WO2023241059A1

WO2023241059A1 - Silicon carbide cladding connection material, silicon carbide ceramic connector and manufacturing method therefor, and device housing

Info

Publication number: WO2023241059A1
Application number: PCT/CN2023/074180
Authority: WO
Inventors: 吴利翔; 薛佳祥; 廖业宏; 任啟森; 翟剑晗; 刘洋; 马海滨; 张显生
Original assignee: 中广核研究院有限公司; 岭东核电有限公司; 中国广核集团有限公司; 中国广核电力股份有限公司
Priority date: 2022-06-17
Filing date: 2023-02-02
Publication date: 2023-12-21
Also published as: CN115057715B; CN115057715A

Abstract

The present application relates to a silicon carbide cladding connection material, a silicon carbide ceramic connector and a manufacturing method therefor, and a device housing. The composition of the silicon carbide cladding connection material comprises at least five of titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, molybdenum carbide, and tungsten carbide.

Description

Silicon carbide cladding connection material, silicon carbide ceramic connector and manufacturing method and device cladding

Related applications

This application requires the priority of the Chinese patent application filed on June 17, 2022, with the application number 202210684083.5 and titled "Silicon carbide cladding connection materials, silicon carbide ceramic connectors and their production methods and applications", and is hereby Its entire text is incorporated by reference.

Technical field

The present application relates to the technical field of silicon carbide ceramics, and in particular to a silicon carbide cladding connection material, a silicon carbide ceramic connector, a manufacturing method thereof, and a device cladding.

Background technique

Silicon carbide ceramic (SiC) has a high melting point, excellent mechanical, thermal and corrosion resistance properties, making it widely used in vehicles, marine engineering, nuclear energy, aerospace and other fields, especially in nuclear cladding. Advantage. However, due to the high melting point and low diffusion coefficient of silicon carbide ceramics, it is difficult to connect silicon carbide ceramics. Therefore, there is an urgent need to develop suitable silicon carbide ceramic connection and packaging methods to promote the application of silicon carbide ceramics in the field of nuclear cladding.

At present, silicon carbide ceramic connections can be connected and encapsulated through metal diffusion and brazing, and the joint density and connection strength are better. However, metal as a connecting material results in poor joint resistance to high temperature and corrosion resistance, and the joints are Because the thermal expansion coefficient mismatch between metal and silicon carbide ceramics is large, large residual stress is easily generated in the prepared silicon carbide ceramic joints. In addition, there are ways to blend polysiloxane precursor or glass powder with carbide materials as connecting materials. However, during the connection process of the precursor, a large amount of gas is generated due to cracking, and more pore defects are easily generated at the joint, thus Reduce joint connection performance; when glass powder and carbide are doped as connection materials, the presence of glass powder not only reduces the high-temperature performance of the joint, but also causes poor corrosion resistance.

In order to solve the above problems, it is mainly considered to use ceramic materials with better corrosion resistance and high temperature resistance as the connecting layer, such as MAX phase dissimilar materials and the same material as silicon carbide ceramics. Among them, when MAX phase dissimilar materials are used to connect, the residual stress at the joint cannot be alleviated. When silicon carbide ceramics are used as connecting materials, liquid phase sintering additives need to be introduced. The presence of liquid phase sintering additives will inevitably reduce the high temperature performance and corrosion resistance of the joint.

Contents of the invention

Based on this, this application provides a silicon carbide cladding connection material, a silicon carbide ceramic connector, a manufacturing method thereof, and a device cladding.

A first aspect of the application provides a silicon carbide cladding connection material. The composition of the silicon carbide cladding connection material includes titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, carbide, At least five of molybdenum and tungsten carbide.

A second aspect of this application provides a method for preparing the silicon carbide cladding connection material described in the first aspect, including the following steps:

The components of the silicon carbide cladding connecting material are mixed and then ball milled; the components of the silicon carbide cladding connecting material include titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, and molybdenum carbide. and at least five of tungsten carbide.

A third aspect of the present application provides a method for manufacturing a silicon carbide ceramic connector, using the silicon carbide cladding connecting material described in the first aspect or the silicon carbide cladding connecting material prepared by the preparation method described in the second aspect. Make a connection.

