A multilayer metal-ceramic composite material and its preparation method and application

Abstract

The present invention belongs to the field of new materials technology, and specifically relates to a multilayer metal-ceramic composite material and its preparation method and application. The multilayer metal-ceramic composite material comprises a rhenium-molybdenum alloy layer, a metal-ceramic transition layer and a SiC f / SiC composite material layer, the metal ceramic transition layer is located between the rhenium-molybdenum alloy layer and the SiC f The multilayered metal-ceramic composite material is obtained by stacking the preforms sequentially between the layers of the SiC composite material and then pressurizing and sintering them. This invention solves the problems of the poor creep properties of current rhenium-molybdenum alloys used in space reactor structures, as well as the poor airtightness and high brittleness of silicon carbide-based composite materials. This multilayered metal-ceramic composite material can be used as a space reactor cladding material, heat pipes, and other structural materials with corresponding needs.

Description

Technical Field

[0001] The present invention belongs to the technical field of new materials, and in particular relates to a multilayer metal-ceramic composite material and a preparation method and application thereof. Background Art

[0002] In the space environment, energy supply is the foundation for the realization of human deep space exploration projects. In this field, not only are there technical requirements for energy systems such as long life and high specific power, but also their safety, especially their performance in the event of accidents, is tested. Nuclear energy has a high energy density, and 1 kg of uranium 235 ( 235 U) fission can release energy equivalent to the combustion of 2,700 metric tons of standard coal. Space nuclear reactor systems offer advantages such as high power, long life, and strong environmental tolerance, making them the preferred energy supply for deep space exploration missions.

[0003] During reactor design and implementation, the selection of nuclear fuel cladding materials is a critical step in its successful application. Nuclear fuel cladding tubes contain nuclear fuel pellets and prevent the release of radioactive fission products through the coolant and ultimately into the external environment. The advent of microreactors has posed new challenges to the performance of nuclear fuel cladding, such as airtightness, high-temperature stability, and high-temperature mechanical strength.

[0004] Zirconium-based alloys are widely used as structural materials in second- and third-generation nuclear reactors, boasting advantages such as a small neutron absorption cross-section, high strength, and corrosion resistance. However, hundreds of ppm of dissolved hydrogen in zirconium alloys can form large amounts of zirconium hydride, significantly degrading the mechanical properties of the structural material. Furthermore, zirconium alloys undergo phase transformations at temperatures above 450°C and react with water at temperatures above 1000°C. This interaction forms zirconium oxide and hydrogen, leading to increased reactor pressure. The mixture of hydrogen and oxygen can cause explosions, seriously endangering the safety of nuclear power systems.

[0005] Accidents at the Three Mile Island nuclear power plant (USA) and the Fukushima-1 nuclear power plant (Japan) due to loss of coolant and reactivity surges demonstrated the true dangers of high-temperature zirconium. Steam reactions led to the formation of explosive hydrogen. These accidents have spurred accelerated development efforts across all nuclear power countries to improve the resistance of zirconium cladding to loss-of-coolant accidents (LOCAs) and to develop more resilient fuels—accident-tolerant fuels (ATFs).

[0006] Compared with zirconium alloy, silicon carbide composite material (SiC f / SiC) has a smaller neutron capture cross section, a higher melting point, radiation resistance, and significantly higher high-temperature oxidation resistance (2-3 orders of magnitude higher), and the use of SiCf / SiC as a core structural material will eliminate the possibility of forming an explosive hydrogen mixture. f / SiC's high brittleness, high porosity and low density restrict its application as a structural material in nuclear reactors. Metallic rhenium has a large thermal neutron absorption cross-section and a small fast neutron absorption cross-section, and has a neutron spectrum shift property, which can protect the reactor from nuclear criticality safety issues in the event of a launch accident. Rhenium-molybdenum alloys with high rhenium content (rhenium content exceeding 50%) reduce the alloy's ductile-brittle transition temperature, giving the composite material an advantage in aerospace applications. However, the creep performance of metallic rhenium is relatively poor, and the introduction of silicon carbide (SiC), an important candidate for future nuclear reactor structural materials, into composite materials can effectively improve the creep performance of structural materials. In addition, both SiC and rhenium have excellent properties such as radiation resistance, high temperature resistance, and corrosion resistance. The metal-ceramic composites composed of them have advantages and potential in use as space reactor ATF structural materials (such as cladding tubes, heat pipes, etc.). Summary of the Invention

