CN114133263B - High-entropy alloy connection method of silicon carbide and silicon carbide connecting piece - Google Patents
High-entropy alloy connection method of silicon carbide and silicon carbide connecting piece Download PDFInfo
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- CN114133263B CN114133263B CN202111275959.2A CN202111275959A CN114133263B CN 114133263 B CN114133263 B CN 114133263B CN 202111275959 A CN202111275959 A CN 202111275959A CN 114133263 B CN114133263 B CN 114133263B
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- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 title claims abstract description 106
- 229910010271 silicon carbide Inorganic materials 0.000 title claims abstract description 105
- 238000000034 method Methods 0.000 title claims abstract description 40
- 229910045601 alloy Inorganic materials 0.000 title claims abstract description 28
- 239000000956 alloy Substances 0.000 title claims abstract description 28
- 229910052751 metal Inorganic materials 0.000 claims abstract description 59
- 239000002184 metal Substances 0.000 claims abstract description 59
- 239000000758 substrate Substances 0.000 claims abstract description 46
- 238000005245 sintering Methods 0.000 claims abstract description 37
- 210000001503 joint Anatomy 0.000 claims abstract description 14
- 230000008595 infiltration Effects 0.000 claims abstract description 12
- 238000001764 infiltration Methods 0.000 claims abstract description 12
- 229910000905 alloy phase Inorganic materials 0.000 claims abstract description 7
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 14
- 238000005406 washing Methods 0.000 claims description 13
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 12
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 12
- 239000003513 alkali Substances 0.000 claims description 10
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims description 9
- 239000002253 acid Substances 0.000 claims description 9
- 229910052804 chromium Inorganic materials 0.000 claims description 9
- 239000011651 chromium Substances 0.000 claims description 9
- 239000000843 powder Substances 0.000 claims description 9
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 8
- 238000004140 cleaning Methods 0.000 claims description 8
- 229910002804 graphite Inorganic materials 0.000 claims description 8
- 239000010439 graphite Substances 0.000 claims description 8
- 150000002739 metals Chemical class 0.000 claims description 8
- 238000004321 preservation Methods 0.000 claims description 8
- 229910052782 aluminium Inorganic materials 0.000 claims description 7
- 229910017052 cobalt Inorganic materials 0.000 claims description 7
- 239000010941 cobalt Substances 0.000 claims description 7
- 229910052742 iron Inorganic materials 0.000 claims description 7
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 6
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 5
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 5
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 5
- 229910052750 molybdenum Inorganic materials 0.000 claims description 5
- 239000011733 molybdenum Substances 0.000 claims description 5
- 229910052759 nickel Inorganic materials 0.000 claims description 5
- 229910052758 niobium Inorganic materials 0.000 claims description 5
- 239000010955 niobium Substances 0.000 claims description 5
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims description 5
- 229910052720 vanadium Inorganic materials 0.000 claims description 5
- 229910052582 BN Inorganic materials 0.000 claims description 3
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 claims description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 3
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 3
- 238000001035 drying Methods 0.000 claims description 3
- 229910052735 hafnium Inorganic materials 0.000 claims description 3
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 claims description 3
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 3
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims description 3
- 229910052762 osmium Inorganic materials 0.000 claims description 3
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 claims description 3
- 229910052702 rhenium Inorganic materials 0.000 claims description 3
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 claims description 3
- 229910052715 tantalum Inorganic materials 0.000 claims description 3
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 239000010936 titanium Substances 0.000 claims description 3
- 229910052721 tungsten Inorganic materials 0.000 claims description 3
- 239000010937 tungsten Substances 0.000 claims description 3
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims description 3
- 229910052727 yttrium Inorganic materials 0.000 claims description 3
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 claims description 3
- 229910052726 zirconium Inorganic materials 0.000 claims description 3
- 229910000676 Si alloy Inorganic materials 0.000 claims 1
- 239000012466 permeate Substances 0.000 abstract description 2
- 239000012071 phase Substances 0.000 description 26
- 238000005253 cladding Methods 0.000 description 3
- 230000007797 corrosion Effects 0.000 description 3
- 238000005260 corrosion Methods 0.000 description 3
- 238000001272 pressureless sintering Methods 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical compound [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- SFJBWZNTPHYOEH-UHFFFAOYSA-N cobalt Chemical compound [Co].[Co].[Co] SFJBWZNTPHYOEH-UHFFFAOYSA-N 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 239000012535 impurity Substances 0.000 description 2
- ZYTNDGXGVOZJBT-UHFFFAOYSA-N niobium Chemical compound [Nb].[Nb].[Nb] ZYTNDGXGVOZJBT-UHFFFAOYSA-N 0.000 description 2
- 238000005498 polishing Methods 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 238000010008 shearing Methods 0.000 description 2
- 230000003746 surface roughness Effects 0.000 description 2
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 2