A fourth aspect of the present application provides a silicon carbide ceramic connector produced by the manufacturing method described in the third aspect.

A fifth aspect of the present application provides a device enclosure, including the silicon carbide ceramic connector described in the fourth aspect.

Detailed ways

The silicon carbide cladding connection material, silicon carbide ceramic connector, manufacturing method and device cladding of the present application will be further described in detail below with reference to specific examples. The application may be implemented in many different forms and is not limited to the embodiments described herein. Rather, these embodiments are provided so that a thorough understanding of this disclosure will be provided.

Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the technical field to which this application belongs. The terminology used herein in the description of the application is for the purpose of describing specific embodiments only and is not intended to limit the application.

In this article, "one or more" refers to any one, any two, or any two or more of the listed items.

In this article, "at least five kinds" refers to any five kinds, any six kinds or any seven or more kinds of the listed items.

In this application, the terms "first aspect", "second aspect", "third aspect", "fourth aspect", "fifth aspect", etc. are only used for descriptive purposes and cannot be understood as indicating or implying relative importance or quantity, nor shall it be understood as implying an indication of the importance or quantity of the technical features indicated. Moreover, “first”, “second”, “third”, “fourth”, “fifth”, etc. only serve the purpose of non-exhaustive enumeration and description, and it should be understood that they do not constitute a closed limit to the quantity.

In this application, the technical features described in open format include closed technical solutions composed of the listed features, and also include open technical solutions including the listed features.

In this application, when it comes to numerical intervals, unless otherwise specified, the above numerical interval is considered to be continuous and includes the minimum value and maximum value of the range, as well as every value between such minimum value and maximum value. Further, when a range refers to an integer, every integer between the minimum value and the maximum value of the range is included. Additionally, when multiple ranges are provided to describe a feature or characteristic, the ranges can be combined. In other words, unless otherwise indicated, all ranges disclosed herein are to be understood to include any and all subranges subsumed therein.

The percentage content involved in this application, unless otherwise specified, refers to mass percentage for solid-liquid mixing and solid-solid phase mixing, and refers to volume percentage for liquid-liquid phase mixing.

The percentage concentrations mentioned in this application refer to the final concentration unless otherwise specified. The final concentration refers to the proportion of the added component in the system after adding the component.

The temperature parameters in this application, unless otherwise specified, allow for constant temperature treatment or treatment within a certain temperature range. The thermostatic treatment described allows the temperature to fluctuate within the accuracy of the instrument control.

The room temperature in this application generally refers to 4°C to 30°C, preferably 20±5°C.

The present application provides a silicon carbide cladding connecting material. The composition of the silicon carbide cladding connecting material includes titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, molybdenum carbide and tungsten carbide. of at least five.

The above-mentioned silicon carbide cladding connection materials are compounded by selecting more than five types of specific carbides, and can be used to connect silicon carbide ceramic materials. The residual stress at the connection is small, and it also has good resistance to high temperatures and corrosion. Performance, with high shear strength at room temperature and high temperature.

In some specific examples, the silicon carbide cladding connection material is composed of five materials: zirconium carbide, titanium carbide, niobium carbide, tantalum carbide, and molybdenum carbide; or includes zirconium carbide, titanium carbide, hafnium carbide, and tantalum carbide. and tungsten carbide; or include zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and vanadium carbide.

Further, the silicon carbide cladding connection material is composed of five materials: zirconium carbide, titanium carbide, niobium carbide, tantalum carbide and molybdenum carbide; or five kinds of zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and tungsten carbide. Material; or five materials: zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and vanadium carbide.

In some specific examples, the molar ratio of the five materials is (0.5~1.5):(0.5~1.5):(0.5~1.5):(0.5~1.5):(0.5~1.5). Specifically, the molar ratios of the five materials include but are not limited to: 1:(0.5～1.5):(0.5～1.5):(0.5～1.5):(0.5～1.5), (0.5～1.5):1:(0.5 ~1.5):(0.5~1.5):(0.5~1.5), (0.5~1.5):(0.5~1.5):1:(0.5~1.5):(0.5~1.5), (0.5~1.5):(0.5 ~1.5): (0.5～1.5):1:(0.5～1.5), (0.5～1.5):(0.5～1.5):(0.5～1.5):(0.5～1.5):1 or a range consisting of any two of the aforementioned values.