[0007] The present invention aims to address the existing problems of poor creep properties of rhenium-molybdenum alloys and the poor airtightness and high brittleness of silicon carbide-based composites by providing a multilayer metal-ceramic composite material, its preparation method, and its application. This material meets the requirements for space reactor use and exhibits neutron spectrum shifting properties, high strength, and excellent sealing properties.

[0008] In order to achieve the above object, the technical solution of the present invention is as follows:

[0009] A multilayer metal-ceramic composite material comprising a rhenium-molybdenum alloy layer, a metal-ceramic transition layer and a SiC f / SiC composite material layer (continuous silicon carbide fiber reinforced silicon carbide based composite material), the metal ceramic transition layer is located between the rhenium molybdenum alloy layer and the SiC f The multilayer metal-ceramic composite material is obtained by stacking the preforms in sequence and then sintering them under pressure between the preforms of the SiC composite material layers.

[0010] Furthermore, in the multilayer metal-ceramic composite material as described above, the rhenium-molybdenum alloy layer is made by sintering evenly mixed molybdenum powder and rhenium powder, with 0wt% < molybdenum content < 50wt%; and the preform thickness of the rhenium-molybdenum alloy layer is 50μm-500μm.

[0011] Furthermore, in the multilayer metal-ceramic composite material as described above, wherein the SiC f The SiC composite material layer comprises at least two SiC matrix layers and at least one SiC fiber layer, wherein the SiC fiber layer is located between the two SiC matrix layers; the SiC fiber content accounts for 10% of the SiC f / 10wt% to 50wt% of the SiC composite material layer.

[0012] Furthermore, the SiC fiber layer is composed of orthogonally woven or orthogonally placed SiC fibers, and the SiC matrix layer is made by sintering SiC powder or pre-ceramic paper with SiC powder as filler; the thickness of the SiC fiber layer is 10μm-100μm, and the fiber volume fraction is 20%-75%; the thickness of the SiC matrix layer is 20μm-500μm.

[0013] Furthermore, in the multilayer metal-ceramic composite material as described above, the metal-ceramic transition layer is composed of a rhenium-molybdenum alloy and SiC, and the metal-ceramic transition layer is formed from the adjacent rhenium-molybdenum alloy layer to the SiC f On the side of the R / SiC composite material layer, the proportion of rhenium-molybdenum alloy gradually decreases, and the proportion of SiC gradually increases.

[0014] Furthermore, the metal ceramic transition layer is formed from the adjacent rhenium-molybdenum alloy layer to the SiC f One side of the SiC / SiC composite material layer is composed of multiple layers with step-by-step increasing silicon carbide molar ratios; the preform thickness of the metal-ceramic transition layer is 100 μm-300 μm.

[0015] Furthermore, each layer of the metal-ceramic transition layer is made of rhenium, molybdenum powder and SiC powder or of pre-ceramic paper with rhenium, molybdenum powder and SiC powder as fillers by sintering.

[0016] Furthermore, the multilayer metal-ceramic composite material as described above is composed of two or more layers of rhenium-molybdenum alloy layers, metal-ceramic transition layers and SiC f The preforms of the / SiC composite material layers are stacked in sequence and then pressurized and sintered.

[0017] The present invention further provides a method for preparing the multilayer metal-ceramic composite material, comprising the following steps:

[0018] 1) Prepare the rhenium-molybdenum alloy layer preform and SiC f / SiC composite material layer preform and metal ceramic transition layer preform;

[0019] 2) The prepared preforms are stacked in order according to the design requirements to obtain a composite material preform, wherein the rhenium-molybdenum alloy layer preform and the SiC f A metal ceramic transition layer preform needs to be placed between the / SiC composite material layer preforms;

[0020] 3) sintering the composite material preform under a set pressure of 100 MPa to 120 MPa, a sintering temperature of 2100° C. to 2200° C., and maintaining time of 2 to 10 minutes to obtain a multi-layer metal-ceramic composite material.

