Multi-scale structure ceramic matrix composite material and preparation method thereof

Abstract

The invention relates to a multi-scale structure ceramic matrix composite material and a preparation method thereof. The method comprises the following steps: dispersing graphene oxide in deionized water to obtain a graphene oxide suspension; carrying out suction filtration on the graphene oxide suspension to the surface of a microporous filter membrane by a vacuum suction filtration method to obtain a layered graphene oxide membrane; taking at least one layered graphene oxide film as a layered prefabricated body, and depositing an interface layer in the layered prefabricated body through a chemical vapor infiltration method to obtain the layered prefabricated body deposited with the interface layer; and taking a ceramic precursor solution as a reactant, performing matrix densification on the layered preform deposited with the interface layer through an impregnation and pyrolysis method, and performing high-temperature treatment to obtain the multi-scale structure ceramic matrix composite material. The strength and toughness of the ceramic-based composite material are synchronously and greatly improved, and the prepared ceramic-based composite material has excellent high-temperature-resistant mechanical performance and can be used for high-performance bearing type complex profile structural parts.

Description

Technical Field

[0001] This invention belongs to the field of ceramic matrix composite material preparation technology, and particularly relates to a multi-scale structure ceramic matrix composite material and its preparation method. Background Technology

[0002] With the rapid development of high-end equipment manufacturing and other fields, stringent requirements have been placed on the service performance of key hot-end structural components under extreme high temperatures, high stresses, and complex environments. Ceramic matrix composites, due to their high temperature resistance, oxidation resistance, and low density, are considered ideal candidate materials to replace traditional high-temperature alloys.

[0003] However, structural components place increasingly higher demands on the high-temperature resistance and mechanical properties of ceramic matrix composites (CMCs). Traditional CMC structures are insufficient to meet these requirements, necessitating structural design to enhance their service performance. Conventional methods using carbon fiber as reinforcement often limit the improvement of mechanical properties; therefore, there is an urgent need to develop a multi-scale structural CMC and its preparation method. Summary of the Invention

[0004] To address one or more technical problems existing in the prior art, this invention provides a multi-scale structural ceramic matrix composite material and its preparation method. This invention enables a simultaneous and significant improvement in the strength and toughness of the ceramic matrix composite material. The ceramic matrix composite material prepared by this invention exhibits excellent high-temperature mechanical properties and can be used for high-performance load-bearing complex surface structures.

[0005] The present invention provides a method for preparing a multi-scale structured ceramic matrix composite material in a first aspect, the method comprising the following steps: (1) Graphene oxide is dispersed in deionized water to obtain a graphene oxide suspension; (2) The graphene oxide suspension was filtered onto the surface of a microporous membrane by vacuum filtration to obtain a layered graphene oxide membrane. (3) Using at least one layer of layered graphene oxide film as a layered preform, an interface layer is deposited in the layered preform by chemical vapor infiltration to obtain a layered preform with an interface layer deposited. (4) Using ceramic precursor solution as reactant, the matrix densification of the layered preform with the deposited interface layer is carried out by impregnation pyrolysis method, and then high temperature treatment is performed to prepare multi-scale structure ceramic matrix composite material.

[0006] Preferably, in step (1): the concentration of the graphene oxide suspension is 1-5 mg / mL; and / or the graphene oxide is dispersed in deionized water by ultrasonic treatment.

[0007] Preferably, the ultrasonic treatment power is 300-500W, and the ultrasonic treatment time is 1-2 hours.

[0008] Preferably, the ultrasonic treatment is pulsed ultrasonic treatment, and the power density of the pulsed ultrasonic treatment is 80-150 W / cm². 2 The pulse duration is 20-30 seconds, the duty cycle is 60-80%, and the pulse ultrasound treatment time is 1-2 hours.

[0009] Preferably, in step (2): the pore size of the microporous filter membrane is 0.2-0.3 μm; and / or the microporous filter membrane is a microporous nylon filter membrane.

[0010] Preferably, in step (2): the thickness of the single-layer layered graphene oxide membrane is 5-50 μm; the filtration is performed under a vacuum of -0.08 to -0.095 MPa; and / or during filtration, the graphene oxide suspension is added to the microporous filter membrane at a dropping rate of 0.5-2 mL / min for vacuum filtration, so that the graphene oxide is stacked layer by layer on the surface of the microporous filter membrane to obtain the layered graphene oxide membrane.

[0011] Preferably, in step (3): the thickness of the layered preform is 4-6 mm; the interface layer is a pyrolytic carbon interface layer and / or a boron nitride interface layer; when depositing the pyrolytic carbon interface layer, propane is used as the reaction source gas, the propane flow rate is 50-200 sccm, the deposition temperature is 950-1050℃, the deposition pressure is 1-5 kPa, and the deposition time is 0.5-2 h. Preferably, the thickness of the pyrolytic carbon interface layer is 50-150 nm; when depositing the boron nitride interface layer, boron trichloride and ammonia are used as the reaction source gases, the molar ratio of boron trichloride to ammonia is 1:(3-5), the deposition temperature is 900-1100℃, the deposition pressure is 0.5-2 kPa, and the deposition time is 0.5-2 h. Preferably, the thickness of the boron nitride interface layer is 30-100 nm.

[0012] Preferably, in step (4): the ceramic precursor solution is a silicon carbide ceramic precursor solution; the temperature of the high-temperature treatment is 1400-1600℃ and the time is 0.5-1.5h; and / or the high-temperature treatment is carried out in an inert atmosphere, preferably an argon atmosphere.

[0013] Preferably, step (4) includes the following sub-steps: (a) vacuum impregnating the layered preform with the deposited interface layer using a ceramic precursor solution, and then curing and high-temperature pyrolysis; preferably, the curing temperature is 150-350℃, the curing time is 1-3h, the high-temperature pyrolysis temperature is 1000-1500℃, the time is 1-3h, and the heating rate is 2-5℃ / min; (b) repeating step (a) multiple times, preferably repeating step (a) more than 10 times; (c) subjecting the material obtained in step (b) to high-temperature treatment to obtain the multi-scale structure ceramic matrix composite material.

[0014] In a second aspect, the present invention provides a multi-scale structured ceramic matrix composite material, which is prepared using the preparation method described in the first aspect of the present invention.