In some specific examples, the molar ratio of the five materials is (0.8~1.2):(0.8~1.2):(0.8~1.2):(0.8~1.2):(0.8~1.2) zirconium carbide and titanium carbide , niobium carbide, tantalum carbide and molybdenum carbide. Specifically, the molar ratios of the five materials include but are not limited to: 1:(0.8~1.2):(0.8~1.2):(0.8~1.2):(0.8~1.2), (0.8~1.2):1:(0.8 ~1.2):(0.8~1.2):(0.8~1.2), (0.8~1.2):(0.8~1.2):1:(0.8~1.2):(0.8~1.2), (0.8~1.2):(0.8 ~1.2):(0.8~1.2):1:(0.8~1.2), (0.8~1.2):(0.8~1.2):(0.8~1.2):(0.8~1.2):1 or any two of the above values range.

In some specific examples, the composition of the silicon carbide cladding connection material includes zirconium carbide, titanium carbide, niobium carbide, tantalum carbide and molybdenum carbide in a molar ratio of 1:1:1:1:1, or a molar ratio of Zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and tungsten carbide in a molar ratio of 1:1:1:1:1, or zirconium carbide, titanium carbide, hafnium carbide, carbide in a molar ratio of 1:1:1:1:1 Tantalum and vanadium carbide.

In some specific examples, the particle sizes of titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, molybdenum carbide and tungsten carbide are (each independently) 0.01 μm to 10 μm. . Specifically, the particle diameter includes but is not limited to: 0.01 μm, 0.05 μm, 0.1 μm, 0.2 μm, 0.5 μm, 1 μm, 3 μm, 5 μm, 7 μm, 9 μm, 10 μm or a range consisting of any two of the aforementioned values.

In some specific examples, the particle sizes of titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, molybdenum carbide and tungsten carbide are the same.

This application also provides a method for preparing a silicon carbide cladding connection material, which includes the following steps:

It can be understood that the composition of the silicon carbide cladding connection material has similar technical solutions and advantages to the above-mentioned silicon carbide cladding connection material, and will not be described again here.

Without limitation, the method of ball milling is one or a combination of dry ball milling, wet ball milling, and high-energy ball milling.

In some specific examples, the conditions for the ball milling process include: the ball milling medium is silicon nitride grinding balls.

In some specific examples, the conditions for the ball milling treatment include: the ball milling liquid is acetone.

In some specific examples, the conditions for the ball milling treatment include: the ball milling rotation speed is 300 to 500 r/min. Specifically, the ball mill rotation speed includes but is not limited to: 300r/min, 350r/min, 380r/min, 400r/min, 420r/min, 450r/min, 500r/min or a range consisting of any two of the aforementioned values.

In some specific examples, the conditions for the ball milling treatment include: the ball milling time is 20h to 30h. Specifically, the ball milling time includes but is not limited to: 20h, 21h, 22h, 23h, 24h, 25h, 26h, 27h, 28h, 29h, 30h or a range consisting of any two of the aforementioned values.

In some of these specific examples, after the ball milling process is completed, a drying step is also included.

The present application also provides a method for making silicon carbide ceramic connectors, using the silicon carbide cladding connecting material as mentioned above or the silicon carbide cladding connecting material prepared by the above preparation method for connection.

In some specific examples, the manufacturing method of silicon carbide ceramic connectors includes the following steps:

S1: Place the silicon carbide cladding connecting material between the silicon carbide ceramics to be connected to prepare a preform;

S2: Perform heat treatment on the preform to prepare the silicon carbide ceramic connector.

Specifically, in step S1:

In some specific examples, the method of placing the silicon carbide cladding connecting material between the silicon carbide ceramics to be connected includes one or more of casting, slurry and powder spreading.

In some of these specific examples, the prefabricated parts are in a sandwich structure.

Specifically, in step S2:

In some specific examples, the heat treatment conditions include: a temperature of 1800°C to 2200°C. Specifically, the temperature includes but Not limited to: 1800℃, 1810℃, 1850℃, 1900℃, 2000℃, 2100℃, 2200℃ or the range consisting of any two of the aforementioned values.