- 230000004888 barrier function Effects 0.000 description 1
- 238000005219 brazing Methods 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- 230000003749 cleanliness Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000003032 molecular docking Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 238000005086 pumping Methods 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 239000006104 solid solution Substances 0.000 description 1
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- 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
- 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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- 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
- C04B2237/12—Metallic interlayers
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- 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
- C04B2237/12—Metallic interlayers
- C04B2237/121—Metallic interlayers based on aluminium
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- 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
- C04B2237/12—Metallic interlayers
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- 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
- C04B2237/12—Metallic interlayers
- C04B2237/123—Metallic interlayers based on iron group metals, e.g. steel
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- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
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- C04B2237/00—Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
- C04B2237/30—Composition of layers of ceramic laminates or of ceramic or metallic articles to be joined by heating, e.g. Si substrates
- C04B2237/32—Ceramic
- C04B2237/36—Non-oxidic
- C04B2237/365—Silicon carbide
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Abstract
The invention discloses a high-entropy alloy connection method of silicon carbide and a silicon carbide connecting piece, wherein the high-entropy alloy connection method of the silicon carbide comprises the following steps: s1, butting and fixing two silicon carbide substrates by connecting surfaces to form a butting assembly; s2, placing the butt joint assembly in a sintering environment with a high-entropy metal permeable phase and sintering; in the sintering process, the high-entropy metal infiltration phase infiltrates into the connection surfaces of the silicon carbide substrates in a gas phase form, and the high-entropy metal infiltration phase are mutually and fixedly fused to form a high-entropy alloy phase which is used as a connection layer between the silicon carbide substrates. According to the high-entropy alloy connection method of the silicon carbide, high-entropy metal permeates into silicon carbide substrates in a gas phase form to form a compact connection layer, so that high-strength connection between the silicon carbide substrates under low pressure is realized.
Description
Technical Field
The invention relates to the technical field of ceramic material connection, in particular to a high-entropy alloy connection method of silicon carbide and a silicon carbide connecting piece.
Background
The silicon carbide ceramic has high melting point, excellent mechanical, thermal and corrosion resistance properties, so that the silicon carbide ceramic has wide application in the fields of vehicles, ocean engineering, nuclear energy, aerospace and the like. The above applications require not only that the silicon carbide has good high temperature resistance, but also have high requirements for its shape and structure.
In the connection of silicon carbide, when metal is used as a connection layer, the connection of silicon carbide can be carried out under relatively mild conditions, and the shape structure requirement of silicon carbide can be met, but a larger connection pressure, such as metal solid phase diffusion connection, is still required. When brazing is used for connection, silicon carbide connection can be achieved at low temperature and low pressure, but the high-temperature performance and the corrosion resistance of the joint are poor.
Therefore, it is highly desirable to develop a preparation method capable of realizing high-strength connection of silicon carbide under low-temperature and low-pressure conditions.
Disclosure of Invention
The invention aims to provide a high-entropy alloy connection method of silicon carbide and a silicon carbide connecting piece formed by the method, wherein the high-entropy alloy connection method of the silicon carbide can realize high-strength connection of the silicon carbide under low pressure.
The technical scheme adopted by the invention for solving the technical problem is as follows: the high-entropy alloy connection method of the silicon carbide comprises the following steps:
s1, butting and fixing two silicon carbide substrates by connecting surfaces to form a butting assembly;
s2, placing the butt joint assembly in a sintering environment with a high-entropy metal permeable phase and sintering;
in the sintering process, the high-entropy metal infiltration phase infiltrates into the connection surfaces of the silicon carbide substrates in a gas phase form, and the high-entropy metal infiltration phase are mutually and fixedly fused to form a high-entropy alloy phase which is used as a connection layer between the silicon carbide substrates.
Preferably, in step S1, the roughness of the connection surface of the silicon carbide substrate is 0.01 μm to 50 μm.
Preferably, in step S1, the silicon carbide substrate is subjected to a cleaning process in advance.
Preferably, the cleaning process comprises: and (3) carrying out acid washing or alkali washing on the silicon carbide substrate, then cleaning with acetone or ethanol, and drying.
Preferably, the acid solution used for acid washing is hydrochloric acid or an HF solution; the alkali liquor adopted by the alkali washing is NaOH.
Preferably, in step S2, the metal-infiltrated phase includes at least one of a metal powder and a metal block.