[0015] Compared with the prior art, the present invention has at least the following beneficial effects: This invention simulates the "brick-and-mortar" structure of natural nacre, utilizing two-dimensional nanomaterials (two-dimensional GO nanosheets) as "bricks" and bonding them to the ceramic matrix "mortar" through weak interfaces. This constructs a toughening structure at the nano / micro scale capable of guiding large-scale crack deflection and bridging, thereby achieving a simultaneous and significant improvement in the strength and toughness of the ceramic matrix composite material. The ceramic matrix composite material prepared by this invention exhibits excellent high-temperature mechanical properties and can be used for high-performance load-bearing complex surface structures. Detailed Implementation

[0016] To make the objectives, technical solutions, and advantages of this invention clearer, the technical solutions of this invention will be clearly and completely described below in conjunction with the embodiments of this invention. Obviously, the described embodiments are only some, not all, of the embodiments of this invention. All other embodiments obtained by those skilled in the art based on the embodiments of this invention without creative effort are within the scope of protection of this invention.

[0017] The present invention provides a method for preparing a multi-scale structured ceramic matrix composite material in a first aspect, the method comprising the following steps: (1) Graphene oxide is dispersed in deionized water to obtain a graphene oxide suspension (also referred to as GO suspension). This step (1) completes the preparation of the "brick" suspension. The present invention does not specifically limit the graphene oxide. Products that can be purchased directly or products prepared by existing methods can be used. In some specific embodiments, graphite powder (e.g., high-purity graphite powder) can be used as raw material to prepare graphene oxide powder using the improved Hummers method in the prior art. Then, the graphene oxide powder is dispersed in deionized water to form a uniformly dispersed GO suspension. (2) The graphene oxide suspension is filtered to the surface of the microporous filter membrane by vacuum filtration (also known as vacuum-assisted filtration) to obtain a layered graphene oxide membrane (also known as a layered GO membrane); In step (2), the vacuum-assisted filtration method is used to form a layered GO membrane with a highly consistent orientation, which is to obtain a macroscopic aggregate of "bricks"; The layered graphene oxide obtained by this invention is a self-supporting layered GO membrane. After the layered graphene oxide membrane is prepared and peeled off from the filter membrane, it can maintain its own shape and integrity without relying on any external substrate or framework; (3) Using at least one layer of layered graphene oxide film as a layered preform (also referred to as a biomimetic layered preform), an interface layer is deposited in the layered preform by chemical vapor infiltration (CVI) to obtain a layered preform with an interface layer deposited thereon; In this invention, when the layered preform includes multiple (two or more) layered graphene oxide films, the layered preform is formed by stacking multiple layered graphene oxide films; In this step (3), a weak interface layer is introduced by CVI, and the layered preform is placed in a chemical vapor infiltration (CVI) reactor to deposit an ultra-weak interface layer with controllable thickness on its surface; (4) Using a ceramic precursor solution (e.g., a silicon carbide ceramic precursor solution) as a reactant, the layered preform with the deposited interface layer is densified by the impregnation pyrolysis method (PIP process), and then subjected to high temperature treatment to prepare a multi-scale structure (nano / micron scale structure) ceramic matrix composite material (abbreviated as ceramic matrix composite material); In this step (4), the PIP process is used to penetrate the matrix (e.g., SiC matrix) "slurry": the layered preform with the deposited interface layer is impregnated in the ceramic precursor solution, and a ceramic matrix is ​​formed by multiple rounds of impregnation-curing-pyrolysis, and finally subjected to high temperature treatment to promote the sintering of the ceramic matrix.

[0018] This invention simulates the "brick-and-mortar" structure of natural nacre, utilizing two-dimensional nanomaterials (two-dimensional GO nanosheets) as "bricks" and bonding them to a ceramic matrix "mortar" through weak interfaces. This constructs a toughening structure at the nano / micron scale (the ceramic matrix after the pyrolysis of the ceramic precursor is at the micron scale), capable of guiding large-scale crack deflection and bridging, thereby achieving a simultaneous and significant improvement in the strength and toughness of the ceramic matrix composite material. The ceramic matrix composite material prepared by this invention exhibits excellent high-temperature mechanical properties and can be used for high-performance load-bearing complex surface structures.

[0019] According to some preferred embodiments, in step (1): the concentration of the graphene oxide suspension is 1-5 mg / mL (e.g., 1, 2, 3, 4 or 5 mg / mL); and / or the graphene oxide is dispersed in deionized water by ultrasonic treatment.

[0020] According to some preferred embodiments, the ultrasonic power is 300-500W, and the ultrasonic treatment time is 1-2h.

[0021] According to some specific implementation methods, step (1) is as follows: graphene oxide powder is prepared by using graphite powder (high-purity graphite powder) as raw material and the modified Hummers method. Then, the graphene oxide powder is dispersed in deionized water by ultrasonic treatment to form a uniformly dispersed GO suspension. The concentration of the graphene oxide suspension is 1-5 mg / mL, the power of the ultrasonic treatment is 300-500 W, and the treatment time is 1-2 h.

[0022] According to some preferred embodiments, the ultrasonic treatment is pulsed ultrasonic treatment, and the power density (sound intensity) of the pulsed ultrasonic treatment is 80-150 W / cm². 2 (e.g., 80, 90, 100, 110, 120, 130, 140 or 150 W / cm) 2 The pulse duration is 20-30s (e.g., 20, 25, or 30s), the duty cycle is 60-80% (e.g., 60%, 65%, 70%, 75%, or 80%), and the pulse ultrasound treatment time is 1-2h (e.g., 1, 1.5, or 2h); the power of the pulse ultrasound treatment is 300-500W; the frequency of the pulse ultrasound treatment is 15-40kHz; in a specific embodiment of the present invention, for example, a probe-type pulse ultrasound is used. Specifically, during pulse ultrasound, the probe of a probe-type pulse ultrasound instrument is inserted into the system, for example, with a working time of 30s and an interval of 10s (duty cycle 75%), that is, during pulse ultrasound, the pulse ultrasound is performed with a 10s interval for 30s.