In some specific examples, the heat treatment conditions include: a pressure of 20MPa to 35MPa. Specifically, the pressure includes but is not limited to: 20MPa, 21MPa, 22MPa, 23MPa, 24MPa, 25MPa, 26MPa, 27MPa, 28MPa, 29MPa, 30MPa, 31MPa, 32MPa, 33MPa, 34MPa, 35MPa or a range consisting of any two of the aforementioned values. Understandably, this pressure is mechanical pressure.

In some specific examples, the heat treatment steps are as follows:

Raise the temperature to 1800℃~2200℃ at a heating rate of 10~15℃/min, keep it at 1800℃~2200℃ for 1h~2h, and then cool down symmetrically at a cooling rate of 10~15℃/min after the insulation.

Specifically, the heating rate includes but is not limited to: 10°C/min, 11°C/min, 12°C/min, 13°C/min, 14°C/min, and 15°C/min. The cooling rate includes but is not limited to: 10°C/min, 11°C/min, 12°C/min, 13°C/min, 14°C/min, 15°C/min or a range consisting of any two of the aforementioned values.

Specifically, the holding time includes but is not limited to: 1 h, 1.5 h, 2 h or a range consisting of any two of the aforementioned values.

In some specific examples, the heat treatment is performed in an atmosphere or vacuum, and the atmosphere is one or more of argon, helium, nitrogen and air.

This application also provides a silicon carbide ceramic connector, which is produced by the above-mentioned production method.

This application also provides a device enclosure, including the silicon carbide ceramic connector as mentioned above. Without limitation, the device cladding may include, for example, a nuclear cladding.

The following are specific examples. Unless otherwise specified, the raw materials used in the examples are all commercially available products.

Example 1

This embodiment is a method for manufacturing a silicon carbide ceramic connector. The steps are as follows:

(1) Preparation of silicon carbide cladding connection material:

Zirconium carbide (0.1μm), titanium carbide (0.1μm), niobium carbide (0.1μm), tantalum carbide (0.1μm) and molybdenum carbide (0.1μm) are used as raw material powders, and the molar ratio of the powders is 1:1:1 : 1:1, the above powder is ball milled in a planetary ball mill according to this molar ratio, the ball milling speed is 400r/min, the ball milling time is 24h, the ball milling medium is silicon nitride grinding ball, the ball milling liquid is acetone, and it is evaporated by rotary Separate acetone and mixed powder in the above slurry, and then dry the above mixed powder to obtain dry mixed powder, that is, silicon carbide cladding connecting material.

(2)Sealing:

The silicon carbide cladding connection material prepared in step (1) is placed between silicon carbide ceramic materials to form a sandwich structure, and then the above sandwich structure is placed in a sintering furnace for connection. The connection process is: heating at a heating rate of 10°C/min to 1800°C, and hold at 1800°C for 2 hours. After the heat preservation is completed, the temperature is symmetrically cooled at a cooling rate of 10°C/min. The connection atmosphere is an argon atmosphere, and the mechanical pressure of 30MPa is maintained during the heat preservation stage. In the silicon carbide ceramic connector prepared through the above process, the composition of the connection layer is (Zr _0.2 Ti _0.2 Nb _0.2 Ta _0.2 Mo _0.2 )C.

Among the above-mentioned silicon carbide ceramic connectors, the shear strength at room temperature is 80MPa, the high-temperature shear strength at 1200℃ reaches 90MPa, the residual stress of the joint is 50MPa, and the weight change after corrosion in a water vapor environment of 360℃/18.6MPa for 30 days is less than 2mg/dm ² .

Example 2

(1) Preparation of silicon carbide cladding connection material:

Zirconium carbide (10μm), titanium carbide (10μm), niobium carbide (10μm), tantalum carbide (10μm) and molybdenum carbide (10μm) are used as raw material powders. The molar ratio of the powders is 1:1:1:1:1. The above powder is ball milled in a planetary ball mill according to the molar ratio. The ball milling speed is 400r/min, the ball milling time is 24h, the ball milling medium is silicon nitride grinding ball, and the ball milling liquid is acetone. The above powder is milled by rotary evaporation. The acetone and mixed powder in the slurry are separated, and then the above mixed powder is dried to obtain dry mixed powder, that is, silicon carbide cladding connecting material.