[0021] Furthermore, in the preparation method of the multilayer metal-ceramic composite material as described above, the preparation method of the rhenium-molybdenum alloy layer preform in step 1) includes: mixing molybdenum powder and rhenium powder evenly in a set ratio, pre-sintering into a molybdenum-rhenium pre-sintered body, and then further sintering to form a rhenium-molybdenum alloy foil as the rhenium-molybdenum alloy layer preform.

[0022] Furthermore, in the method for preparing the multilayer metal-ceramic composite material as described above, in step 1) SiC f The preparation method of the SiC composite material layer preform comprises:

[0023] Sintering SiC powder or pre-ceramic paper containing SiC powder as filler to form a SiC matrix layer;

[0024] Placing a SiC fiber layer in which SiC fibers are orthogonally woven or orthogonally placed on a SiC matrix layer;

[0025] A SiC matrix layer is placed on top of the SiC fiber layer.

[0026] Furthermore, in the method for preparing the multilayer metal-ceramic composite material as described above, the method for preparing the metal-ceramic transition layer preform in step 1) includes:

[0027] A multilayer metal-ceramic transition layer preform is formed by sintering rhenium, molybdenum powder and SiC powder uniformly mixed in different set proportions or pre-ceramic paper with rhenium, molybdenum and SiC powder as fillers, wherein each layer of the metal-ceramic transition layer preform has a different molar ratio of silicon carbide;

[0028] The multi-layer metal ceramic transition layer preform is stacked and arranged, and the adjacent rhenium-molybdenum alloy layer is directed to the SiC f The molar ratio of silicon carbide in each metal-ceramic transition layer preform on one side of the / SiC composite material layer increases step by step.

[0029] Furthermore, in the method for preparing the multilayer metal-ceramic composite material as described above, the pre-ceramic paper is a sintered raw material in the form of paper with a specified sintered material powder as a paper filler, and the corresponding material is obtained after high-temperature sintering. The preparation of the pre-ceramic paper includes:

[0030] preparing an aqueous suspension containing a filler and wood pulp or cellulose fibers;

[0031] using polymer additives to coagulate fibers and fillers in the suspension;

[0032] Paper is formed by dehydrating the raw material.

[0033] The present invention further provides the use of the multilayer metal-ceramic composite material as described above, using it as a space stack structural material (such as a cladding tube, a heat pipe).

[0034] The structural material may be a planar structural material (such as a hexagonal tube) or a curved structural material (such as a round tube).

[0035] The beneficial effects of the present invention are as follows:

[0036] 1. The present invention provides a method for preparing a structural material for nuclear reactors having a metal-ceramic composite structure. This method solves the problems of poor creep properties of rhenium-molybdenum alloys and poor airtightness and high brittleness of silicon carbide-based composite materials.

[0037] 2. Rhenium, as a component of space reactor materials, can achieve a neutron spectrum shifting effect, ensuring that nuclear criticality is not compromised in the event of an accident. The introduction of a refractory rhenium layer creates a laminated metal-ceramic composite material with low density, high-temperature and corrosion resistance, and a high degree of structural freedom. It also maintains the creep properties of SiC while retaining the neutron characteristics of rhenium.

[0038] 3. The introduction of a metal layer improves the composite material's ductility and enhances its resistance to sudden impact. Due to the differing properties of these multiple layers of heterogeneous materials, they can redirect incoming objects or metal jets, thus also acting as an outer protective layer for improved protection.

[0039] 4. The introduction of rhenium-molybdenum alloy with a rhenium content of more than 50% reduces the ductile-brittle transition temperature of the alloy, giving the composite material an advantage in application in the aerospace field.