[0023] In this invention, pulsed ultrasound treatment is preferably used to disperse graphene oxide in deionized water. This plays a crucial role in achieving a simultaneous and significant improvement in the strength and toughness of the ceramic matrix composite material. Pulsed ultrasound, through intermittent high-energy output and cooling cycles, can effectively exfoliate graphene oxide powder into single-layer and / or few-layer GO nanosheets, allowing these nanosheets to fully expand and stably suspend in the solvent. Simultaneously, it minimizes damage to the sheet structure (such as tearing or excessive fragmentation) and / or chemical structure destruction (loss of oxygen-containing functional groups) caused by continuous thermal effects and excessive cavitation shear forces. This ensures that the GO nanosheets, as the core "building blocks," possess a complete two-dimensional morphology and a large lateral dimension. This lays the foundation for the subsequent construction of highly ordered, controllable layered graphene oxide films. If conventional continuous high-power-density ultrasound treatment is used, the continuous and intense cavitation and local overheating can easily cause the GO sheets to become over-layered. The fragmentation, size reduction, and increased defects in the self-assembled membrane structure lead to a decrease in its orderliness and a deterioration in its mechanical properties. This may also weaken the synergistic toughening effect between the self-assembled membrane structure and the subsequent deposited interface layer and ceramic matrix, ultimately affecting the simultaneous improvement of the strength and toughness of the ceramic matrix composite. Conventional low-power density ultrasonic treatment is also difficult to achieve the same effect. The energy input provided by low-power density ultrasound is limited, and its cavitation effect and shear force are weak, which cannot fully and uniformly peel it into single-layer and / or few-layer GO nanosheets. This results in the presence of many unpeeled thick sheets or agglomerates in the suspension, making the subsequent layered graphene oxide membrane structure formed by vacuum filtration uneven and poorly compact. These structural defects directly weaken the load-bearing capacity and uniformity of the "bricks," ultimately leading to a decrease in the crack deflection and bridging ability of the ceramic matrix composite at the nano / micro scale, and failing to achieve a simultaneous and significant improvement in strength and toughness.

[0024] In this invention, a graphene oxide suspension with a concentration of 1-5 mg / mL is preferably obtained by pulsed ultrasonic treatment. This concentration range is beneficial to ensure that the graphene oxide sheets are fully exfoliated and stably dispersed, avoiding insufficient sheet quantity and difficulty in forming a continuous structure due to too low a concentration; it can also prevent problems such as increased suspension viscosity and easy re-agglomeration of sheets caused by too high a concentration, effectively avoiding problems such as dispersion defects, decreased fluidity or uneven coating.

[0025] According to some preferred embodiments, in step (2): the pore size of the microporous filter membrane is 0.2-0.3 μm (e.g., 0.2, 0.22, 0.24, 0.26, 0.28, or 0.3 μm); in this invention, it is preferred to use a microporous filter membrane with a pore size of 0.2-0.3 μm, which can effectively trap graphene oxide sheets, which is beneficial to ensure that graphene oxide sheets (two-dimensional GO nanosheets) are stacked layer by layer on the filter membrane surface, forming a dense and uniform layered graphene oxide film structure on the filter membrane, while allowing the solvent to pass through quickly, ensuring the filtration efficiency; this invention has found that if the pore size is too large, it can This can lead to the graphene oxide sheets penetrating or becoming loosely packed, making it difficult to form a continuous and complete layered graphene oxide membrane; if the pore size is too small, it will reduce the filtration rate, prolong the process time, and may cause sheet deformation due to excessive filtration resistance, ultimately affecting the precise construction of the "brick-slurry" and thus the mechanical properties of the resulting ceramic matrix composite material; and / or the microporous filter membrane is a microporous nylon filter membrane, the flexibility and chemical stability of which can avoid structural damage when the graphene oxide membrane is detached from the filter membrane; in this invention, the graphene oxide membrane is detached from the filter membrane before performing the CVI process.

[0026] According to some preferred embodiments, in step (2): the thickness of the single-layer layered graphene oxide membrane is 5-50 μm; the filtration is performed under a vacuum of -0.08 to -0.095 MPa; and / or during the filtration, the graphene oxide suspension is added to the microporous filter membrane at a dropping rate of 0.5-2 mL / min for vacuum filtration, so that the graphene oxide is stacked layer by layer on the surface of the microporous filter membrane to obtain the layered graphene oxide membrane. In this invention, the preferred method is to use a graphene oxide suspension for vacuum filtration at a dropping rate of 0.5-2 mL / min. This allows the sheets to be stacked in an orderly, layer-by-layer uniform manner on the surface of the microporous filter membrane, thereby forming a dense and highly oriented layered graphene oxide membrane. This avoids potential localized agglomeration or uneven stacking of the sheets and ensures timely solvent removal, providing an ideal two-dimensional substrate for constructing the "brick" structure. This is beneficial for improving the strength and toughness of ceramic matrix composites. However, if the dropping rate is too fast, the graphene oxide suspension may not have enough time to spread and dry evenly on the filter membrane surface, which can easily lead to disordered sheet stacking, uneven film thickness, or defects. On the other hand, if the dropping rate is too slow, it will significantly prolong the process time, and the semi-dry state of the filtration interface for a long time may cause localized shrinkage or wrinkling of the deposited graphene oxide sheets, which is also not conducive to forming a flat and continuous layered structure.

[0027] According to some specific implementation methods, step (2) is as follows: using vacuum-assisted filtration, the prepared GO suspension is slowly added dropwise (the adding speed is, for example, 0.5-2 mL / min) to a filtration device with a microporous filter membrane (such as a microporous nylon membrane with a pore size of 0.22 μm). Under negative pressure, the solvent is removed, and the two-dimensional GO nanosheets will be stacked layer by layer on the surface of the filter membrane to form a layered GO film with a consistent orientation (i.e., a macroscopic aggregate of "bricks"). In this invention, the thickness of the film can be precisely controlled by adjusting the amount of GO suspension. In this invention, the thickness of a single layer of layered graphene oxide film is, for example, 5-50 μm. According to the application requirements, a layered preform can be formed by stacking multiple layers of layered graphene oxide films. The thickness of the layered preform is preferably 4-6 mm. In the vacuum filtration of this invention, the negative pressure (i.e., the vacuum degree) is controlled at -0.08 to -0.095 MPa.

[0028] According to some preferred embodiments, in step (3): the thickness of the layered preform is 4-6 mm; the interface layer is a pyrolytic carbon interface layer and / or a boron nitride interface layer; when depositing the pyrolytic carbon interface layer, propane is used as the reaction source gas (precursor gas), argon is used as the carrier gas, the propane flow rate is 50-200 sccm, the argon flow rate is 50-200 sccm, the deposition temperature is 950-1050℃, the deposition pressure is 1-5 kPa, and the deposition time is 0.5-2 h. Preferably, the thickness of the pyrolytic carbon interface layer is 50-150 nm; when depositing the boron nitride interface layer, boron trichloride (BCl3) and ammonia (NH3) are used as the reaction source gas (precursor gas), and the boron trichloride and ammonia... The molar ratio of the gases is 1:(3-5), the deposition temperature is 900-1100℃, the deposition pressure is 0.5-2kPa, and the deposition time is 0.5-2h. Preferably, the thickness of the boron nitride interface layer is 30-100nm. During the deposition of the boron nitride interface layer, argon and hydrogen are also introduced. The present invention does not impose specific limitations on the flow rates of argon and hydrogen, which can be conventionally selected by those skilled in the art. In the present invention, the molar ratio of boron trichloride to ammonia is preferably 1:(3-5). This can promote reaction equilibrium, ensure complete reaction of BCl3, improve the stoichiometry, reduce nitrogen vacancies, suppress the formation of undesirable byproducts, and control the deposition rate and morphology of boron nitride deposition.

