CN111334743B - Preparation method of zirconium boride-zirconium carbide-silicon carbide composite coating - Google Patents

Preparation method of zirconium boride-zirconium carbide-silicon carbide composite coating Download PDF

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CN111334743B
CN111334743B CN202010178928.4A CN202010178928A CN111334743B CN 111334743 B CN111334743 B CN 111334743B CN 202010178928 A CN202010178928 A CN 202010178928A CN 111334743 B CN111334743 B CN 111334743B
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zirconium
silicon carbide
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CN111334743A (en
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杨勇
崔宇航
马玉夺
孙文韦
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Hebei University of Technology
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    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C4/00—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge
    • C23C4/12—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge characterised by the method of spraying
    • C23C4/131—Wire arc spraying
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C4/00—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge
    • C23C4/02—Pretreatment of the material to be coated, e.g. for coating on selected surface areas
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C4/00—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge
    • C23C4/04—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge characterised by the coating material
    • C23C4/06—Metallic material
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C4/00—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge
    • C23C4/04—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge characterised by the coating material
    • C23C4/06—Metallic material
    • C23C4/073—Metallic material containing MCrAl or MCrAlY alloys, where M is nickel, cobalt or iron, with or without non-metal elements
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C4/00—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge
    • C23C4/04—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge characterised by the coating material
    • C23C4/10—Oxides, borides, carbides, nitrides or silicides; Mixtures thereof

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Abstract

The invention relates to a preparation method of a zirconium boride-zirconium carbide-silicon carbide composite coating. The method comprises the following steps: firstly, preparing zirconium/boron carbide/silicon carbide composite powder or zirconium oxide/boron carbide/aluminum/silicon carbide composite powder: and thirdly, spraying the composite powder prepared in the first step on the surface of the base material by adopting a thermal spraying method, thereby obtaining the zirconium boride-zirconium carbide-silicon carbide composite coating through in-situ reaction synthesis. The invention overcomes the defects of high raw material cost, high process cost, low deposition efficiency, poor coating performance and unsuitability for large-scale industrial production of a direct spraying method. Meanwhile, the defects of poor high-temperature oxidation resistance and poor ablation resistance of the zirconium boride-zirconium carbide composite coating prepared by the prior art are overcome.

Description

Preparation method of zirconium boride-zirconium carbide-silicon carbide composite coating
Technical Field
The technical scheme of the invention relates to the plating of materials by using boride, carbide and silicon carbide, in particular to a preparation method of a zirconium boride-zirconium carbide-silicon carbide composite coating.
Background
With the development of modern technologies such as aerospace, aviation, atomic energy, new smelting technology and the like, increasingly strict requirements are put on high-temperature and high-performance structural materials, and the materials are required to have good high-temperature resistance to adapt to harsh operating environments such as thermal shock resistance, high-temperature strength, corrosion resistance and oxidation resistance. Zirconium boride (ZrB)2) The high-temperature-resistant high-temperature-resistant high-temperature-resistant high-temperature-resistant high-temperature-resistant high-temperature-resistant high-temperature-resistant high-temperature-resistant high-temperature resistant high-temperature resistant high-. However, the preparation process of the zirconium boride block material is complicated due to the higher melting pointThe sintering temperature is high, the period is long, and the difficulty that compact large-size parts are difficult to obtain exists; meanwhile, the strength and toughness of the alloy are relatively low, and the thermal shock resistance and high-temperature oxidation resistance of the alloy are insufficient, so that the application of the alloy in harsh operating environments is limited.
One solution to the above problem is to deposit zirconium boride on a substrate material by advanced surface coating techniques, such as: the zirconium boride coating material deposited on the surface of a base material is prepared on the surfaces of metal materials such as steel, cast iron, aluminum alloy, titanium alloy, nickel-based superalloy, intermetallic compound and the like and inorganic nonmetal materials such as graphite, carbon/carbon composite material, carbon/silicon carbide composite material, silicon carbide/silicon carbide and the like, so that the wear resistance, corrosion resistance and ablation resistance of the base material can be improved, and the mechanical property and the integral light weight of a part can be maintained.
On the other hand, in order to improve the high-temperature oxidation resistance of zirconium boride, researchers have added silicon carbide to zirconium boride. The addition of silicon carbide in zirconium boride can change the oxidation kinetics characteristic of zirconium boride at high temperature, prevent the high-temperature volatilization of the oxidation product boron oxide, and obviously improve the initial volatilization temperature of boron oxide. In addition, the silicon oxide generated by the silicon carbide under the high-temperature oxidation condition has certain fluidity, can effectively seal and fill the pores generated after the coating is oxidized, and has very low oxygen permeability, so that the permeation of oxygen at high temperature can be reduced, and the matrix is protected. The addition of a certain amount of silicon carbide in zirconium boride can improve the high-temperature oxidation resistance of zirconium boride while maintaining the high-temperature stability of zirconium boride. The zirconium boride-silicon carbide composite coating has good antioxidant effect by combining the characteristics of the two materials.
At present, the technology for preparing the zirconium boride composite coating mainly comprises the following steps: embedding, brush coating, chemical vapor deposition, cladding, thermal spraying, and the like.