[0040] 5. The sintered raw materials are used as paper fillers to make pre-ceramic paper, which is then sintered under pressure and high temperature to obtain a preparation process for a metal-ceramic composite material with a laminated structure. This is conducive to quickly and economically obtaining high-performance structural materials with complex geometric shapes. By sintering the pre-ceramic paper, it is easy to obtain a metal-ceramic transition layer with a specified metal and ceramic content gradient. BRIEF DESCRIPTION OF THE DRAWINGS

[0041] Figure 1 Schematic diagram of the preparation process of the multilayer metal-ceramic composite material of the present invention;

[0042] Figure 2 Schematic diagram of the process flow of the multilayer metal-ceramic composite material of the present invention;

[0043] Figure 3 This is a schematic structural diagram of a preform of a space pile structural material in Example 1 of the present invention;

[0044] Figure 4This is a schematic structural diagram of the space pile structural material preform in Example 2 of the present invention. DETAILED DESCRIPTION

[0045] In order to make the purpose, technical solutions and advantages of the present invention more clearly understood, the present invention will be further described in detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are only used to explain the present invention and are not intended to limit the present invention.

[0046] The present invention aims to provide a multilayer metal-ceramic composite material that meets the requirements for use in space reactors, has neutron spectrum shift characteristics, high strength, and good sealing. Figure 1 As shown, the multilayer metal-ceramic composite material includes a rhenium-molybdenum alloy layer, a metal-ceramic transition layer and a SiC f / SiC composite material layer (continuous silicon carbide fiber reinforced silicon carbide based composite material), SiC f The / SiC composite material layer includes at least two SiC matrix layers and at least one SiC fiber layer, and the metal ceramic transition layer is located between the rhenium-molybdenum alloy layer and the SiC f / SiC composite material layers, each preform is stacked in a required order and then pressure-sintered in a graphite mold to obtain the multi-layer metal-ceramic composite material.

[0047] The rhenium-molybdenum alloy layer is prepared by sintering rhenium powder and molybdenum powder uniformly mixed in a required proportion, wherein 0wt% < molybdenum content < 50wt%; the preform thickness of the rhenium-molybdenum alloy layer can be 50μm-500μm.

[0048] The SiC f The SiC composite material layer is composed of an alternating SiC matrix layer and a SiC fiber layer, wherein the SiC fiber layer is located between the two SiC matrix layers. The SiC matrix layer is made of SiC powder or pre-ceramic paper with SiC powder as filler by sintering, and the thickness of each layer can be 20μm-500μm. The SiC fiber layer is composed of orthogonally woven or orthogonally placed SiC fibers, and the thickness of the SiC fiber layer can be 10μm-100μm, with a fiber volume fraction of 20%-75%, and the SiC fiber content accounts for 10% of the SiC f / 10wt% to 50wt% of the SiC composite material layer.

[0049] The metal ceramic transition layer is composed of rhenium-molybdenum alloy and SiC, and the metal ceramic transition layer is formed from the adjacent rhenium-molybdenum alloy layer to the SiC f On one side of the / SiC composite material layer, the proportion of the rhenium-molybdenum alloy gradually decreases, and the proportion of SiC gradually decreases and increases. Specifically, the metal-ceramic transition layer is formed from the adjacent rhenium-molybdenum alloy layer to the SiC fOne side of the SiC / SiC composite material layer is composed of multiple layers with step-by-step increasing silicon carbide molar ratios, and the total thickness of the metal-ceramic transition layer can be 100 μm-300 μm.

[0050] Each layer of the metal-ceramic transition layer can be made by sintering rhenium, molybdenum powder and SiC powder in a specified ratio or by sintering pre-ceramic paper with rhenium, molybdenum powder and SiC powder as fillers.

[0051] It should be clear to those skilled in the art that the thickness of each layer of the preform can be determined as needed, and the above thickness range is only exemplary and not restrictive.

[0052] like Figure 2 As shown, the present invention further provides a method for preparing the above-mentioned multilayer metal-ceramic composite material, comprising the following steps:

[0053] 1) Prepare the rhenium-molybdenum alloy layer preform and SiC f / SiC composite material layer preform (including SiC matrix layer preform and SiC fiber layer preform) and metal ceramic transition layer preform;

[0054] 2) The prepared preforms are stacked in order according to the design requirements to obtain a composite material preform, wherein the rhenium-molybdenum alloy layer preform and the SiC f A metal ceramic transition layer preform needs to be placed between the / SiC composite material layer preforms;

[0055] 3) sintering the composite material preform under a set pressure of 100 MPa to 120 MPa, a sintering temperature of 2100° C. to 2200° C., and maintaining time of 2 to 10 minutes to obtain a multilayer metal-ceramic composite material with neutron spectrum shift characteristics.