[0029] According to some specific implementation methods, step (3) is as follows: a self-supporting layered GO membrane or a pre-cut multilayer layered GO membrane stack is used as a layered preform. The layered preform is placed in a chemical vapor infiltration (CVI) reactor. Under high temperature and low pressure conditions, a precursor gas (such as C3H8 for depositing pyrolytic carbon PyC, or BCl3+NH3 for depositing boron nitride BN) is introduced. The gas molecules diffuse into the nanopores between the GO sheets and decompose and deposit on their surface to form an ultra-thin interface layer (PyC interface layer or BN interface layer) with controllable thickness, thus obtaining a layered preform with an interface layer deposited. For the PyC interface layer CVI deposition, the deposition temperature is 950-1050℃, the pressure is 1-5kPa, the propane flow rate is 50-200sccm, the deposition time is 0.5-2h, and the target thickness is 50-150nm. For the BN interface layer CVI deposition, the deposition temperature is 900-1100℃, the pressure is 0.5-2kPa, the molar ratio of BCl3 to NH3 is 1:3-1:5, and the target thickness is 30-100nm.

[0030] According to some preferred embodiments, in step (4): the ceramic precursor solution is a silicon carbide ceramic precursor solution; the present invention does not specifically limit the silicon carbide ceramic precursor solution, and those skilled in the art can conventionally select it; in the present invention, the silicon carbide ceramic precursor solution is, for example, prepared by xylene and polycarbosilane, and the mass percentage of polycarbosilane contained in the silicon carbide ceramic precursor solution is 40-60%; the temperature of the high-temperature treatment is 1400-1600℃, and the time is 0.5-1.5h, preferably 1h; in the present invention, during the high-temperature treatment, the sample after PIP densification is heat-treated at a higher temperature (such as 1400-1600℃, argon atmosphere), which can promote the sintering of the ceramic matrix and is beneficial to improving the mechanical properties and high-temperature stability of the matrix; in the present invention, the temperature of the high-temperature treatment is higher than the temperature of the high-temperature pyrolysis; and / or the high-temperature treatment is carried out in an inert atmosphere, preferably, the inert atmosphere is an argon atmosphere.

[0031] According to some preferred embodiments, step (4) includes the following sub-steps: (a) The layered preform with the deposited interface layer is impregnated with a ceramic precursor solution, followed by curing and high-temperature pyrolysis; preferably, the impregnation is first vacuum impregnation for 1-2 hours, followed by pressure impregnation for 0.5-1 hours, the curing temperature is 150-350°C, the curing time is 1-3 hours, the high-temperature pyrolysis temperature is 1000-1500°C, the time is 1-3 hours, and the heating rate is 2-5°C / min; in this invention, the curing at 150-350°C and / or the high-temperature pyrolysis are carried out in an inert atmosphere, preferably in a nitrogen and / or argon atmosphere; this invention does not specifically limit the amount of the ceramic precursor solution, as long as it is sufficient to completely immerse the layered preform with the deposited interface layer in the ceramic precursor solution. (b) Repeat step (a) multiple times, preferably repeat step (a) more than 10 times; (c) The material obtained in step (b) is subjected to high-temperature treatment to obtain the multi-scale structure ceramic matrix composite material.

[0032] According to some specific implementation methods, step (4) is as follows: During the penetration process of the ceramic matrix "slurry", the layered preform with the interface layer deposited is immersed in the ceramic precursor solution. Through vacuum impregnation process (vacuum first, then introduce the ceramic precursor solution) and pressure impregnation process, it is ensured that the ceramic precursor solution can fully penetrate into every corner between the layers. After the impregnated layered preform is taken out, it is cured at 150-350℃ for 1-3h, and then the PIP pyrolysis process is carried out. The heating rate is 2-5℃ / min, the pyrolysis temperature is 1000-1500℃, and the temperature is held for 2h. The number of times the impregnation-room temperature curing-pyrolysis is repeated is ≥10 times. Then the high temperature treatment is carried out.

[0033] In a second aspect, the present invention provides a multi-scale structured ceramic matrix composite material, which is prepared using the preparation method described in the first aspect of the present invention.

[0034] The present invention will be further described below by way of examples, but the scope of protection of the present invention is not limited to these embodiments. The present invention may have many other embodiments. Without departing from the spirit and essence of the present invention, those skilled in the art can make various corresponding changes and modifications according to the present invention, but these corresponding changes and modifications should all fall within the scope of protection of the appended claims. Unless otherwise specified, the experimental methods used in the following embodiments are conventional methods. Unless otherwise specified, the materials, reagents, etc., used in the following embodiments can be obtained commercially or prepared by existing methods. The graphene oxide powder involved in the following embodiments and comparative examples is graphene oxide powder obtained by the improved Hummers method in the prior art.

[0035] Example 1 (1) Preparation of graphene oxide suspension: Graphene oxide powder was dispersed in deionized water by pulsed ultrasound treatment to form a uniformly dispersed graphene oxide suspension (GO suspension); the concentration of the GO suspension was 3 mg / mL, the power of the pulsed ultrasound treatment was 400 W, the pulsed ultrasound treatment time was 1.5 h, the frequency of the pulsed ultrasound treatment was 20 kHz, and the power density of the pulsed ultrasound treatment was 100 W / cm³. 2 The pulse duration is 30 seconds, and the duty cycle is 75% (i.e., 10-second interval pulse ultrasound for 30 seconds).

[0036] (2) Preparation of layered preform: Using vacuum filtration, GO suspension is slowly added dropwise at a rate of 1 mL / min to a micron nylon membrane with a pore size of 0.22 μm in the filtration device. Under negative pressure (controlled at -0.085 MPa), the solvent is removed, and two-dimensional GO nanosheets are stacked layer by layer on the surface of the filter membrane to form a layered graphene oxide membrane with a thickness of 30 μm. Multiple layered graphene oxide membranes are obtained by vacuum filtration and cut. The cut multilayer (multiple sheets) graphene oxide membranes are stacked to form a layered preform with a thickness of 5 mm.