Preferably, the metal-infiltrated phase comprises at least three of the following metals: aluminum, iron, cobalt, nickel, titanium, zirconium, hafnium, yttrium, vanadium, niobium, tantalum, chromium, molybdenum, tungsten, manganese, rhenium, osmium.
Preferably, the molar ratio between the metals in the metal-infiltrated phase is 1.
Preferably, step S2 comprises: firstly, the butt joint component and the metal permeable phase are placed in a crucible, and then the crucible is placed in a sintering furnace for sintering.
Preferably, the crucible is a graphite crucible, a boron nitride crucible, an alumina crucible or an agate crucible.
Preferably, in the step S2, the sintering temperature is 1000-1800 ℃, and the heat preservation time is 0.5-10 h.
Preferably, in step S2, the sintering is performed under vacuum with a degree of vacuum of 10 -6 Pa～1Pa。
Preferably, the thickness of the connection layer is 1 μm to 100 μm.
The invention also provides a silicon carbide connecting piece which is formed by adopting the high-entropy alloy connecting method of the silicon carbide.
According to the high-entropy alloy connection method of the silicon carbide, high-strength connection between the silicon carbide under low pressure is realized by permeating high-entropy metal into silicon carbide substrates in a gas phase form to form a compact connection layer (high-entropy alloy phase).
In the invention, the high-entropy alloy phase is used as the connecting layer, so that the high-temperature-resistant and corrosion-resistant performance is better than that of a single metal, the thermal expansion coefficient mismatching degree between the metal phase in the silicon carbide and the silicon carbide substrate is reduced, and the reliability of the connecting piece is improved. In addition, the method can be carried out at low temperature and low pressure, the preparation condition of the silicon carbide joint is reduced, and the processing precision requirement of the silicon carbide substrate is also reduced.
Detailed Description
The high-entropy alloy connection method of silicon carbide can comprise the following steps of:
s1, butting and fixing two silicon carbide substrates by using connecting surfaces to form a butting assembly.
The connection surface of each silicon carbide substrate has the roughness requirement, so that subsequent high-entropy metal infiltration phases can be conveniently infiltrated and fixed on the connection surface. In contrast, the roughness of the connection surface of the silicon carbide substrate is 0.01 μm to 50 μm, preferably 1 μm to 10 μm. The roughness of the joint surface of the silicon carbide substrate can be achieved by polishing or the like.
In addition, before the two silicon carbide substrates are butted, the two silicon carbide substrates are cleaned in advance to remove impurities and the like, so that the cleanliness of a connecting surface is ensured. The cleaning treatment comprises the following steps: the silicon carbide substrate is firstly subjected to acid washing or alkali washing, then is washed by acetone or ethanol, and is dried. The acid liquor used for acid washing is hydrochloric acid or HF solution, and the concentration can be preferably 40vol%; the alkali liquor used for alkali washing is NaOH, and the concentration can be preferably 10vol%.
When the two silicon carbide substrates are fixed after being butted, the two silicon carbide substrates can be fixed by adopting modes such as clamping and the like, the two silicon carbide substrates are ensured to be relatively fixed after being butted to form a butted assembly, and no barrier is provided for a butted surface in the butted assembly.
S2, placing the butt joint assembly in a sintering environment with high-entropy metal permeable phases and sintering.
Wherein, in structural form, the metal permeable phase comprises at least one of metal powder and metal block. The metal infiltration phase includes, on the metal species, at least three of the following metals: aluminum, iron, cobalt, nickel, titanium, zirconium, hafnium, yttrium, vanadium, niobium, tantalum, chromium, molybdenum, tungsten, manganese, rhenium, osmium. In the metal-infiltrated phase, the molar ratio between the metals is 1.
The step S2 may specifically include: the butt joint assembly and the metal permeable phase are placed in a crucible, and then the crucible is placed in a sintering furnace (a pressureless sintering furnace) to be sintered. The crucible is a graphite crucible, a boron nitride crucible, an alumina crucible or an agate crucible.
When the metal-infiltrated phase is metal powder, the metal powder can be placed at the bottom of the crucible first, and then the butt joint assembly is placed above the metal powder. When the metal infiltration phase is a metal block, the metal block can be placed at the bottom of the crucible firstly, and then the butt joint component is placed above the metal powder; alternatively, a metal block is placed around the docking assembly within the crucible.
In the sintering furnace, pressure does not need to be applied to the silicon carbide substrates, the two silicon carbide substrates are butted at a certain connection pressure, and the butt joint assembly formed by the two silicon carbide substrates is stable only by ensuring that the butt joint surfaces of the two silicon carbide substrates are not staggered.