(2)Sealing:

The silicon carbide cladding connection material prepared in step (1) is placed between silicon carbide ceramic materials to form a sandwich structure, and then the above sandwich structure is placed in a sintering furnace for connection. The connection process is: heating at a heating rate of 15°C/min to 2200°C, and hold at 2200°C for 1 hour. After the heat preservation is completed, the temperature is symmetrically cooled at a cooling rate of 15°C/min. The connection atmosphere is an argon atmosphere, and the mechanical pressure of 30MPa is maintained during the heat preservation stage. In the silicon carbide ceramic connector prepared through the above process, the composition of the connection layer is (Zr _0.2 Ti _0.2 Nb _0.2 Ta _0.2 Mo _0.2 )C.

Among the above-mentioned silicon carbide ceramic connectors, the shear strength at room temperature is 90MPa, the high-temperature shear strength at 1200℃ reaches 100MPa, the residual stress of the joint is 60MPa, and the weight change after corrosion in a water vapor environment of 360℃/18.6MPa for 30 days is less than 1mg/dm ² .

Example 3

(1) Preparation of silicon carbide cladding connection material:

Zirconium carbide (5μm), titanium carbide (5μm), niobium carbide (5μm), tantalum carbide (5μm) and molybdenum carbide (5μm) are used as raw material powders. The molar ratio of the powders is 1:1:1:1:1. The above powder is ball milled in a planetary ball mill according to the molar ratio. The ball milling speed is 400r/min, the ball milling time is 24h, the ball milling medium is silicon nitride grinding ball, and the ball milling liquid is acetone. The above slurry is removed by rotary evaporation. Acetone and mixed powder are separated, and then the above mixed powder is dried to obtain dry mixed powder, that is, silicon carbide cladding connecting material.

(2)Sealing:

The silicon carbide cladding connection material prepared in step (1) is placed between silicon carbide ceramic materials to form a sandwich structure, and then the above sandwich structure is placed in a sintering furnace for connection. The connection process is: heating at a heating rate of 15°C/min to 2000°C, and hold at 2000°C for 1.5 hours. After the heat preservation is completed, the temperature is symmetrically cooled at a cooling rate of 15°C/min. The connection atmosphere is an argon atmosphere, and the mechanical pressure of 30MPa is maintained during the heat preservation stage. In the silicon carbide ceramic connector prepared through the above process, the composition of the connection layer is (Zr _0.2 Ti _0.2 Nb _0.2 Ta _0.2 Mo _0.2 )C.

Among the above-mentioned silicon carbide ceramic connectors, the shear strength at room temperature is 85MPa, the high-temperature shear strength at 1200℃ reaches 90MPa, the residual stress of the joint is 55MPa, and the weight change after corrosion in a water vapor environment of 360℃/18.6MPa for 30 days is less than 1.5mg/ ^dm2 .

Example 4

(1) Preparation of connection materials:

Zirconium carbide (0.01μm), titanium carbide (0.01μm), hafnium carbide (0.01μm), tantalum carbide (0.01μm) and tungsten carbide (0.01μm) are used as raw material powders, and the molar ratio of the powders is 1:1:1 : 1:1, the above powder is ball milled in a planetary ball mill according to this molar ratio, the ball milling speed is 400r/min, the ball milling time is 24h, the ball milling medium is silicon nitride grinding ball, the ball milling liquid is acetone, and it is evaporated by rotary Separate the acetone and mixed powder in the above slurry, and then dry the above mixed powder to obtain dry mixed powder, that is, the connecting material.

(2)Sealing:

The connection material prepared in step (1) is placed between silicon carbide ceramic materials to form a sandwich structure, and then the above sandwich structure is placed in a sintering furnace for connection. The connection process is: heating to 1800°C at a heating rate of 15°C/min. Incubate at 1800℃ for 1 hour. After the insulation is completed, the temperature is symmetrically cooled at a cooling rate of 15℃/min. The connection atmosphere is an argon atmosphere. The mechanical pressure of 30MPa is maintained during the insulation period. In the silicon carbide ceramic connector prepared through the above process, the composition of the connection layer is (Zr _0.2 Ti _0.2 Hf _0.2 Ta _0.2 W _0.2 )C.