[0037] (3) Preparation of pyrolytic carbon interface layer: The layered preform is placed in a chemical vapor infiltration (CVI) reactor and a pyrolytic carbon PyC interface layer is deposited using propane (C3H8). The deposition temperature during chemical vapor infiltration is 1025℃, the pressure is 2kPa, the propane flow rate is 80sccm, the argon (carrier gas) flow rate is 100sccm, and the deposition time is 1h to obtain a layered preform with an interface layer deposited.

[0038] (4) Preparation of ceramic matrix: The layered preform with the interface layer deposited is impregnated with silicon carbide ceramic precursor solution, and then the impregnated layered preform with the interface layer deposited is taken out from the silicon carbide ceramic precursor solution, cured at 200°C for 2 hours, and then heated to 1300°C for high-temperature pyrolysis at a heating rate of 5°C / min for 2 hours; the impregnation, curing and pyrolysis steps are repeated 10 times; wherein, the silicon carbide ceramic precursor solution is prepared by xylene and polycarbosilane, and the mass percentage of polycarbosilane contained in the silicon carbide ceramic precursor solution is 50%; the impregnation is first vacuum impregnated to 150Pa for 1.5 hours, and then pressure impregnated for 1 hour, the pressure of the pressure impregnation is 3MPa; the curing and high-temperature pyrolysis are carried out under an argon atmosphere.

[0039] (5) High temperature treatment: The material treated in step (4) is heated to 1400℃ at a heating rate of 5℃ / min and heat-treated for 1h in an argon atmosphere to promote the sintering of the ceramic matrix, so as to improve the mechanical properties and high temperature stability of the matrix and prepare a multi-scale structure ceramic matrix composite material.

[0040] Performance testing: The multi-scale ceramic matrix composite material prepared in this embodiment was tested, and its room temperature fracture toughness was measured to be 25 MPa·m. 1 / 2 The room temperature flexural strength is 510 MPa, and the flexural strength in an air environment at 1450℃ reaches 338 MPa.

[0041] Example 2 Example 2 is basically the same as Example 1, except that: (1) Preparation of graphene oxide suspension: Graphene oxide powder was dispersed in deionized water by pulsed ultrasound treatment to form a uniformly dispersed graphene oxide suspension (GO suspension); the concentration of the GO suspension was 1 mg / mL, the power of the pulsed ultrasound treatment was 400 W, the pulsed ultrasound treatment time was 1.5 h, the frequency of the pulsed ultrasound treatment was 20 kHz, and the power density of the pulsed ultrasound treatment was 100 W / cm³. 2 The pulse duration is 30 seconds, and the duty cycle is 75% (i.e., 10-second interval pulse ultrasound for 30 seconds).

[0042] (2) Preparation of layered preform: Using vacuum filtration, GO suspension is slowly added dropwise at a rate of 0.5 mL / min to a micron-sized nylon membrane with a pore size of 0.2 μm in the filtration device. Under negative pressure (controlled at -0.085 MPa), the solvent is removed, and two-dimensional GO nanosheets are stacked layer by layer on the surface of the filter membrane to form a layered graphene oxide membrane with a thickness of 30 μm. Multiple layered graphene oxide membranes are obtained by vacuum filtration and cut. The cut multilayer (multiple sheets) graphene oxide membranes are stacked to form a layered preform with a thickness of 5 mm.

[0043] Performance testing: The multi-scale ceramic matrix composite material prepared in this embodiment was tested, and the room temperature fracture toughness was measured to be 22.4 MPa·m. 1 / 2 The room temperature flexural strength is 475 MPa, and the air flexural strength at 1450℃ is 307 MPa.

[0044] Example 3 Example 3 is basically the same as Example 1, except that: (1) Preparation of graphene oxide suspension: Graphene oxide powder was dispersed in deionized water by pulsed ultrasound treatment to form a uniformly dispersed graphene oxide suspension (GO suspension); the concentration of the GO suspension was 5 mg / mL, the power of the pulsed ultrasound treatment was 400 W, the pulsed ultrasound treatment time was 1.5 h, the frequency of the pulsed ultrasound treatment was 20 kHz, and the power density of the pulsed ultrasound treatment was 100 W / cm³. 2 The pulse duration is 30 seconds, and the duty cycle is 75% (i.e., 10-second interval pulse ultrasound for 30 seconds).

[0045] (2) Preparation of layered preform: Using vacuum filtration, GO suspension is slowly added dropwise at a rate of 2 mL / min to a micron-sized nylon membrane with a pore size of 0.3 μm in the filtration device. Under negative pressure (controlled at -0.085 MPa), the solvent is removed, and two-dimensional GO nanosheets are stacked layer by layer on the surface of the filter membrane to form a layered graphene oxide membrane with a thickness of 30 μm. Multiple layered graphene oxide membranes are obtained by vacuum filtration and cut. The cut multilayer (multiple sheets) graphene oxide membranes are stacked to form a layered preform with a thickness of 5 mm.

[0046] Performance testing: The multi-scale ceramic matrix composite material prepared in this embodiment was tested, and the room temperature fracture toughness was measured to be 21.2 MPa·m. 1 / 2 The room temperature flexural strength is 466 MPa, and the air flexural strength at 1450℃ is 297 MPa.

[0047] Example 4 Example 4 is basically the same as Example 1, except that: (1) Preparation of graphene oxide suspension: Graphene oxide powder was dispersed in deionized water by pulsed ultrasound treatment to form a uniformly dispersed graphene oxide suspension (GO suspension); the concentration of the GO suspension was 0.5 mg / mL, the power of the pulsed ultrasound treatment was 400 W, the pulsed ultrasound treatment time was 1.5 h, the frequency of the pulsed ultrasound treatment was 20 kHz, and the power density of the pulsed ultrasound treatment was 100 W / cm³. 2 The pulse duration is 30 seconds, and the duty cycle is 75% (i.e., 10-second interval pulse ultrasound for 30 seconds).

[0048] (2) Preparation of layered preform: Using vacuum filtration, GO suspension is slowly added dropwise at a rate of 0.2 mL / min to a micron-sized nylon membrane with a pore size of 0.1 μm in the filtration device. Under negative pressure (controlled at -0.085 MPa), the solvent is removed, and two-dimensional GO nanosheets are stacked layer by layer on the surface of the filter membrane to form a layered graphene oxide membrane with a thickness of 30 μm. Multiple layered graphene oxide membranes are obtained by vacuum filtration and cut. The cut multilayer (multiple sheets) graphene oxide membranes are stacked to form a layered preform with a thickness of 5 mm.