(1) Embedding method: also called solid infiltration method, the deposition mechanism is that coating raw material powder or mixed powder containing target coating components is put around the base material and is kept warm at a certain temperature, and complex physical and chemical reactions occur between the coating raw material powder or between the raw material powder and the base material, so as to form a coatingA method of forming the coating. ZrB prepared by embedding method2The thickness of the composite ceramic coating is generally several micrometers to tens of micrometers. CN201410001380.0 discloses ZrB2The preparation method of the-SiC/SiC ceramic coating adopts an embedding method to sequentially prepare the intermediate layer SiC and the surface layer ZrB2-SiC/SiC ceramic coating. In the preparation step of the intermediate SiC layer, the matrix component embedded with the mixed powder is heated to 1600-2000 ℃ in a protective atmosphere, and the ceramic surface layer ZrB2In the preparation step of-SiC/SiC, the matrix component embedded with the mixed powder is heated to 2000-3000 ℃ under the protective atmosphere. However, the embedding process usually needs to keep the substrate material at a high temperature (2000-3000 ℃), so that the defects of large heat damage to the substrate and high cost exist; meanwhile, the deposition and diffusion speeds of different elements are different, so that the thickness of the zirconium boride coating cannot be controlled and the uniformity of components in the coating cannot be ensured; in addition, the embedding technique is difficult to meet for preparing coatings on large-sized parts, subject to the crucible size and the influence of heat sources.
(2) Brushing: the coating sintering method is also called as coating sintering method, and is characterized in that raw materials are mixed into slurry according to a certain proportion, then the slurry is coated on the surface of a substrate material, and then the slurry is solidified on the substrate through sintering to form a coating. The coating thickness produced by this method is about several tens of microns. However, the zirconium boride composite coating prepared by the method has the defects of low bonding strength between the coating and the matrix, poor thermal shock resistance, high sintering temperature and the like.
(3) Chemical vapor deposition method: the CVD method is a process technology for depositing a solid film on the surface of a substrate by means of space gas phase chemical reaction. Firstly, raw materials such as compounds and simple substances containing coating elements are injected into a reaction chamber provided with a substrate in a certain mode, then the raw materials are subjected to processes such as decomposition, synthesis, diffusion, adsorption and the like under certain conditions, and finally a film is formed on the surface of the substrate. The types of reactions mainly include: thermal decomposition, hydrogen reduction, metal reduction, chemical transport, oxidation, and the like. The feedstock for the CVD process may be gaseous, liquid or solid. CN201410005289.6 discloses a preparation method of a zirconium diboride coating, which uses a double-temperature-zone heating mode and ZrCl4、BCl3And H2As source gas, Ar gas or N2The zirconium diboride coating is prepared by adopting a chemical vapor deposition method as a carrier gas and a protective gas, and the technology has the defects of large equipment investment, high production cost, very slow growth process, long production period, small coating thickness, single component and incapability of preparing the zirconium boride composite material film.
(4) A cladding method: the method comprises laser cladding and plasma cladding, and is characterized in that coating powder is placed on the surface of a base material by using different filling modes, and then a high-energy laser beam or a high-energy plasma beam is used for radiating the surface of the base material, so that the coating material and the surface layer of the base material are simultaneously melted and solidified to form a surface coating. Document [ Repana. ZrB2Research on in-situ synthesis of/Fe composite coating [ D]Tianjin university, 2012, pointed out that ZrB can be synthesized in situ on the surface of a steel substrate by plasma transferred arc cladding or high energy laser beam cladding2Ceramic coating, but ZrB2The surface of the ceramic coating is poorly formed and the coating does not bond well to the substrate. The reason is mainly as follows: (B)4C and ZrB2All have extremely high melting points and have poor wettability with Fe-based metal; during cladding, molten B4C and ZrB2The surface of the cladding layer is not easy to form due to the agglomeration property; (II) ZrB2The crystallization and solidification process of the ceramic coating adopts a mode that a cladding layer is solidified from top to bottom and then from the middle, so that a large number of defects such as air holes, inclusions, cracks and the like are formed in the cladding layer; ③ to Zr + B4For the powder formula of C, the selection of a cladding method and process parameters thereof is crucial; when the cladding heat input is too high, the iron matrix dilutes the coating greatly, and the structure and the performance of the cladding layer are affected; if the heat input is too low, the preset powder is difficult to be fully melted, and the coating is not firmly combined with the matrix and is easy to fall off.
(5) Thermal spraying method: the method is a method for rapidly heating a coating material in a wire or powder state to a molten or semi-molten state by utilizing a specific heat source, such as electric arc, oxyacetylene flame or plasma flame flow, and spraying the coating material on the surface of a substrate at a high speed to form a zirconium boride coating. Preparation of ZrB by thermal spraying technology2Coating layerHas the main advantages of relatively simple process, large selection range of the substrate, large variation range of the thickness of the coating, high deposition rate and easy formation of the composite coating. However, from thermal spraying ZrB2In the research history of the coating, ZrB is prepared by adopting a direct spraying method in the prior art2Coating, i.e. spraying ZrB directly2Powder or ZrB2The powder being mixed with other powders, e.g. SiC, ZrC or/and ZrO2ZrB prepared from composite powder consisting of powder2And (4) base coating. CN201310364496.6 discloses a method for preparing a zirconium diboride-silicon carbide high-temperature oxidation resistant coating, which comprises the steps of firstly preparing ZrB by a spray drying method2Preparing ZrB from-SiC-coated composite powder by ultra-low pressure plasma spraying2-SiC composite coating. CN201410695915.9 discloses an ablation-resistant composite coating and a preparation method thereof, wherein the ablation-resistant layer consists of a bonding layer and a composite ceramic ablation-resistant layer, and the composite ceramic ablation-resistant layer consists of ZrB2-ZrC-SiC-ZrO2The complex phase ceramic is prepared by plasma spraying deposition. The disadvantages of the direct spray coating method are: first, high purity ZrB2Raw materials such as ZrC are expensive, which results in high cost; second, ZrB2The sintering temperature in the preparation process of the-SiC composite powder is 1800-2200 ℃, the heat preservation is carried out for 2 hours, the sintering temperature is high, and the process cost is high; thirdly, due to the raw material ZrB2The ZrC has high melting point, low melting degree in the spraying process, difficult spreading, low deposition efficiency, high porosity of the coating, low bonding strength with the matrix, poor thermal shock resistance and poor high-temperature oxidation resistance. These disadvantages significantly affect the quality and application of zirconium boride coatings prepared by direct spray coating. In order to solve the problem of preparing zirconium boride composite coatings by a direct spraying method, CN106381459A discloses a method for preparing zirconium boride-based coatings, which adopts a method of thermally spraying zirconia/boron carbide/aluminum composite powder to prepare zirconium boride-based coatings. Although the method overcomes the problems of high porosity, poor uniformity and the like of the zirconium boride-based coating prepared by a direct spraying method, the prepared coating only contains zirconium boride, zirconium carbide, alumina and zirconia phases, and the high-temperature oxidation resistance of the coating needs to be further improved.