Among the above-mentioned silicon carbide ceramic connectors, the shear strength at room temperature is 80MPa, the high-temperature shear strength at 1200℃ reaches 95MPa, the residual stress of the joint is 40MPa, and the weight change after corrosion in a water vapor environment of 360℃/18.6MPa for 30 days is less than 1.5mg/ ^dm2 .

Example 5

(1) Preparation of connection materials:

Zirconium carbide (0.1μm), titanium carbide (0.1μm), hafnium carbide (0.1μm), tantalum carbide (0.1μm) and vanadium carbide (0.1μm) are used as raw material powders, and the molar ratio of the powders is 1:1:1 : 1:1, the above powder is ball milled in a planetary ball mill according to this molar ratio, the ball milling speed is 400r/min, the ball milling time is 24h, the ball milling medium is silicon nitride grinding ball, the ball milling liquid is acetone, and it is evaporated by rotary Separate the acetone and mixed powder in the above slurry, and then dry the above mixed powder to obtain dry mixed powder, that is, the connecting material.

(2)Sealing:

The connection material prepared in step (1) is placed between silicon carbide ceramic materials to form a sandwich structure, and then the above sandwich structure is placed in a sintering furnace for connection. The connection process is: heating to 1900°C at a heating rate of 15°C/min. Incubate at 1900℃ for 1 hour. After the insulation is completed, the temperature is symmetrically cooled at a cooling rate of 15℃/min. The connection atmosphere is an argon atmosphere. The mechanical pressure of 20MPa is maintained during the insulation period. In the silicon carbide ceramic connector prepared through the above process, the composition of the connection layer is (Zr _0.2 Ti _0.2 Hf _0.2 Ta _0.2 V _0.2 )C.

Among the above-mentioned silicon carbide ceramic connectors, the shear strength at room temperature is 95MPa, the high-temperature shear strength at 1200℃ reaches 100MPa, the residual stress of the joint is 50MPa, and the weight change after corrosion in a water vapor environment of 360℃/18.6MPa for 30 days is less than 1mg/dm ² .

The technical features of the above-described embodiments can be combined in any way. To simplify the description, not all possible combinations of the technical features in the above-described embodiments are described. However, as long as there is no contradiction in the combination of these technical features, All should be considered to be within the scope of this manual.

The above-described embodiments only express several implementation modes of the present application, and their descriptions are relatively specific and detailed, but they should not be construed as limiting the scope of the patent application. It should be noted that, for those of ordinary skill in the art, several modifications and improvements can be made without departing from the concept of the present application, and these all fall within the protection scope of the present application. Therefore, the protection scope of this patent application should be determined by the appended claims.

Claims

A silicon carbide cladding connecting material, the composition of the silicon carbide cladding connecting material includes at least five of titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, molybdenum carbide and tungsten carbide. kind.
The silicon carbide cladding connection material according to claim 1, wherein the composition of the silicon carbide cladding connection material includes zirconium carbide, titanium carbide, niobium carbide, tantalum carbide and molybdenum carbide;

or includes zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and tungsten carbide;

Or include zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and vanadium carbide.
The silicon carbide cladding connection material according to claim 1 or 2, characterized in that the composition of the silicon carbide cladding connection material includes a molar ratio of (0.5~1.5): (0.5~1.5): (0.5~1.5 ): (0.5～1.5): (0.5～1.5) zirconium carbide, titanium carbide, niobium carbide, tantalum carbide and molybdenum carbide;

Or include zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and tungsten carbide in a molar ratio of (0.5～1.5): (0.5～1.5): (0.5～1.5): (0.5～1.5): (0.5～1.5);

Or it includes zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and vanadium carbide in a molar ratio of (0.5～1.5): (0.5～1.5): (0.5～1.5): (0.5～1.5): (0.5～1.5).
The silicon carbide cladding connecting material according to any one of claims 1 to 3, characterized in that the composition of the silicon carbide cladding connecting material includes a molar ratio of (0.8~1.2):(0.8~1.2):( 0.8～1.2):(0.8～1.2):(0.8～1.2) zirconium carbide, titanium carbide, niobium carbide, tantalum carbide and molybdenum carbide;