[0049] Performance testing: The multi-scale ceramic matrix composite material prepared in this embodiment was tested, and the room temperature fracture toughness was measured to be 15.1 MPa·m. 1 / 2 The room temperature flexural strength is 394 MPa, and the air flexural strength at 1450℃ is 250 MPa.

[0050] Comparative Example 1 (1) Preparation of graphene oxide suspension: Graphene oxide powder was dispersed in deionized water by pulsed ultrasound treatment to form a graphene oxide suspension (GO suspension); the concentration of the GO suspension was 10 mg / mL, the power of the pulsed ultrasound treatment was 400 W, the pulsed ultrasound treatment time was 1.5 h, the frequency of the pulsed ultrasound treatment was 20 kHz, and the power density of the pulsed ultrasound treatment was 100 W / cm³. 2 The pulse duration is 30 seconds, and the duty cycle is 75% (i.e., 10-second interval pulse ultrasound for 30 seconds).

[0051] (2) Preparation of layered preform: Using vacuum filtration, GO suspension is slowly added dropwise at a rate of 1 mL / min to a micron-sized nylon membrane with a pore size of 1 μm in the filtration device. Under negative pressure (controlled at -0.085 MPa), the solvent is removed, and two-dimensional GO nanosheets are stacked layer by layer on the surface of the filter membrane to form a layered graphene oxide membrane with a thickness of 30 μm. Multiple layered graphene oxide membranes are obtained by vacuum filtration and cut. The cut multilayer (multiple sheets) graphene oxide membranes are stacked to form a layered preform with a thickness of 5 mm.

[0052] (3) Preparation of pyrolytic carbon interface layer: The layered preform is placed in a chemical vapor infiltration (CVI) reactor and a pyrolytic carbon PyC interface layer is deposited using C3H8. The deposition temperature during chemical vapor infiltration is 1025℃, the pressure is 2kPa, the propane flow rate is 500sccm, the argon (carrier gas) flow rate is 500sccm, and the deposition time is 1h to obtain a layered preform with an interface layer deposited.

[0053] (4) Preparation of ceramic matrix: The layered preform with the interface layer deposited is impregnated with silicon carbide ceramic precursor solution, and then the impregnated layered preform with the interface layer deposited is taken out from the silicon carbide ceramic precursor solution and cured at 200℃ for 2h, and then heated to 1300℃ at a heating rate of 5℃ / min for high-temperature pyrolysis for 2h; the impregnation, curing and pyrolysis steps are repeated 10 times; wherein, the silicon carbide ceramic precursor solution is prepared by xylene and polycarbosilane, and the mass percentage of polycarbosilane contained in the silicon carbide ceramic precursor solution is 50%; the impregnation is first vacuum impregnated to 150Pa for 1.5h, and then pressure impregnated for 1h, the pressure of the pressure impregnation is 3MPa; the curing and high-temperature pyrolysis are carried out under an argon atmosphere.

[0054] (5) High temperature treatment: The material treated in step (4) is heated to 1400°C at a heating rate of 5°C / min and heat-treated for 1 hour in an argon atmosphere to obtain ceramic matrix composite material.

[0055] Performance testing: The ceramic matrix composite material prepared in this comparative example was tested, and its room temperature fracture toughness was measured to be 12 MPa·m.1 / 2 The room temperature flexural strength is 375 MPa, and the flexural strength in an air environment at 1450℃ is 235 MPa.

[0056] Comparative Example 2 (1) Preparation of graphene oxide suspension: Graphene oxide powder was dispersed in deionized water by pulsed ultrasound treatment to form a graphene oxide suspension (GO suspension); the concentration of the GO suspension was 10 mg / mL, the power of the pulsed ultrasound treatment was 400 W, the pulsed ultrasound treatment time was 1.5 h, the frequency of the pulsed ultrasound treatment was 20 kHz, and the power density of the pulsed ultrasound treatment was 100 W / cm³. 2 The pulse duration is 30 seconds, and the duty cycle is 75% (i.e., 10-second interval pulse ultrasound for 30 seconds).

[0057] (2) Preparation of layered preform: Using vacuum filtration, GO suspension is slowly added dropwise at a rate of 1 mL / min to a micron-sized nylon membrane with a pore size of 1 μm in the filtration device. Under negative pressure (controlled at -0.085 MPa), the solvent is removed, and two-dimensional GO nanosheets are stacked layer by layer on the surface of the filter membrane to form a layered graphene oxide membrane with a thickness of 30 μm. Multiple layered graphene oxide membranes are obtained by vacuum filtration and cut. The cut multilayer (multiple sheets) graphene oxide membranes are stacked to form a layered preform with a thickness of 5 mm.

[0058] (3) Preparation of ceramic matrix: The layered preform is impregnated with silicon carbide ceramic precursor solution, and then the impregnated layered preform is taken out from the silicon carbide ceramic precursor solution and cured at 200℃ for 2h. Then, the temperature is raised to 1300℃ at a heating rate of 5℃ / min for high-temperature pyrolysis for 2h. The impregnation, curing and pyrolysis steps are repeated 10 times. The silicon carbide ceramic precursor solution is prepared by xylene and polycarbosilane, and the mass percentage of polycarbosilane in the silicon carbide ceramic precursor solution is 50%. The impregnation is first vacuum impregnated to 150Pa for 1.5h, and then pressure impregnated for 1h. The pressure impregnation pressure is 3MPa. The curing and high-temperature pyrolysis are carried out in an argon atmosphere.

[0059] (4) High temperature treatment: The material treated in step (3) is heated to 1400°C at a heating rate of 5°C / min and heat-treated for 1 hour in an argon atmosphere to obtain ceramic matrix composite material.

[0060] Performance testing: The ceramic matrix composite material prepared in this comparative example was tested, and its room temperature fracture toughness was measured to be 8 MPa·m. 1 / 2 The room temperature flexural strength is 200 MPa, and the flexural strength in an air environment at 1450℃ is 118 MPa.

[0061] Comparative Example 3 (1) Preparation of pyrolytic carbon interface layer: A carbon fiber preform with a thickness of 5 mm was placed in a chemical vapor infiltration (CVI) reactor and a pyrolytic carbon PyC interface layer was deposited using propane (C3H8). The deposition temperature during chemical vapor infiltration was 1025℃, the pressure was 2 kPa, the propane flow rate was 80 sccm, the argon (carrier gas) flow rate was 100 sccm, and the deposition time was 1 h to obtain a carbon fiber preform with an interface layer deposited.