Disclosure of Invention
The invention aims to provide a preparation method of a zirconium boride-zirconium carbide-silicon carbide composite coating aiming at the defects in the prior art. The method adopts an in-situ reaction synthesis method, adopts zirconium oxide-boron carbide-aluminum-silicon carbide composite powder or zirconium-boron carbide-silicon carbide composite powder, and utilizes the reaction of zirconium-boron carbide-silicon carbide or zirconium oxide-boron carbide-aluminum-silicon carbide under the high-temperature condition of thermal spraying flame flow to generate the composite coating with the main phase of zirconium boride, zirconium carbide and silicon carbide in situ. The invention overcomes the defects of high raw material cost, high process cost, low deposition efficiency, poor coating performance and unsuitability for large-scale industrial production of a direct spraying method in the prior art. Meanwhile, the invention also overcomes the defects of poor high-temperature oxidation resistance and poor ablation resistance of the zirconium boride-zirconium carbide composite coating prepared by the prior art.
The technical scheme adopted by the invention for solving the technical problem is as follows:
a preparation method of a zirconium boride-zirconium carbide-silicon carbide composite coating comprises the following steps:
the first step is any one of the following two methods:
the method comprises the following steps: preparing zirconium/boron carbide/silicon carbide composite powder:
zirconium powder, boron carbide powder and silicon carbide powder are mixed into composite powder, and then mixed into a binder, so that zirconium/boron carbide/silicon carbide composite powder for thermal spraying is prepared;
the silicon carbide powder accounts for 5-30% of the composite powder by mass, the weight ratio of the zirconium powder to the boron carbide powder is 60-90: 40-10, and the binder is used in a weight ratio of the composite powder to the binder of 100: 0.1-3;
or, preparing zirconium oxide/boron carbide/aluminum/silicon carbide composite powder by the second method:
mixing zirconia powder, boron carbide powder, aluminum powder and silicon carbide powder into composite powder, and uniformly mixing the composite powder with a binder to prepare zirconia/boron carbide/aluminum/silicon carbide composite powder for thermal spraying;
wherein the silicon carbide powder accounts for 5-30% of the composite powder, the boron carbide powder accounts for 5-30% of the total mass of the zirconia powder, the boron carbide powder and the aluminum powder, the weight ratio of the zirconia powder to the aluminum powder is 60-90: 40-10, the binder is used in a weight ratio of the composite powder to the binder of 100: 0.1-3,
the particle sizes of the zirconium powder, the boron carbide powder and the silicon carbide powder are all 0.001-10 microns; the granularity of the aluminum powder is 0.1-10 microns;
the binder is polyvinyl alcohol or methyl cellulose;
secondly, the surface of the base material with the required coating is pretreated in one of the following two ways:
1) when the base material is a metal base material, firstly, sand blasting is adopted, and then a bonding layer is sprayed on the surface of the metal base material after the sand blasting;
or, 2) when the base material is an inorganic non-metallic material base, adopting sand blasting or sand paper polishing treatment;
thirdly, preparing the zirconium boride-zirconium carbide-silicon carbide composite coating:
and spraying the composite powder for thermal spraying prepared in the first step on the surface of the base material pretreated in the second step by adopting a thermal spraying method, so as to obtain the zirconium boride-zirconium carbide-silicon carbide composite coating through in-situ synthesis.
The technological parameters of the thermal spraying method are as follows: the flow of the powder feeding gas is 0.3-0.6 m3The arc power is 32-45 KW, and the distance between the spray guns is 80-120 mm. The powder feeding gas is argon;
the thickness of the coating is 200-500 microns;
the metal material matrix is steel, cast iron, aluminum alloy, copper alloy, titanium alloy, magnesium alloy, nickel-based superalloy, nickel-chromium alloy, cobalt-based superalloy, tantalum-based alloy, tungsten-based alloy or intermetallic compound.
The inorganic non-metallic material matrix is graphite, a carbon/carbon composite material, a carbon/silicon carbide composite material or a silicon carbide/silicon carbide composite material.
The bonding layer material is: NiAl, NiCrAl, FeAl, NiCrAlY, CoCrAlY, CoNiCrAlY, NiCoCrAlYTa or NiCrBSi.
The preparation method of the zirconium boride-zirconium carbide-silicon carbide composite coating relates to commercially available raw materials, and the sand blasting process, the sand paper grinding process and the bonding layer spraying process are well known in the prior art.