The sintering is preferably carried out under vacuum at a vacuum of 10 deg.C -6 Pa to 1Pa. During sintering, the sintering temperature is 1000-1800 ℃, and the heat preservation time is 0.5-10 h; the sintering temperature is preferably 1200-1500 ℃, and the heat preservation time is preferably 1-5 h.
In the sintering process, the high-entropy metal infiltration phase infiltrates into the connection surfaces of the silicon carbide substrates in a gas phase form, and is mutually and fixedly fused to form a high-entropy alloy phase which is used as a connection layer between the silicon carbide substrates to connect the two silicon carbide substrates into a whole. Wherein the thickness of the connecting layer is 1-100 μm.
The silicon carbide connecting piece is formed by adopting the high-entropy alloy connecting method of the silicon carbide. The shearing strength of the silicon carbide connecting piece is 50MPa to 150MPa at room temperature, and the shearing strength is 80MPa to 200MPa at the high temperature of 1200 ℃; the leakage rate is 0-1 x 10 -8 Pa.L/s and good air tightness.
The silicon carbide connector of the invention is suitable for nuclear cladding, such as SiC cladding, and realizes high-strength connection between the SiC end plug and the SiC cladding tube.
The invention is further illustrated by the following specific examples:
example 1
Polishing the connecting surface of the silicon carbide substrate, wherein the surface roughness of the connecting surface is 10 mu m, then performing alkali washing on the silicon carbide substrate by adopting NaOH, then further cleaning and removing impurities on the surface of the silicon carbide substrate by adopting acetone, and drying in a 50 ℃ oven. And butting the dried silicon carbide substrates and fixing the silicon carbide substrates by using a clamp to form a butting assembly.
Placing the butt joint assembly in a graphite crucible, and mixing aluminum, cobalt, chromium, iron and nickel powder according to the proportion of 1:1:1:1:1, and pressing into metal blocks, wherein the purity of each metal powder is 99.99%, and the particle size is 10-30 μm. Placing the three metal blocks in a graphite crucible, placing the three metal blocks around the butt joint assembly, and covering a graphite crucible cover. Placing the graphite crucible in a pressureless sintering furnace of a graphite heating element, and pumping the vacuum degree in the sintering furnace to 10 -2 Pa, raising the temperature to 1500 ℃ at the heating rate of 10 ℃/min, and keeping the temperature for 1h. And in the sintering process, the saturated vapor pressure of the metals of aluminum, cobalt, chromium, iron and nickel at 1500 ℃ is higher than the vacuum degree in a pressureless sintering furnace, at the moment, the metals permeate into the connecting surface of the butt joint component in a gas phase form, the metals are subjected to mutual solid solution in the gas phase permeation process to form a high-entropy alloy phase, a connecting layer is formed, and the two silicon carbide substrates are connected into a whole to obtain the silicon carbide connecting piece.
The connecting layer of the prepared silicon carbide connecting piece is made of AlCoCrFeNi high-entropy alloy, and the thickness of the connecting layer is 30 micrometers. The shear strength test is carried out on the silicon carbide connecting piece, and the result shows that the shear strength at room temperature reaches 100MPa and the shear strength at high temperature of 1200 ℃ reaches 120MPa; the leakage rate of the connecting piece is 1 multiplied by 10 -11 Pa·L/s。
Example 2
The silicon carbide was bonded by the method of example 1 using aluminum, cobalt, chromium, iron, and nickel powders as metal-infiltrated metal phases with a surface roughness of 0.1 μm, and a sintering furnace with a vacuum degree of 10 -5 Pa, the sintering temperature is 1450 ℃, and the heat preservation time is 2h.
In the silicon carbide connector prepared in this example, the connection layer is made of AlCoCrFeNi high-entropy alloy and the thickness is 2 μm. The shear strength test shows that the shear strength is 80MPa at room temperature and 90MPa at high temperature of 1200 ℃; the leakage rate of the connecting piece is 1 multiplied by 10 -9 Pa·L/s。
Example 3
Using aluminum, cobalt, chromium, iron and nickel powder as metalPenetrating the metal phase, the roughness of the connecting surface of the silicon carbide substrate is 50 mu m, the connection of the silicon carbide is realized according to the method of the embodiment 1, the vacuum degree of a sintering furnace is 10 -1 Pa, the sintering temperature is 1600 ℃, and the heat preservation time is 2h.