[0062] (2) Preparation of ceramic matrix: The carbon fiber preform with the interface layer deposited is impregnated with silicon carbide ceramic precursor solution. Then, the impregnated carbon fiber preform with the interface layer deposited is taken out of the silicon carbide ceramic precursor solution and cured at 200℃ for 2h. Then, it is heated to 1300℃ at a heating rate of 5℃ / min for high-temperature pyrolysis for 2h. The impregnation, curing and pyrolysis steps are repeated 10 times. The silicon carbide ceramic precursor solution is prepared by xylene and polycarbosilane. The mass percentage of polycarbosilane in the silicon carbide ceramic precursor solution is 50%. The impregnation is carried out by first vacuum impregnation at 150Pa for 1.5h, and then pressure impregnation for 1h. The pressure impregnation pressure is 3MPa. The curing and high-temperature pyrolysis are carried out in an argon atmosphere.

[0063] (3) High temperature treatment: The material treated in step (2) is heated to 1400°C at a heating rate of 5°C / min and heat-treated for 1 hour in an argon atmosphere to obtain ceramic matrix composite material.

[0064] Performance testing: The ceramic matrix composite material prepared in this comparative example was tested, and its room temperature fracture toughness was measured to be 13.5 MPa·m. 1 / 2 The room temperature flexural strength is 400 MPa, and the flexural strength in an air environment at 1450℃ is 248 MPa.

[0065] Comparative Example 4 Comparative Example 4 is basically the same as Example 1, except that it does not include the high-temperature treatment in step (5).

[0066] Performance testing: The ceramic matrix composite material prepared in this comparative example was tested, and the room temperature fracture toughness was measured to be 20.7 MPa·m. 1 / 2 The room temperature flexural strength is 457 MPa, and the air flexural strength at 1450℃ is 288 MPa.

[0067] Comparative Example 5 Comparative Example 5 is basically the same as Example 1, except that: (1) Preparation of graphene oxide suspension: Graphene oxide powder was dispersed in deionized water by continuous ultrasonic treatment to obtain graphene oxide suspension (GO suspension); the concentration of GO suspension was 3 mg / mL, the frequency of ultrasonic treatment was 20 kHz, the power of ultrasonic treatment was 400 W, the ultrasonic treatment time was 1.5 h, and the power density of continuous ultrasonic treatment was 5 W / cm³. 2 .

[0068] Performance testing: The ceramic matrix composite material prepared in this comparative example was tested, and the room temperature fracture toughness was measured to be 11.2 MPa·m. 1 / 2 The room temperature flexural strength is 310 MPa, and the air flexural strength at 1450℃ is 198 MPa.

[0069] Comparative Example 6 (1) Preparation of graphene oxide suspension: Graphene oxide powder was dispersed in deionized water by pulsed ultrasound treatment to form a uniformly dispersed graphene oxide suspension (GO suspension); the concentration of the GO suspension was 3 mg / mL, the power of the pulsed ultrasound treatment was 400 W, the pulsed ultrasound treatment time was 1.5 h, the frequency of the pulsed ultrasound treatment was 20 kHz, and the power density of the pulsed ultrasound treatment was 100 W / cm³. 2 The pulse duration is 30 seconds, and the duty cycle is 75% (i.e., 10-second interval pulse ultrasound for 30 seconds).

[0070] (2) Impregnating carbon fiber preform with graphene oxide suspension: A carbon fiber preform with a thickness of 5 mm is placed in a graphene oxide suspension for vacuum impregnation, and then the carbon fiber preform is taken out from the graphene oxide suspension and vacuum dried at 40°C for 24 h to obtain a modified carbon fiber preform; the vacuum impregnation is vacuum impregnation at 150 Pa for 1.5 h.

[0071] (3) Preparation of pyrolytic carbon interface layer: The modified carbon fiber preform is placed in a chemical vapor infiltration (CVI) reactor and a pyrolytic carbon PyC interface layer is deposited using C3H8. The deposition temperature during chemical vapor infiltration is 1025℃, the pressure is 2kPa, the propane flow rate is 80sccm, the argon (carrier gas) flow rate is 100sccm, and the deposition time is 1h to obtain a modified carbon fiber preform with an interface layer deposited.

[0072] (4) Preparation of ceramic matrix: The modified carbon fiber preform with an interface layer deposited is impregnated with a silicon carbide ceramic precursor solution. Then, the impregnated modified carbon fiber preform with an interface layer deposited is removed from the silicon carbide ceramic precursor solution and cured at 200°C for 2 hours. Then, it is heated to 1300°C at a heating rate of 5°C / min for high-temperature pyrolysis for 2 hours. The impregnation, curing and pyrolysis steps are repeated 10 times. The silicon carbide ceramic precursor solution is prepared by xylene and polycarbosilane. The polycarbosilane content in the silicon carbide ceramic precursor solution is 50% by mass. The impregnation is carried out by first vacuum impregnation at 150Pa for 1.5 hours, and then pressure impregnation for 1 hour. The pressure impregnation pressure is 3MPa. The curing and high-temperature pyrolysis are carried out under an argon atmosphere.

[0073] (5) High temperature treatment: The material treated in step (4) is heated to 1400°C at a heating rate of 5°C / min and heat-treated for 1 hour in an argon atmosphere to obtain ceramic matrix composite material.

[0074] Performance testing: The ceramic matrix composite material prepared in this comparative example was tested, and the room temperature fracture toughness was measured to be 14.7 MPa·m. 1 / 2 The room temperature flexural strength is 412 MPa, and the air flexural strength at 1450℃ is 258 MPa.

[0075] Comparative Example 7 (1) Preparation of graphene oxide / carbon nanotube foam as a preform: First, weigh 5g of graphite powder and 2.5g of sodium nitrate. Pour 140mL of concentrated sulfuric acid into a beaker. Add graphite powder and sodium nitrate to the concentrated sulfuric acid in sequence, stir evenly, and slowly add 15g of potassium permanganate. Place the reaction solution in a 35℃ water bath and stir evenly for 30min to obtain a dark brown liquid. Then stir at 90℃ for 20min. Slowly add 25mL of hydrogen peroxide solution (concentration 30%). After standing, discard the supernatant. Wash the centrifuged precipitate with deionized water and ethanol alternately until the pH value is neutral to obtain graphene oxide nanosheets. Weigh 3g of graphene oxide nanosheets, add water to 100mL, add 0.4g of carbon nanotube whiskers, and perform conventional ultrasonic dispersion (the ultrasonic dispersion frequency is 20kHz, the ultrasonic dispersion power is 400W, the time is 1.5h, and the ultrasonic dispersion power density is 5W / cm). 2 After being evenly dispersed, the mixture is poured into a mold and freeze-dried for 48 hours to obtain graphene oxide / carbon nanotube foam.