The invention has the substantive characteristics that:
in the prior art (patent 2016108967591-preparation method of zirconium boride-based coating), zirconium boride-zirconium carbide-aluminum oxide composite coating is prepared by using zirconium oxide-boron carbide-aluminum composite powder; the prepared coating only contains zirconium boride, zirconium carbide, alumina and zirconia phases, so that the coating has the defects of poor high-temperature oxidation resistance and poor ablation resistance.
According to the invention, zirconium-boron carbide-silicon carbide or zirconium oxide-boron carbide-aluminum-silicon carbide can react under the high-temperature condition of thermal spraying flame flow, and the composite coating with the main phase of zirconium boride, zirconium carbide and silicon carbide is generated in situ. The existence of the silicon carbide in the coating can not only improve the high-temperature oxidation resistance of the coating, but also ensure that the coating obtains the crack self-healing capability. The zirconium boride-zirconium carbide-silicon carbide composite coating has high density, hardness, wear resistance, corrosion resistance, thermal shock resistance, oxidation resistance and ablation resistance.
The invention has the following beneficial effects:
(1) the zirconium boride-zirconium carbide-silicon carbide composite coating is prepared by adopting the zirconium/boron carbide/silicon carbide composite powder and the zirconium oxide/boron carbide/aluminum/silicon carbide composite powder for the first time, the selected raw material powder is rich in resources and relatively low in price, the thermal spraying technology is adopted, the preparation process is simple, the cost is low, and the novel method for preparing the zirconium boride-zirconium carbide-silicon carbide composite coating is provided.
(2) The zirconium boride-zirconium carbide-silicon carbide composite coating prepared by the method overcomes the defects that the zirconium boride, the zirconium carbide and the silicon carbide are isolated from each other and are not bonded in a loose state, the main phase, namely the zirconium boride and the zirconium carbide, in the prepared zirconium boride-zirconium carbide-silicon carbide composite coating are formed by in-situ reaction, the interfaces of the phases are pure, the interphase bonding is tight, and the cohesive strength of the coating is high. The defects of complex process, high cost, large energy consumption, large pollution, low efficiency, low coating thickness, low coating density and low binding force between the coating and a substrate in the prior art for preparing the zirconium boride-zirconium carbide-silicon carbide composite coating are overcome.
(3) The zirconium boride-zirconium carbide-silicon carbide composite coating prepared by the method has high density, hardness, toughness, wear resistance, corrosion resistance, high-temperature oxidation resistance and ablation resistance, and the in-situ formation of zirconium boride and zirconium carbide phases in the coating is favorable for improving the hardness, toughness, high-temperature resistance, thermal shock resistance, high-temperature oxidation resistance and ablation resistance of the coating; the existence of the silicon carbide phase in the coating can not only improve the high-temperature oxidation resistance of the coating, but also enable the coating to obtain the crack self-healing capability, thereby expanding the application range of the zirconium boride-zirconium carbide-silicon carbide composite coating in a high-temperature environment.
(4) In order to obtain the zirconium boride-zirconium carbide-silicon carbide composite coating with excellent performance, a raw material system is optimized firstly, the inventor team successfully adopts the method to prepare the zirconium boride-zirconium carbide-silicon carbide composite coating through years of deep research and hundreds of repeated experiments, the preparation process is simple, the performance of the obtained zirconium boride-zirconium carbide-silicon carbide composite coating is good, and unexpected technical effects and obvious economic benefits are obtained in advance.
Compared with the oxidation resistance and the ablation resistance of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared by the same process, the oxidation resistance of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared by the invention is improved by 16% at most, and the mass ablation rate is reduced by 1.86%.
Drawings
The invention is further illustrated with reference to the following figures and examples.
Fig. 1 is an XRD spectrum of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared in example 2.
Fig. 2 is an SEM image of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared in example 2.
Fig. 3 is a high-magnification SEM image of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared in example 2.
FIG. 4 is an XRD pattern of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared in example 16.
FIG. 5 is an SEM photograph of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared in example 16.
FIG. 6 is a high magnification SEM image of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared in example 16.
Detailed Description
Example 1
The preparation method of the zirconium boride-zirconium carbide-silicon carbide composite coating adopts a method of in-situ synthesis of the zirconium boride-zirconium carbide-silicon carbide composite coating, and comprises the following steps:
firstly, preparing zirconium/boron carbide/silicon carbide composite powder for thermal spraying:
uniformly mixing zirconium powder with the particle size range of 0.001-10 microns, boron carbide powder with the particle size range of 0.001-10 microns and silicon carbide powder with the particle size range of 0.001-10 microns into composite powder, wherein the weight percentage of the silicon carbide powder to the total mass of the three raw material powders, namely the zirconium powder, the boron carbide powder and the silicon carbide powder is 5%, the weight percentage of the zirconium powder to the boron carbide powder to the total mass of the three raw material powders, namely the zirconium powder, the boron carbide powder and the silicon carbide powder is 95%, the weight ratio of the zirconium powder to the boron carbide powder is 60:40, and uniformly mixing a binder (methyl cellulose, the same as in examples 2-15), wherein the weight ratio of the binder to the composite powder is 100:0.1, so as to prepare the zirconium/boron carbide/silicon carbide composite powder for thermal spraying;
secondly, preprocessing a base material:
the base material is nickel-based superalloy, the pretreatment mode adopts sand blasting, and then a NiAl bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the nickel-based superalloy base material after the sand blasting;
step three, preparing the zirconium boride-zirconium carbide composite coating:
by usingThe atmospheric plasma spraying method comprises the following process parameters: the flow of the powder feeding gas is 0.3m3H, the arc power is 32KW, the distance of the spray gun is 80mm, and the powder feeding gas is argon (the same as the powder feeding gas in the following embodiments); and spraying the zirconium/boron carbide/silicon carbide composite powder prepared in the first step for thermal spraying on the surface of the nickel-based high-temperature alloy base material pretreated in the second step to form a zirconium boride-zirconium carbide-silicon carbide composite coating with the thickness of 200 microns.
