the protective atmosphere may be an inert gas such as argon. The heat preservation time can be 0.1-5 h.
The bending strength of the silicon carbide ceramic connecting joint realized by the invention at room temperature reaches 200-300 MPa, and the bending strength at high temperature of 1400 ℃ reaches 100-150 MPa. The steel is subjected to corrosion by concentrated sulfuric acid (98 wt%) and concentrated nitric acid (98 wt%) for 48h without change. The four-point bending strength of the steel is in accordance with the national standard (GB/T6569-2006/ISO14704:2000), and the bending strength is higher than the shearing strength value.
The invention provides the application of the silicon carbide ceramic connected based on the liquid phase sintering technology, and the silicon carbide ceramic can be applied to the fields of pharmaceutical chemicals, nuclear energy and the like in extreme service environments.
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.
Example 1
1) Preparing slurry: adding SiC balls, absolute ethyl alcohol, castor oil phosphate, polyvinyl butyral and mixed powder (SiC, AlN and Y) into a ball milling tank in sequence2O3) Ball milling is carried out, the rotating speed is controlled to be 300 r/min, hourThe time is 12h, the ball-material ratio is 1: 1. wherein the mass fraction of the castor oil phosphate is 5.5%, the mass fraction of the polyvinyl butyral ester is 2.5%, the solid content is 50%, and the viscosity of the slurry is 800mPa.s (when the shear rate is 20/S). SiC: AlN: y is2O3The mass ratio of (A) to (B) is 90: 2: 8. d of SiC powder500.35 μm, D of AlN500.18 μm, Y2O3Median particle diameter D of504.87 μm;
2) the connection process comprises the following steps: and coating slurry on the SiC ceramics with the surfaces treated by the grinding machine by using a rotary coating instrument, controlling the thickness of the slurry layer to be 100 mu m, and assembling by using a graphite clamp with the pressure of 5 MPa. And then the connection is carried out in a pressureless sintering furnace. The specific process parameters are as follows: heating to 1400 deg.C at 10 deg.C/min, heating to 1900 deg.C at 5 deg.C/min, and maintaining for 1h in argon atmosphere;
3) the connection effect is as follows: observing the microstructure of the joint by using a scanning electron microscope, wherein the thickness of the connecting layer is about 60 mu m as shown in FIG. 2, and the connecting layer is mainly an SiC phase and is found to have the connecting strength of 224MPa by energy spectrum surface scanning; the strength is 213MPa at 1400 ℃, the corrosion rate is consistent with that of the parent metal in concentrated sulfuric acid corrosion for 48 hours, the microstructure is shown in figure 3, no obvious change is caused before corrosion, and the strength is 200 MPa; after 48h of concentrated nitric acid etching, the microstructure of the alloy is shown in FIG. 4, and the alloy has no obvious change from that before etching and has the strength of 187 MPa. The corroded joint still has high strength.
Example 2
1) Preparing slurry: similar to embodiment 1, the differences are: wherein the solid content is 50%, the ball milling time of the slurry is 24h, and the viscosity of the slurry is 630mPa.s (when the shear rate is 20/S);
2) the connection process comprises the following steps: similar to example 1, except that the maximum temperature was 1700 ℃ and the holding time was 2 hours;
3) connection performance: the joint after connection in this embodiment has a connection strength of 150MPa at normal temperature and a connection strength of 100MPa at a high temperature of 1400 ℃.
Example 3
1) Preparing slurry: similarly to embodiment 1, except that in which SiC: AlN:Y2O3the mass ratio of (A) to (B) is 95: 1: 4;
2) the connection process comprises the following steps: similar to example 1, except that the maximum temperature was 1800 ℃ and the holding time was 0.5 h;
3) connection performance: the joint after connection of this embodiment had a connection strength of 197MPa at normal temperature and 167MPa at a high temperature of 1400 ℃. After the concentrated sulfuric acid is corroded for 72 hours, the connection strength is 170 MPa; after being corroded for 72 hours by concentrated nitric acid, the connection strength is 150 MPa.
Example 4
1) Preparing slurry: similarly to embodiment 1, except that in which SiC: AlN: y is2O3Is 85: 3: 12;
2) the connection process comprises the following steps: similar to example 1, except that the maximum temperature was 1850 ℃ and the holding time was 1.5 hours;
3) connection performance: the joint after connection in this example had a connection strength of 179MPa at normal temperature and 165MPa at a high temperature of 1400 ℃. The joint was subjected to oxidation treatment at a high temperature of 1500 ℃ for 8 hours, and then the joint strength was tested to 153 MPa.