[0056] Furthermore, in the preparation method of the above-mentioned multilayer metal-ceramic composite material, the preparation method of the rhenium-molybdenum alloy layer preform includes: mixing molybdenum powder and rhenium powder evenly in a set ratio, the particle size of the molybdenum powder and the rhenium powder can be between 2 and 50 microns, pre-sintering into a molybdenum-rhenium pre-sintered body, and then further sintering at a high temperature to form a rhenium-molybdenum alloy foil as the rhenium-molybdenum alloy layer preform.

[0057] Furthermore, in the preparation method of the multilayer metal-ceramic composite material, SiC f The preparation method of the SiC composite material layer preform comprises:

[0058] The SiC matrix layer is formed by sintering SiC powder or pre-ceramic paper with SiC powder as filler, wherein the particle size of the SiC powder can be between 1 and 5 microns;

[0059] Placing a SiC fiber layer in which SiC fibers are orthogonally woven or orthogonally placed on a SiC matrix layer;

[0060] A SiC matrix layer is placed on top of the SiC fiber layer.

[0061] Furthermore, in the above-mentioned method for preparing the multilayer metal-ceramic composite material, the method for preparing the metal-ceramic transition layer preform includes:

[0062] A multilayer metal-ceramic transition layer preform is formed by sintering rhenium, molybdenum powder and SiC powder uniformly mixed in different set proportions or pre-ceramic paper with rhenium, molybdenum and SiC powder as fillers, wherein each layer of the metal-ceramic transition layer preform has a different molar ratio of silicon carbide;

[0063] The multi-layer metal ceramic transition layer preform is stacked and arranged, and the adjacent rhenium-molybdenum alloy layer is directed to the SiC f The molar ratio of silicon carbide in each metal-ceramic transition layer preform on one side of the / SiC composite material layer increases step by step.

[0064] In the above technical solution, a pre-ceramic paper sintering process can be used to prepare the SiC matrix layer and the metal-ceramic transition layer. The pre-ceramic paper is a sintered raw material in the form of paper using a specified powder as the paper filler, and the corresponding material is produced after high-temperature sintering. The preparation process of the pre-ceramic paper includes: preparing an aqueous suspension containing filler and wood pulp or cellulose fiber, using a polymer additive to coagulate the fibers and filler in the suspension, and forming the paper by dehydrating the raw material. Pre-ceramic paper can provide greater operational convenience than powder alone. Specific preparation methods can be found in documents such as "Study on the Preparation of Silicon Carbide Composite Materials Using a Novel Ceramic Paper Substrate."

[0065] The method for preparing the multilayer metal-ceramic composite material provided by the present invention can prepare planar structural materials (such as hexagonal tubes) or curved structural materials (such as round tubes).

[0066] The above-mentioned multilayer metal-ceramic composite material can be used as a structural material (such as cladding tubes, heat pipes) in space reactors, and can also be used in other fields with corresponding needs.

[0067] Example 1

[0068] In this embodiment, the space stack structure material is composed of a rhenium-molybdenum alloy layer 1, a metal-ceramic transition layer 2 and a SiC f / SiC composite material layer, the SiC f The SiC composite material layer is composed of an alternating SiC matrix layer 3 and a SiC fiber layer 4. The SiC fiber layer 4 is located between two SiC matrix layers 3. In this embodiment, there are three SiC matrix layers 3 and two SiC fiber layers 4. The specific structure is as follows: Figure 3 shown.