Example 2
The preparation method of the zirconium boride-zirconium carbide-silicon carbide composite coating adopts a method for synthesizing the zirconium boride-zirconium carbide-silicon carbide composite coating in situ, and comprises the following steps:
the first step, preparing zirconium/boron carbide/silicon carbide composite powder for thermal spraying:
uniformly mixing zirconium powder with the granularity range of 0.001-10 microns, boron carbide powder with the granularity range of 0.001-10 microns and silicon carbide powder with the granularity range of 0.001-10 microns into composite powder, wherein the weight percentage of the silicon carbide powder to the total mass of the three raw material powders of the zirconium powder, the boron carbide powder and the silicon carbide powder is 10%, the weight percentage of the zirconium powder to the boron carbide powder to the total mass of the three raw material powders of the zirconium powder, the boron carbide powder and the silicon carbide powder is 90%, the weight ratio of the zirconium powder to the boron carbide powder is 83:17, and uniformly mixing the zirconium powder to the silicon carbide powder into a binder, wherein the weight ratio of the composite powder to the binder is 1: 0.1, thereby formulating a zirconium/boron carbide/silicon carbide composite powder for thermal spraying;
secondly, preprocessing a base material:
the base material is titanium alloy, the pretreatment mode adopts sand blasting, and then a NiCrAlY bonding layer is sprayed on the surface of the titanium alloy base material after the sand blasting;
thirdly, preparing the zirconium boride-zirconium carbide-silicon carbide composite coating:
an atmospheric plasma spraying method is adopted, and the technological parameters are as follows: the flow of the powder feeding gas is 0.5m3H arc power 35KW and lance distance 100mm, zirconium/carbide prepared in the first step above for thermal sprayingAnd spraying boron/silicon carbide composite powder on the surface of the titanium alloy base material pretreated in the second step to form the zirconium boride-zirconium carbide-silicon carbide composite coating.
Fig. 1 is an XRD pattern of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared in this example, and it can be seen from the XRD pattern that the zirconium boride-zirconium carbide-silicon carbide composite coating is mainly composed of zirconium boride, zirconium carbide, silicon carbide and zirconium oxide phases. It can be seen that the zirconium boride-zirconium carbide-silicon carbide composite coating with the main components of zirconium boride, zirconium carbide and silicon carbide can be successfully prepared on the surface of the matrix by using the zirconium/boron carbide/silicon carbide composite powder as the raw material and adopting an atmospheric plasma spraying method. Fig. 2 is an SEM image of the zirconium boride-zirconium carbide-silicon carbide composite coating layer prepared in this example. It can be seen that the coating has a higher density. Fig. 3 is a high-magnification SEM image of the zirconium boride-zirconium carbide-silicon carbide composite coating obtained in this example. From this high magnification SEM image it can be seen that the coating consists of a large number of fine grains. As can be seen from the comprehensive analysis of the figures 1,2 and 3, the zirconium boride-zirconium carbide-silicon carbide composite coating with the main components of zirconium boride, zirconium carbide and silicon carbide can be successfully prepared on the surface of the matrix by using the zirconium/boron carbide/silicon carbide composite powder as the raw material and adopting the atmospheric plasma spraying method.
Example 3
The preparation method of the zirconium boride-zirconium carbide-silicon carbide composite coating adopts a method for synthesizing the zirconium boride-zirconium carbide-silicon carbide composite coating in situ, and comprises the following steps:
the first step, preparing zirconium/boron carbide/silicon carbide composite powder for thermal spraying:
uniformly mixing zirconium powder with the granularity range of 0.001-10 microns, boron carbide powder with the granularity range of 0.001-10 microns and silicon carbide powder with the granularity range of 0.001-10 microns into composite powder, wherein the silicon carbide powder accounts for 30 wt% of the total mass of the three raw materials, namely the zirconium powder, the boron carbide powder and the silicon carbide powder, the zirconium powder, the boron carbide powder and the silicon carbide powder account for 70 wt% of the total mass of the three raw materials, the weight ratio of the zirconium powder to the boron carbide powder is 90:10, and uniformly mixing the zirconium powder to the boron carbide powder with a binder, wherein the weight ratio of the composite powder to the binder is 1, so that the zirconium/boron carbide/silicon carbide composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the matrix material is graphite, and the pretreatment mode adopts sand blasting treatment;
thirdly, preparing the zirconium boride-zirconium carbide-silicon carbide composite coating:
an atmospheric plasma spraying method is adopted, and the technological parameters are as follows: the flow of the powder feeding gas is 0.6m3And h, the electric arc power is 45KW, the distance between spray guns is 120mm, and the zirconium/boron carbide/silicon carbide composite powder for thermal spraying prepared in the first step is sprayed on the surface of the graphite base material pretreated in the second step, so that the zirconium boride-zirconium carbide-silicon carbide composite coating with the thickness of 200 microns is formed.
Example 4
The process was the same as example 1 except that the metal substrate was cast iron and the adhesive layer was a FeAl base layer.
Example 5
The process is the same as example 2 except that the metal material substrate is aluminum alloy and the bonding layer is a NiCrAlY bottom layer.