Example 5
1) Preparing slurry: similar to embodiment 1;
2) the connection process comprises the following steps: similar to embodiment 1, except that the paste coating is performed by screen printing, the thickness of the paste layer is controlled to be 60 μm, the maximum temperature is 1850 ℃, and the temperature is kept for 1 h;
3) connection performance: the joint after connection of this embodiment had a connection strength of 272MPa at normal temperature. The bond strength at a high temperature of 1400 ℃ was 234 MPa. The joint was subjected to thermal shock treatment at a high temperature of 1500 ℃ for a total of 5 times, and then the joint strength was tested to 100 MPa.
Example 6
1) Preparing slurry: similar to embodiment 1, the difference is that SiC: AlN and Y2O3The mass ratio of (A) to (B) is 90: 10, wherein AlN: y is2O3The mass ratio of (1): 7;
2) the connection process comprises the following steps: similar to embodiment 1, except that the paste coating is performed by screen printing, the thickness of the paste layer is controlled to be 60 μm, the maximum temperature is 1850 ℃, and the temperature is kept for 1 h;
3) connection performance: the joint after connection of the present embodiment has a connection strength of 110MPa at normal temperature and a joint strength of 95MPa at 1400 ℃.
Example 7
1) Preparing slurry: similar to embodiment 1, the difference is that SiC: AlN and Y2O3The mass ratio of (A) to (B) is 90: 10, wherein AlN: y is2O3The mass ratio of (1): 1.5;
2) the connection process comprises the following steps: similar to embodiment 1, except that the paste coating is performed by screen printing, the thickness of the paste layer is controlled to be 60 μm, the maximum temperature is 1850 ℃, and the temperature is kept for 1 h;
3) connection performance: the joint after connection of this embodiment had a connection strength of 143MPa at normal temperature and a joint strength of 130MPa at 1400 ℃.
Example 8
1) Preparing slurry: similar to embodiment 1, the difference is that SiC: AlN and Y2O3The mass ratio of (A) to (B) is 90: 10, wherein AlN: y is2O3The mass ratio of (A) to (B) is 3: 2;
2) the connection process comprises the following steps: similar to embodiment 1, except that the paste coating is performed by screen printing, the thickness of the paste layer is controlled to be 60 μm, the maximum temperature is 1850 ℃, and the temperature is kept for 1 h;
3) connection performance: the joint after connection of the embodiment has the connection strength of 138MPa at normal temperature and the joint strength of 126MPa at 1400 ℃.
Example 9
1) Preparing slurry: similar to embodiment 1, the difference is that SiC: AlN and Y2O3The mass ratio of (A) to (B) is 90: 10, wherein AlN: y is2O3The mass ratio of (1): 3;
2) the connection process comprises the following steps: similar to embodiment 1, except that the paste coating is performed by screen printing, the thickness of the paste layer is controlled to be 60 μm, the maximum temperature is 1850 ℃, and the temperature is kept for 1 h;
3) connection performance: the joint after connection of this embodiment had a joint strength of 153MPa at normal temperature and 126MPa at 1400 ℃.
Example 10
1) Preparing slurry: similar to embodiment 1, the difference is that SiC: AlN and Y2O3The mass ratio of (A) to (B) is 90: 10, wherein AlN: y is2O3The mass ratio of (1): 5;
2) the connection process comprises the following steps: similar to embodiment 1, except that the paste coating is performed by screen printing, the thickness of the paste layer is controlled to be 60 μm, the maximum temperature is 1850 ℃, and the temperature is kept for 1 h;
3) connection performance: the joint after connection of the present embodiment has a connection strength of 134MPa at normal temperature and a connection strength of 116MPa at 1400 ℃.
Comparative example 1
1) Preparing slurry: similar to example 1;
2) the connection process comprises the following steps: similar to embodiment 1, the differences are: assembling without using a graphite clamp;
3) connection performance: the joining of the two pieces of silicon carbide ceramic was not achieved as shown in fig. 5.
Comparative example 2
1) Preparing slurry: similar to embodiment 1;
2) the connection process comprises the following steps: similar to embodiment 1, the difference is that: a hot-pressing sintering furnace is used, and 20MPa pressure is directly applied to two sides of the SiC ceramic.
3) Connection performance: the SiC ceramic surface was found to have cracks under an electron microscope, as shown in fig. 6.
Comparative example 3
1) Preparing slurry: similar to example 1, except that the solid content was 30%;
2) the connection process comprises the following steps: similar to embodiment 1;
3) connection performance: the connection layer is not dense, and more holes are formed in the middle as shown in fig. 7.
Comparative example 4
1) Preparing slurry: similar to example 1, except that the solid content was 70%;
2) the connection process comprises the following steps: similar to embodiment 1;
3) connection performance: the slurry is unevenly coated as shown in fig. 8, so that the two ceramic surfaces are difficult to be tightly contacted, and the connecting effect is poor.