[0069] The specific preparation method of the multilayer structure material is as follows:

[0070] Step 1): Molybdenum powder and rhenium powder are uniformly mixed, wherein the weight percentage of molybdenum is 49%, and pre-sintered into a molybdenum-rhenium pre-sintered body, and then sintered at 2100° C. to form a rhenium-molybdenum alloy foil with a thickness of 100 μm as a rhenium-molybdenum alloy layer preform;

[0071] Step 2): SiC fibers are orthogonally woven in two dimensions with a weaving thickness of 15 μm and a fiber volume fraction of 50% to form a SiC fiber layer preform;

[0072] Step 3): preparing an aqueous suspension containing SiC powder and wood pulp or cellulose fibers, coagulating the fibers and fillers in the suspension using a polymer additive, and forming a pre-ceramic paper having a thickness of 300 μm and a SiC mass fraction of 50% by dehydrating the raw materials, as a SiC matrix layer preform;

[0073] Step 4): The molybdenum powder and rhenium powder uniformly mixed in step 1) were mixed with SiC powder in molar ratios of 3:1, 1:1, and 1:3, respectively, and used as fillers. Three sets of pre-ceramic paper with a thickness of 100 μm were prepared according to the method of step 3 to serve as metal-ceramic transition layer preforms;

[0074] Step 5): Cut the preforms prepared in steps 1), 2), 3) and 4) into discs with a diameter of 20 mm;

[0075] Step 6): placing the rhenium-molybdenum alloy layer preform prepared in step 1) on the bottom layer of the graphite mold;

[0076] Step 7): placing the three groups of metal-ceramic transition layer preforms prepared in step 4) on the preforms prepared in step 6) in descending order of rhenium-molybdenum alloy content;

[0077] Step 8): placing the SiC substrate layer preform prepared in step 3) on the preform prepared in step 7);

[0078] Step 9): placing the SiC fiber layer preform prepared in step 2) on the preform prepared in step 8);

[0079] Step 10): further placing the SiC matrix layer preform prepared in step 3) and the SiC fiber layer preform prepared in step 2) on the preform prepared in step 9) in sequence;

[0080] Step 11): placing the SiC substrate layer preform prepared in step 3) on the preform prepared in step 10);

[0081] Step 12): The preform obtained in step 11) is subjected to spark plasma sintering (such as Figure 1As shown), the sintering pressure is 100 MPa, the sintering temperature is 2200° C., and the temperature is maintained for 3 minutes to obtain a multi-layer structure material with a thickness of 700 μm.

[0082] Example 2

[0083] In this embodiment, the space stack structure material is composed of a rhenium-molybdenum alloy layer 1, a metal-ceramic transition layer 2 and a SiC f / SiC composite material layer cycle, the SiC f The SiC composite material layer is composed of an alternating SiC matrix layer 3 and a SiC fiber layer 4, wherein the SiC fiber layer 4 is located between two SiC matrix layers 3. In this embodiment, the composite material layer comprises two layers of rhenium-molybdenum alloy 1, three layers of metal-ceramic transition layer 2, and two layers of SiC f / SiC composite material layer, the specific structure is as follows Figure 4 shown.

[0084] The specific preparation method of the multilayer structure material is as follows:

[0085] Step 1): Molybdenum powder and rhenium powder are uniformly mixed, wherein the weight percentage of molybdenum is 20%, and pre-sintered into a molybdenum-rhenium pre-sintered body, and then sintered at 2100° C. to form a rhenium-molybdenum alloy foil with a thickness of 50 μm as a rhenium-molybdenum alloy layer preform;

[0086] Step 2): SiC fibers are orthogonally woven in two dimensions with a weaving thickness of 15 μm and a fiber volume fraction of 20% to form a SiC fiber layer preform;

[0087] Step 3): preparing an aqueous suspension containing SiC powder and wood pulp or cellulose fibers, coagulating the fibers and fillers in the suspension using a polymer additive, and forming a pre-ceramic paper with a thickness of 200 μm and a SiC mass fraction of 50% by dehydrating the raw materials to serve as a SiC matrix layer preform;

[0088] Step 4): The molybdenum powder and rhenium powder uniformly mixed in step 1) were mixed with SiC powder in molar ratios of 4:1, 3:2, 2:3, and 1:4, respectively, and used as fillers. Four sets of pre-ceramic paper with a thickness of 50 μm were prepared according to the method of step 3 to serve as metal-ceramic transition layer preforms;