Or include zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and tungsten carbide in a molar ratio of (0.8～1.2): (0.8～1.2): (0.8～1.2): (0.8～1.2): (0.8～1.2);

Or it includes zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and vanadium carbide in a molar ratio of (0.8～1.2): (0.8～1.2): (0.8～1.2): (0.8～1.2): (0.8～1.2).
The silicon carbide cladding connection material according to any one of claims 1 to 4, characterized in that the titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, molybdenum carbide and carbide The particle diameters of tungsten are independently 0.01 μm to 10 μm.
A method for preparing silicon carbide cladding connection material, including the following steps:

The components of the silicon carbide cladding connecting material are mixed and then ball milled; the components of the silicon carbide cladding connecting material include titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, carbide At least five of molybdenum and tungsten carbide.
The preparation method of silicon carbide cladding connection material according to claim 6, characterized in that the conditions of the ball milling treatment include: the ball milling medium is silicon nitride grinding ball, the ball milling liquid is acetone, and the ball milling rotation speed is 300-500r /min, the ball milling time is 20h~30h.
The preparation method of silicon carbide cladding connection material according to claim 6 or 7, characterized in that each component of the silicon carbide cladding connection material includes zirconium carbide, titanium carbide, niobium carbide, tantalum carbide and molybdenum carbide;

or includes zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and tungsten carbide;

Or include zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and vanadium carbide.
The method for preparing a silicon carbide cladding connection material according to any one of claims 6 to 8, characterized in that each component of the silicon carbide cladding connection material includes a molar ratio of (0.5~1.5): (0.5~ 1.5):(0.5～1.5):(0.5～1.5):(0.5～1.5) zirconium carbide, titanium carbide, niobium carbide, tantalum carbide and molybdenum carbide;

Or it includes zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and tungsten carbide in a molar ratio of (0.5～1.5): (0.5～1.5): (0.5～1.5): (0.5～1.5): (0.5～1.5);

Or it includes zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and vanadium carbide in a molar ratio of (0.5～1.5): (0.5～1.5): (0.5～1.5): (0.5～1.5): (0.5～1.5).
The method for preparing a silicon carbide cladding connection material according to any one of claims 6 to 9, characterized in that each composition of the silicon carbide cladding connection material includes a molar ratio of (0.8~1.2): (0.8~ 1.2):(0.8～1.2):(0.8～1.2):(0.8～1.2) zirconium carbide, titanium carbide, niobium carbide, tantalum carbide and molybdenum carbide;

Or include zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and tungsten carbide in a molar ratio of (0.8～1.2): (0.8～1.2): (0.8～1.2): (0.8～1.2): (0.8～1.2);

Or it includes zirconium carbide, titanium carbide, hafnium carbide, tantalum carbide and vanadium carbide in a molar ratio of (0.8～1.2): (0.8～1.2): (0.8～1.2): (0.8～1.2): (0.8～1.2).
The preparation method of silicon carbide cladding connecting material according to any one of claims 6 to 10, characterized in that the titanium carbide, zirconium carbide, hafnium carbide, vanadium carbide, niobium carbide, tantalum carbide, chromium carbide, carbide The particle diameters of molybdenum and tungsten carbide are each independently 0.01 μm to 10 μm.
A method for making silicon carbide ceramic connectors, using the silicon carbide cladding connecting material described in any one of claims 1 to 5 or the silicon carbide cladding prepared by the preparation method described in any one of claims 6 to 11 connection material.
The manufacturing method of silicon carbide ceramic connector according to claim 12, characterized in that it includes the following steps:

Place the silicon carbide cladding connecting material between the silicon carbide ceramics to be connected to prepare a preform;

The preform is heat treated to prepare the silicon carbide ceramic connector.
The manufacturing method of silicon carbide ceramic connectors according to claim 13, wherein the heat treatment conditions include: a temperature of 1800°C to 2200°C and a pressure of 20MPa to 35MPa.
A silicon carbide ceramic connector produced by the production method described in any one of claims 12 to 14.
A device casing includes the silicon carbide ceramic connector according to claim 15.