Example 6
The process is the same as example 1 except that the metal material substrate is copper alloy and the bonding layer is CoCrAlY.
Example 7
The process was the same as in example 2 except that the metal substrate was steel and the adhesion layer was CoNiCrAlY.
Example 8
The process is the same as that of example 1 except that the metal material substrate is magnesium alloy and the bonding layer is NiCoCrAlYTa.
Example 9
The process was the same as in example 1 except that the metallic material substrate was a cobalt-based superalloy and the bond coat was NiCrBSi.
Example 10
The process was the same as example 2 except that the metallic material substrate was an intermetallic compound and the bond coat was NiCrAl.
Example 11
The process was the same as in example 2 except that the metallic material substrate was a nickel-zirconium alloy and the bonding layer was NiCrAl.
Example 12
The process is the same as example 3 except that the inorganic non-metallic material substrate is a carbon/carbon composite material (i.e., a carbon-based composite material with carbon fibers as a reinforcing phase), and the pretreatment method is performed by sanding.
Example 13
The process is the same as example 3 except that the inorganic nonmetallic material matrix is a carbon/silicon carbide composite material.
Example 14
The process is the same as example 3 except that the inorganic nonmetallic material matrix is a silicon carbide/silicon carbide composite material.
In the above examples, the raw materials are commercially available, and the sand blasting process, the sanding process, the bonding layer spraying process, the bonding layer preparation process and the thermal spraying process are well known in the art.
Example 15
The preparation method of the zirconium boride-zirconium carbide-silicon carbide composite coating adopts a method of in-situ synthesis of the zirconium boride-zirconium carbide-silicon carbide composite coating, and comprises the following steps:
firstly, preparing zirconium oxide/boron carbide/aluminum/silicon carbide composite powder for thermal spraying:
uniformly mixing zirconia powder with the particle size range of 0.001-10 microns, boron carbide powder with the particle size range of 0.001-10 microns, aluminum powder with the particle size range of 0.1-10 microns and silicon carbide powder with the particle size range of 0.001-10 microns into composite powder, wherein the silicon carbide powder accounts for 5 percent by weight of the total mass of the zirconia powder, the boron carbide powder, the aluminum powder and the silicon carbide powder, the zirconia powder, the boron carbide powder, the aluminum powder and the silicon carbide powder account for 95 percent by weight of the total mass of the zirconia powder, the boron carbide powder and the aluminum powder, the zirconia powder, the boron carbide powder and the aluminum powder account for 5 percent by weight of the total mass of the zirconia powder, the boron carbide powder and the three raw materials, the weight percent of the total mass of the zirconia powder, the boron carbide powder and the silicon carbide powder is 95 percent by weight, and the weight ratio of the zirconia powder to the aluminum powder is 60:40, uniformly mixing a binder (polyvinyl alcohol, the same as in the following example) in a weight ratio of 100:0.1 to prepare zirconia/boron carbide/aluminum/silicon carbide composite powder for thermal spraying;
secondly, preprocessing a base material:
the base material is nickel-based superalloy, the pretreatment mode adopts sand blasting, and then a NiAl bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the nickel-based superalloy base material after the sand blasting;
step three, preparing the zirconium boride composite coating:
an atmospheric plasma spraying method is adopted, and the technological parameters are as follows: the flow of the powder feeding gas is 0.5m3And h, the electric arc power is 36KW, the distance between spray guns is 110mm, and the zirconium oxide/boron carbide/aluminum/silicon carbide composite powder for thermal spraying prepared in the first step is sprayed on the surface of the nickel-based high-temperature alloy base material pretreated in the second step, so that the zirconium boride-zirconium carbide-silicon carbide composite coating with the thickness of 200 microns is formed.
Example 16
The preparation method of the zirconium boride-zirconium carbide-silicon carbide composite coating adopts a method of in-situ synthesis of the zirconium boride-zirconium carbide-silicon carbide composite coating, and comprises the following steps:
firstly, preparing zirconium oxide/boron carbide/aluminum/silicon carbide composite powder for thermal spraying:
uniformly mixing zirconia powder with the particle size range of 0.001-10 microns, boron carbide powder with the particle size range of 0.001-10 microns, aluminum powder with the particle size range of 0.1-10 microns and silicon carbide powder with the particle size range of 0.001-10 microns into composite powder, wherein the silicon carbide powder accounts for 7% by weight of the total mass of the zirconia powder, the boron carbide powder, the aluminum powder and the silicon carbide powder, the zirconia powder, the boron carbide powder, the aluminum powder, the zirconia powder, the boron carbide powder, the aluminum powder and the silicon carbide powder account for 93% by weight of the total mass of the zirconia powder, the boron carbide powder and the aluminum powder, the zirconia powder and the boron carbide powder account for 10% by weight of the total mass of the zirconia powder, the boron carbide powder and the aluminum powder, and the aluminum powder account for 90% by weight of the total mass of the zirconia powder, the boron carbide powder and the aluminum powder, the weight ratio of the zirconia powder to the aluminum powder is 78: 22.