In the silicon carbide connector prepared in the embodiment, the connecting layer is made of AlCoCrFeNi high-entropy alloy, and the thickness is 80 μm. The shear strength test shows that the shear strength is 60MPa at room temperature and 80MPa at the high temperature of 1200 ℃; the leakage rate of the connecting piece is 1 multiplied by 10 -10 Pa·L/s。
Example 4
The connection of silicon carbide is realized according to the method of the embodiment 1 by taking vanadium, chromium, niobium, molybdenum and tungsten powder as metal infiltration metal phases and the roughness of the connection surface of the silicon carbide substrate is 1 mu m, and the vacuum degree of a sintering furnace is 10 -5 Pa, the sintering temperature is 1800 ℃ and the heat preservation time is 4h.
In the silicon carbide connector prepared in this example, the connection layer is a vcrnbbowhigh-entropy alloy, and the thickness is 10 μm. The shear strength test shows that the shear strength is 100MPa at room temperature and 1100MPa at high temperature of 1200 ℃; the leakage rate of the connecting piece is 1 multiplied by 10 -10 Pa·L/s。
Example 5
The connection of silicon carbide is realized according to the method of the embodiment 1 by taking vanadium, chromium, niobium, molybdenum and tungsten powder as metal infiltration metal phases and the roughness of the connection surface of the silicon carbide substrate is 50 microns, and the vacuum degree of a sintering furnace is 10 -5 Pa, the sintering temperature is 1700 ℃, and the heat preservation time is 2h.
In the silicon carbide connector prepared in this example, the connection layer was VCrNbMoW high-entropy alloy and the thickness was 90 μm. The shear strength test shows that the shear strength is 60MPa at room temperature and 80MPa at the high temperature of 1200 ℃; the leakage rate of the connecting piece is 1 multiplied by 10 -10 Pa·L/s。
The above description is only an embodiment of the present invention, and is not intended to limit the scope of the present invention, and all equivalent structures or equivalent processes performed by the present invention or directly or indirectly applied to other related technical fields are also included in the scope of the present invention.
Claims (11)
1. A high-entropy alloy connection method of silicon carbide is characterized by comprising the following steps:
s1, butting and fixing two silicon carbide substrates by connecting surfaces to form a butting assembly;
the roughness of the connection surface of the silicon carbide substrate is 0.1-50 mu m;
s2, placing the butt joint assembly in a sintering environment with a high-entropy metal permeable phase and sintering;
the sintering is carried out under vacuum, the sintering temperature is 1200-1500 ℃, and the heat preservation time is 1-5 h; in the sintering process, the high-entropy metal infiltration phase infiltrates into the joint surfaces of the silicon carbide substrates in a gas phase form, and is mutually and fixedly fused to form a high-entropy alloy phase serving as a joint layer between the silicon carbide substrates; the thickness of the connecting layer is 1-90 μm.
2. A high-entropy alloy bonding method for silicon carbide according to claim 1, wherein in step S1, the silicon carbide substrate is subjected to a cleaning treatment in advance.
3. A high entropy alloy joining method of silicon carbide, according to claim 2, wherein the cleaning treatment includes: and (3) carrying out acid washing or alkali washing on the silicon carbide substrate, then cleaning with acetone or ethanol, and drying.
4. A high-entropy alloy bonding method for silicon carbide according to claim 3, wherein an acid solution used for the acid washing is hydrochloric acid or an HF solution; the alkali liquor adopted by the alkali washing is NaOH.
5. A high entropy alloy joining method of silicon carbide according to claim 1, wherein in step S2, the metal infiltration phase includes at least one of a metal powder and a metal bulk.
6. A high entropy alloy joining method of silicon carbide according to claim 1, wherein the metal infiltrant phase includes at least three of the following metals: aluminum, iron, cobalt, nickel, titanium, zirconium, hafnium, yttrium, vanadium, niobium, tantalum, chromium, molybdenum, tungsten, manganese, rhenium, osmium.
7. A high entropy alloy joining method of silicon carbide, according to claim 6, wherein the molar ratio between each metal in the metal infiltrated phase is 1.
8. A high entropy alloy joining method of silicon carbide, according to claim 1, wherein step S2 includes: firstly, the butt joint component and the metal permeable phase are placed in a crucible, and then the crucible is placed in a sintering furnace for sintering.
9. A high entropy alloy joining method of silicon carbide according to claim 8, characterized in that the crucible is a graphite crucible, a boron nitride crucible, an alumina crucible or an agate crucible.
10. A high-entropy alloy joining method of silicon carbide, according to claim 1, wherein a degree of vacuum in the sintering process in step S2 is 10 "6 Pa to 1Pa.
11. A silicon carbide connector formed by the method of joining high entropy alloys of silicon carbide as claimed in any one of claims 1 to 10.
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