Table 1 shows the performance parameters of the silicon carbide ceramic connectors:
the above embodiments are possible embodiments of the present invention, but the embodiments of the present invention are not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention and are intended to be equivalent substitutions are included in the scope of the present invention.
Claims (10)
1. A method for joining silicon carbide ceramics based on liquid phase sintering, comprising:
(1) mixing silicon carbide powder, a sintering aid, a dispersing agent, a binder and a solvent to obtain suspension slurry; the sintering aid is AlN powder and Y2O3Pulverizing;
(2) uniformly spreading the obtained suspension slurry on the surface to be connected of the first silicon carbide ceramic to obtain a slurry layer, attaching the surface to be connected of the second silicon carbide ceramic to the slurry layer, fixing the surface to be connected of the second silicon carbide ceramic by using a clamp, and finally realizing the connection of the silicon carbide ceramic in a normal-pressure sintering furnace;
preferably, the temperature of the liquid phase sintering is 1600-2000 ℃, the heat preservation time is 0.5-5 hours, and the atmosphere is inert atmosphere, more preferably argon; wherein the pressure applied by the clamp is 1-10 MPa.
2. The method for connecting silicon carbide ceramics based on liquid phase sintering according to claim 1, wherein the purity of the silicon carbide powder is not less than 99%, the oxygen content is less than 1%, and the particle size is 0.1-1 μm;
the AlN powder has the purity of more than or equal to 99 percent and the particle size of 0.1-1 mu m;
said Y is2O3The purity of the powder is more than or equal to 99 percent, and the particle size is 0.5-5 mu m.
3. The joining method based on liquid phase sintered silicon carbide ceramic according to claim 1 or 2, characterized in that; the mass ratio of the SiC to the sintering aid is (95-85): (5-15); preferably, AlN and Y are contained in the sintering aid2O3The mass ratio of (1): (0.1 to 10), more preferably 1: 4.
4. the method for joining silicon carbide ceramics according to any of claims 1 to 3, wherein the solvent is absolute ethanol or/and acetone; the dispersant is castor oil phosphate and/or castor oil; the binder is polyvinyl butyral and/or phenolic resin.
5. The method for joining silicon carbide ceramics based on liquid phase sintering according to any one of claims 1 to 4, wherein the solid content of the suspension slurry is 40 to 60 wt%;
the dispersing agent accounts for 3-8% of the total mass of the powder;
the binder accounts for 1-5% of the total mass of the powder.
6. The method for joining silicon carbide ceramics according to any one of claims 1 to 5, wherein the mixing is performed by ball milling; the rotation speed of ball milling mixing is 200-300 r/min, and the ball milling time is 12-24 hours;
the viscosity of the suspension slurry at a shear rate of 20/S is 200-1000 mPa & S.
7. The liquid phase sintering-based silicon carbide ceramic joining method according to any one of claims 1 to 6, wherein the spreading is by spin coating or screen printing;
the centrifugal spin coating speed is 1000-1500 rpm, and the time is 0.5-1 min;
the screen mesh number of the screen printing is 200-325 meshes;
the thickness of the slurry layer prepared by centrifugal spin coating or screen printing is 50-150 μm.
8. The liquid phase sintering-based silicon carbide ceramic joining method according to any one of claims 1 to 7, wherein the surface to be joined of the first silicon carbide ceramic and the surface to be joined of the second silicon carbide ceramic are subjected to surface grinding treatment to ensure a roughness Ra of less than 0.5 μm before spreading the slurry.
9. A silicon carbide ceramic connecting member produced by the connecting method based on a liquid phase sintered silicon carbide ceramic according to any one of claims 1 to 8, wherein the bending strength of the silicon carbide ceramic connecting member at room temperature is 200 to 300MPa, and the bending strength at 1400 ℃ is 100 to 150 MPa; the connecting layer of the silicon carbide ceramic connecting piece is subjected to corrosion of concentrated sulfuric acid for 48 hours and corrosion of concentrated nitric acid for 48 hours without change.
10. The silicon carbide ceramic connecting piece of claim 9 has potential application in the fields of pharmaceutical chemistry and nuclear energy in extreme service environments.
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| CN115974573A (en) * | 2022-12-15 | 2023-04-18 | 中国科学院上海硅酸盐研究所 | Silicon carbide connecting piece and method for connecting silicon carbide ceramic and composite material thereof by using laser-assisted silicon-aluminum alloy |
| CN115974573B (en) * | 2022-12-15 | 2023-11-10 | 中国科学院上海硅酸盐研究所 | Silicon carbide connecting piece and method for connecting silicon carbide ceramic and composite material thereof by laser-assisted silicon-aluminum alloy |
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