Uniformly mixing the powder with a binder, wherein the weight ratio of the composite powder to the binder is 100:1, and preparing the zirconium oxide/boron carbide/aluminum/silicon carbide composite powder for thermal spraying;
secondly, preprocessing a base material:
the base material is titanium alloy, the pretreatment mode adopts sand blasting, and then a NiCrAlY bonding layer with the thickness of 50 microns is sprayed on the surface of the titanium alloy base material after the sand blasting;
step three, preparing the zirconium boride composite coating:
an atmospheric plasma spraying method is adopted, and the technological parameters are as follows: the flow of the powder feeding gas is 0.6m3And h, the electric arc power is 40KW, the distance between spray guns is 120mm, and the zirconium oxide/boron carbide/aluminum/silicon carbide composite powder for thermal spraying prepared in the first step is sprayed on the surface of the titanium alloy base material pretreated in the second step, so that the zirconium boride-zirconium carbide-silicon carbide composite coating with the thickness of 200 microns is formed.
Fig. 4 is an XRD pattern of the zirconium boride-zirconium carbide-silicon carbide composite coating prepared in this example, from which it can be seen that the zirconium boride-zirconium carbide-silicon carbide composite coating is mainly composed of zirconium boride, zirconium carbide, silicon carbide and zirconium oxide phases. It can be seen that the zirconium boride-zirconium carbide-silicon carbide composite coating with zirconium boride, zirconium carbide, silicon carbide and zirconium oxide as main components can be successfully prepared on the surface of the matrix by using the zirconium oxide/boron carbide/aluminum/silicon carbide composite powder as a raw material and adopting an atmospheric plasma spraying method. Fig. 5 is an SEM image of the zirconium boride-zirconium carbide-silicon carbide composite coating layer prepared in the present example. It can be seen that the coating has higher density and the coating is well combined with the matrix. Fig. 6 is a high-magnification SEM image of the zirconium boride-zirconium carbide-silicon carbide composite coating obtained in the present example. From this high magnification SEM image it can be seen that the coating consists of a large number of fine grains. It can be known from the comprehensive analysis of fig. 4, 5 and 6 that the zirconium boride-zirconium carbide-silicon carbide composite coating with the main components of zirconium boride, zirconium carbide, silicon carbide and zirconium oxide in the fine crystal structure can be successfully prepared on the surface of the matrix by using the zirconium oxide/boron carbide/aluminum/silicon carbide composite powder as the raw material and adopting the atmospheric plasma spraying method.
Table 1 shows the performance data of the zirconium boride-zirconium carbide-silicon carbide composite coatings obtained in examples 2 and 16, wherein the first line shows the performance of the coating obtained by plasma spraying the zirconium/boron carbide/silicon carbide composite powder in example 2, the second line shows the performance of the coating obtained by plasma spraying the zirconium oxide/boron carbide/aluminum/silicon carbide composite powder in example 16, the third line shows the performance of the coating obtained by plasma spraying the zirconium/boron carbide composite powder, and the fourth line shows the performance of the coating obtained by plasma spraying the zirconium oxide/boron carbide/aluminum carbide composite powder. As can be seen from the comparison of the performance data of the four coatings in Table 1, the performance (wear resistance, thermal shock resistance, oxidation resistance and ablation resistance) of the coating obtained by plasma spraying the zirconium/boron carbide/silicon carbide composite powder and the coating obtained by plasma spraying the zirconium/boron carbide/aluminum/silicon carbide composite powder (comparative examples 1 and 2) is obviously improved compared with the coating obtained by plasma spraying the zirconium/boron carbide/aluminum carbide composite powder and the coating obtained by plasma spraying the zirconium/boron carbide/aluminum carbide composite powder.
Table 1 shows the performance data of the zirconium boride-zirconium carbide-silicon carbide composite coatings obtained in examples 2 and 16
Figure BDA0002411818520000091
Example 17
The preparation method of the zirconium boride-zirconium carbide-silicon carbide composite coating adopts a method for synthesizing the zirconium boride-zirconium carbide-silicon carbide composite coating in situ, and comprises the following steps:
firstly, preparing zirconium oxide/boron carbide/aluminum/silicon carbide composite powder for thermal spraying:
uniformly mixing zirconia powder with the granularity range of 0.001-10 microns, boron carbide powder with the granularity range of 0.001-10 microns, aluminum powder with the granularity range of 0.1-10 microns and silicon carbide powder with the granularity range of 0.001-10 microns into composite powder, wherein the silicon carbide powder accounts for 30 percent by weight of the total mass of the zirconia powder, the boron carbide powder, the aluminum powder and the silicon carbide powder, the zirconia powder, the boron carbide powder, the aluminum powder and the silicon carbide powder account for 70 percent by weight of the total mass of the zirconia powder, the boron carbide powder and the aluminum powder, the zirconium oxide powder accounts for 30 percent by weight of the total mass of the zirconia powder, the boron carbide powder and the aluminum powder, the zirconium oxide powder accounts for 70 percent by weight of the total mass of the zirconia powder, the boron carbide powder and the silicon carbide powder, and the weight ratio of the zirconia powder to the aluminum powder is 90:10, uniformly mixing the powder with a binder, wherein the weight ratio of the composite powder to the binder is 100:3, and preparing the zirconium oxide/boron carbide/aluminum/silicon carbide composite powder for thermal spraying;
secondly, preprocessing a base material:
the matrix material is graphite, and the pretreatment mode adopts sand blasting treatment;
thirdly, preparing the zirconium boride-zirconium carbide-silicon carbide composite coating:
the plasma spraying method is adopted, and the technological parameters are as follows: the flow of the powder feeding gas is 0.6m3And h, the electric arc power is 42KW, the distance between spray guns is 90mm, and the zirconium oxide/boron carbide/aluminum/silicon carbide composite powder for thermal spraying prepared in the first step is sprayed on the surface of the graphite base material pretreated in the second step, so that the zirconium boride-zirconium carbide-silicon carbide composite coating with the thickness of 200 microns is formed.