[0076] (2) Preparation of pyrolytic carbon interface layer: Graphene oxide / carbon nanotube foam is placed in a chemical vapor infiltration (CVI) reactor and a pyrolytic carbon PyC interface layer is deposited using C3H8. The deposition temperature during chemical vapor infiltration is 1025℃, the pressure is 2kPa, the propane flow rate is 80sccm, the argon (carrier gas) flow rate is 100sccm, and the deposition time is 1h to obtain a preform with an interface layer deposited.

[0077] (3) Preparation of ceramic matrix: The preform with the interface layer deposited is impregnated with silicon carbide ceramic precursor solution, and then the impregnated preform with the interface layer deposited is taken out from the silicon carbide ceramic precursor solution and cured at 200℃ for 2h. Then, it is heated to 1300℃ at a heating rate of 5℃ / min for high-temperature pyrolysis for 2h. The impregnation, curing and pyrolysis steps are repeated 10 times. The silicon carbide ceramic precursor solution is prepared by xylene and polycarbosilane, and the mass percentage of polycarbosilane in the silicon carbide ceramic precursor solution is 50%. The impregnation is first vacuum impregnated to 150Pa for 1.5h, and then pressure impregnated for 1h. The pressure impregnation pressure is 3MPa. The curing and high-temperature pyrolysis are carried out in an argon atmosphere.

[0078] (4) High temperature treatment: The material treated in step (3) is heated to 1400°C at a heating rate of 5°C / min and heat-treated for 1 hour in an argon atmosphere to obtain ceramic matrix composite material.

[0079] Performance testing: The ceramic matrix composite material prepared in this comparative example was tested, and the room temperature fracture toughness was measured to be 18 MPa·m. 1 / 2 The room temperature flexural strength is 439 MPa, and the air flexural strength at 1450℃ is 281 MPa.

[0080] The parts of this invention not described in detail are techniques known to those skilled in the art.

[0081] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention, and not to limit them; although the present invention has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that modifications can still be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some of the technical features; and these modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the spirit and scope of the technical solutions of the embodiments of the present invention.

Claims

1. A method for producing a multi-scale structured ceramic matrix composite material, characterized by, The method comprises the following steps: (1) dispersing graphene oxide in deionized water to obtain a graphene oxide suspension; (2) vacuum filtration of the graphene oxide suspension to the surface of a microporous filter membrane to obtain a layered graphene oxide membrane; (3) taking at least one layered graphene oxide membrane as a layered preform, depositing an interfacial layer in the layered preform by chemical vapor infiltration to obtain a layered preform with an interfacial layer deposited thereon; (4) taking a ceramic precursor solution as a reactant, densifying the substrate of the layered preform with the interfacial layer deposited thereon by an impregnation pyrolysis method, and then performing high-temperature treatment to obtain a multi-scale structure ceramic matrix composite material.

2. The production method according to claim 1, characterized by, In step (1): The concentration of the graphene oxide suspension is 1-5 mg / mL; and / or The graphene oxide is dispersed in deionized water by ultrasonic treatment.

3. The preparation method according to claim 2, characterized in that: The power of the ultrasonic treatment is 300-500 W, and the ultrasonic treatment time is 1-2 h.

4. The preparation method according to claim 2, characterized in that: The ultrasonic treatment is pulse ultrasonic treatment, the power density of the pulse ultrasonic treatment is 80-150 W / cm 2 , the pulse time is 20-30 s, the duty cycle is 60-80%, and the time of the pulse ultrasonic treatment is 1-2 h.

5. The preparation method according to claim 1, characterized in that, In step (2): The pore size of the microporous filter membrane is 0.2-0.3 μm; and / or The microporous filter membrane is a microporous nylon filter membrane.

6. The method of claim 1, wherein, In step (2): The thickness of the single-layered graphene oxide membrane is 5-50 μm; The filtration is performed under a vacuum degree of -0.08 to -0.095 MPa; and / or When performing the filtration, the graphene oxide suspension is added dropwise onto the microporous filter membrane at a dropwise adding speed of 0.5-2 mL / min for vacuum filtration, so that the graphene oxide is stacked layer by layer on the surface of the microporous filter membrane to obtain the layered graphene oxide membrane.

7. The preparation method according to claim 1, characterized in that, In step (3): The thickness of the layered preform is 4-6 mm; The interfacial layer is a pyrolytic carbon interfacial layer and / or a boron nitride interfacial layer; When depositing the pyrolytic carbon interfacial layer, propane is used as the reaction source gas, the propane flow rate is 50-200 sccm, the deposition temperature is 950-1050 ℃, the deposition pressure is 1-5 kPa, and the deposition time is 0.5-2 h, preferably, the thickness of the pyrolytic carbon interfacial layer is 50-150 nm; When depositing the boron nitride interfacial layer, boron trichloride and ammonia are used as the reaction source gas, the molar ratio of boron trichloride to ammonia is 1: (3-5), the deposition temperature is 900-1100 ℃, the deposition pressure is 0.5-2 kPa, and the deposition time is 0.5-2 h, preferably, the thickness of the boron nitride interfacial layer is 30-100 nm.

8. The method of claim 1, wherein, In step (4): The ceramic precursor solution is a silicon carbide ceramic precursor solution; The temperature of the high-temperature treatment is 1400-1600 ℃, and the time is 0.5-1.5 h; and / or The high-temperature treatment is performed in an inert atmosphere, preferably, the inert atmosphere is an argon atmosphere.

9. The method of claim 1, wherein, Step (4) comprises the following sub-steps: (a) impregnating the layered preform with the interface layer deposited with a ceramic precursor solution, and then solidifying and high-temperature pyrolyzing; preferably, the solidification temperature is 150-350℃, the solidification time is 1-3h, the high-temperature pyrolysis temperature is 1000-1500℃, the time is 1-3h, and the temperature rising rate is 2-5℃ / min; (b) repeating step (a) for multiple times, preferably 10 times or more; (c) high-temperature treating the material obtained from step (b) to obtain the multi-scale structure ceramic matrix composite material.

10. A multi-scale structured ceramic matrix composite, characterized by: Prepared by the preparation method in any one of claims 1 to 9.