[0089] Step 5): Cut the preforms prepared in steps 1), 2), 3) and 4) into discs with a diameter of 20 mm;

[0090] Step 6): placing the rhenium-molybdenum alloy layer preform prepared in step 1) on the bottom layer of the graphite mold;

[0091] Step 7): placing the four groups of metal-ceramic transition layer preforms prepared in step 4) on the preforms prepared in step 6) in descending order of rhenium-molybdenum alloy content;

[0092] Step 8): placing the SiC substrate layer preform prepared in step 3) on the preform prepared in step 7);

[0093] Step 9): placing the SiC fiber layer preform prepared in step 2) on the preform prepared in step 8);

[0094] Step 10): placing the SiC substrate layer preform prepared in step 3) on the preform prepared in step 9);

[0095] Step 11): placing the four groups of metal-ceramic transition layer preforms prepared in step 4) on the preforms prepared in step 10) in order of metal content from low to high;

[0096] Step 12): placing the rhenium-molybdenum alloy layer preform prepared in step 1) on the preform prepared in step 11);

[0097] Step 13): Repeat steps 7) to 10) once on the preform of step 12);

[0098] Step 14): The preform obtained in step 13) is subjected to spark plasma sintering (such as Figure 1 As shown), the sintering pressure is 120 MPa, the sintering temperature is 2100°C, and the temperature is maintained for 7 minutes to obtain a multi-layer structure material with a thickness of 700 μm.

[0099] Those skilled in the art will readily identify other embodiments of the present invention after considering the specification and practicing the invention disclosed herein. This application is intended to cover any variations, uses, or adaptations of the present invention that follow the general principles of the present invention and include common knowledge or customary techniques in the art not disclosed herein. Thus, if such variations, uses, or adaptations of the present invention fall within the scope of the claims and their equivalents, the present invention is intended to encompass such variations and uses.

[0100] The above embodiments are merely illustrative of the present invention. The present invention may also be implemented in other specific ways or in other specific forms without departing from the gist or essential features of the present invention. Therefore, the described embodiments should be considered in all respects as illustrative rather than restrictive. The scope of protection of the present invention should be described by the claims, and any variations that are equivalent to the intent and scope of the claims should also be included within the scope of protection of the present invention.

Claims

1. A multilayer metal-ceramic composite material, characterized in that: Including rhenium-molybdenum alloy layer, metal-ceramic transition layer and SiC f / SiC composite material layer, the metal ceramic transition layer is located between the rhenium-molybdenum alloy layer and the SiC f Between the layers of / SiC composite materials, the metal-ceramic transition layer is composed of rhenium-molybdenum alloy and SiC, and the metal-ceramic transition layer is composed of rhenium-molybdenum alloy and SiC. f On one side of the / SiC composite material layer, the proportion of the rhenium-molybdenum alloy gradually decreases, and the proportion of SiC gradually decreases and increases. The preforms of each layer are stacked in sequence and then pressurized and sintered to obtain the multilayer metal-ceramic composite material.

2. The multilayer metal-ceramic composite material according to claim 1, wherein: The rhenium-molybdenum alloy layer is made by sintering evenly mixed molybdenum powder and rhenium powder, with 0wt% < molybdenum content < 50wt%; the preform thickness of the rhenium-molybdenum alloy layer is 50μm-500μm.

3. The multilayer metal-ceramic composite material according to claim 1, wherein: The SiC f The SiC composite material layer comprises at least two SiC matrix layers and at least one SiC fiber layer, wherein the SiC fiber layer is located between the two SiC matrix layers; the SiC fiber content accounts for 10% of the SiC f / 10wt% to 50wt% of the SiC composite material layer.

4. The multilayer metal-ceramic composite material according to claim 3, wherein: The SiC fiber layer is composed of orthogonally woven or orthogonally placed SiC fibers, and the SiC matrix layer is made by sintering SiC powder or pre-ceramic paper with SiC powder as filler.

5. The multilayer metal-ceramic composite material according to claim 4, wherein: The thickness of the SiC fiber layer is 10 μm-100 μm, and the fiber volume fraction is 20%-75%; the thickness of the SiC matrix layer is 20 μm-500 μm.

6. The multilayer metal-ceramic composite material according to claim 1, wherein: The metal ceramic transition layer is formed from the adjacent rhenium-molybdenum alloy layer to the SiC f One side of the SiC / SiC composite material layer is composed of multiple layers with step-by-step increasing silicon carbide molar ratios; the preform thickness of the metal-ceramic transition layer is 100 μm-300 μm.

7. The multilayer metal-ceramic composite material according to claim 6, wherein: Each layer of the metal ceramic transition layer is made by sintering rhenium, molybdenum powder and SiC powder or pre-ceramic paper with rhenium, molybdenum powder and SiC powder as fillers.

8. The multilayer metal-ceramic composite material according to any one of claims 1 to 7, characterized in that: It consists of two or more layers of rhenium-molybdenum alloy, metal-ceramic transition layer and SiC f The preforms of the / SiC composite material layers are stacked in sequence and then pressurized and sintered.

9. A method for preparing the multilayer metal-ceramic composite material according to any one of claims 1 to 8, comprising the following steps: 1) Prepare the rhenium-molybdenum alloy layer preform and SiC f / SiC composite material layer preform and metal ceramic transition layer preform; 2) stacking the prepared preforms in order according to the design requirements to obtain a composite material preform, wherein: Rhenium-molybdenum alloy layer preform and SiC f A metal ceramic transition layer preform needs to be placed between the / SiC composite material layer preforms; 3) sintering the composite material preform under a set pressure of 100 MPa to 120 MPa, a sintering temperature of 2100° C. to 2200° C., and maintaining time of 2 to 10 minutes to obtain a multi-layer metal-ceramic composite material.

10. The method for preparing a multilayer metal-ceramic composite material according to claim 9, wherein: The preparation method of the rhenium-molybdenum alloy layer preform in step 1) includes: mixing molybdenum powder and rhenium powder in a set ratio, pre-sintering into a molybdenum-rhenium pre-sintered body, and then further sintering to form a rhenium-molybdenum alloy foil as the rhenium-molybdenum alloy layer preform.

11. The method for preparing a multilayer metal-ceramic composite material according to claim 9, wherein: Step 1) SiC f The preparation method of the SiC composite material layer preform comprises: Sintering SiC powder or pre-ceramic paper containing SiC powder as filler to form a SiC matrix layer; Placing a SiC fiber layer in which SiC fibers are orthogonally woven or orthogonally placed on a SiC matrix layer; A SiC matrix layer is placed on top of the SiC fiber layer.

12. The method for preparing a multilayer metal-ceramic composite material according to claim 9, wherein: The method for preparing the metal-ceramic transition layer preform in step 1) includes: A multilayer metal-ceramic transition layer preform is formed by sintering rhenium, molybdenum powder and SiC powder uniformly mixed in different set proportions or pre-ceramic paper with rhenium, molybdenum and SiC powder as fillers, wherein each layer of the metal-ceramic transition layer preform has a different molar ratio of silicon carbide; The multi-layer metal ceramic transition layer preform is stacked and arranged, and the adjacent rhenium-molybdenum alloy layer is directed to the SiC f The molar ratio of silicon carbide in each metal-ceramic transition layer preform on one side of the / SiC composite material layer increases step by step.

13. The method for preparing the multilayer metal-ceramic composite material according to claim 11 or 12, characterized in that: The pre-ceramic paper is a sintered raw material in the form of paper with a specified sintered material powder as the paper filler. The corresponding material is obtained after high-temperature sintering. The preparation of the pre-ceramic paper includes: preparing an aqueous suspension containing a filler and cellulose fibers; using polymer additives to coagulate fibers and fillers in the suspension; Paper is formed by dehydrating the raw material.

14. Use of the multilayer metal-ceramic composite material according to any one of claims 1 to 8, characterized in that: Use it as a space stack structural material.

15. Use of the multilayer metal-ceramic composite material according to claim 14, characterized in that: The structural material is a planar structural material or a curved structural material.

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