Example 18
The same process as in example 15 was performed except that the metal material substrate was cast iron and the adhesive layer was a FeAl base layer.
Example 19
The process was the same as in example 16 except that the metal substrate was aluminum alloy and the adhesion layer was a NiCrAlY primer layer.
Example 20
The same process as in example 15 was performed except that the metal material substrate was a copper alloy and the adhesive layer was CoCrAlY.
Example 21
The process was the same as in example 16 except that the base metal material was steel and the bond coat was CoNiCrAlY.
Example 22
The same process as in example 15 was performed except that the base metal material was magnesium alloy and the adhesion layer was NiCoCrAlYTa.
Example 23
The process was the same as in example 15 except that the metallic material substrate was a cobalt-based superalloy and the bond coat was NiCrBSi.
Example 24
The process was the same as in example 16 except that the metallic material substrate was an intermetallic compound and the bond coat was NiCrAl.
Example 25
The same procedure as in example 16 was repeated except that the metallic material substrate was made of a nickel-zirconium alloy and the binder layer was made of NiCrAl.
Example 26
The same process as in example 17 was performed except that the inorganic nonmetallic material substrate was a carbon/carbon composite material and the pretreatment was performed by sanding.
Example 27
The process is the same as example 17 except that the inorganic nonmetallic material matrix is a carbon/silicon carbide composite material.
Example 28
The same process as in example 17 was conducted except that the inorganic nonmetallic material substrate was a silicon carbide/silicon carbide composite material.
Comparative example 1
The base material is TC4 titanium alloy, the pretreatment mode adopts sand blasting, and then NiCrAlY bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the TC4 titanium alloy base material after the sand blasting; spraying zirconium/boron carbide composite powder on the surface of the pretreated TC4 titanium alloy matrix material,the parameters of the thermal spraying process are as follows: the flow of the powder feeding gas is 0.3m3H, the electric arc power is 35KW, the distance of a spray gun is 100mm, and the powder feeding gas is argon; thereby synthesizing the zirconium boride-zirconium carbide composite coating with the thickness of 200 microns.
Comparative example 2
The base material is TC4 titanium alloy, the pretreatment mode adopts sand blasting, and then NiCrAlY bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the TC4 titanium alloy base material after the sand blasting; spraying zirconium oxide/boron carbide/aluminum composite powder on the surface of the pretreated TC4 titanium alloy matrix material, wherein the parameters of the thermal spraying process are as follows: the flow of the powder feeding gas is 0.3m3H, the electric arc power is 35KW, the distance of a spray gun is 100mm, and the powder feeding gas is argon; thereby synthesizing the zirconium boride-zirconium carbide-alumina composite coating with the thickness of 200 microns.
In the above examples, the raw materials are commercially available, and the sand blasting process, the sanding process, the bonding layer spraying process and the bonding layer preparation process are well known in the art.
The invention is not the best known technology.

Claims (6)

1. A preparation method of a zirconium boride-zirconium carbide-silicon carbide composite coating is characterized by comprising the following steps:
the first step is any one of the following two methods:
the method comprises the following steps: preparing zirconium/boron carbide/silicon carbide composite powder:
zirconium powder, boron carbide powder and silicon carbide powder are mixed into composite powder, and then mixed into a binder, so that zirconium/boron carbide/silicon carbide composite powder for thermal spraying is prepared;
the silicon carbide powder accounts for 5-30% of the composite powder by mass, the weight ratio of the zirconium powder to the boron carbide powder is 60-90: 40-10, and the binder is used in a weight ratio of the composite powder to the binder of 100: 0.1-3;
or, preparing zirconium oxide/boron carbide/aluminum/silicon carbide composite powder by the second method:
mixing zirconia powder, boron carbide powder, aluminum powder and silicon carbide powder into composite powder, and uniformly mixing the composite powder with a binder to prepare zirconia/boron carbide/aluminum/silicon carbide composite powder for thermal spraying;
wherein the silicon carbide powder accounts for 5-30% of the composite powder, the boron carbide powder accounts for 5-30% of the total mass of the zirconia powder, the boron carbide powder and the aluminum powder, the weight ratio of the zirconia powder to the aluminum powder is 60-90: 40-10, the binder is used in a weight ratio of the composite powder to the binder of 100: 0.1-3,
secondly, the surface of the base material with the required coating is pretreated in one of the following two ways:
1) when the base material is a metal base material, firstly, sand blasting is adopted, and then a bonding layer is sprayed on the surface of the metal base material after the sand blasting;
or, 2) when the base material is an inorganic non-metallic material base, adopting sand blasting or sand paper polishing treatment;
thirdly, preparing the zirconium boride-zirconium carbide-silicon carbide composite coating:
spraying the composite powder for thermal spraying prepared in the first step on the surface of the base material pretreated in the second step by adopting a thermal spraying method, so as to obtain a zirconium boride-zirconium carbide-silicon carbide composite coating through in-situ synthesis;
the technological parameters of the thermal spraying method are as follows: the flow of the powder feeding gas is 0.3-0.6 m3The arc power is 32-45 KW, and the distance between spray guns is 80-120 mm;
the particle sizes of the zirconium powder, the boron carbide powder and the silicon carbide powder are all 0.001-10 microns; the granularity of the aluminum powder is 0.1-10 microns;
the binder is polyvinyl alcohol or methyl cellulose.
2. The method for preparing zirconium boride-zirconium carbide-silicon carbide composite coating according to claim 1, wherein the thickness of the coating is 200-500 μm.
3. The method of preparing a zirconium boride-zirconium carbide-silicon carbide composite coating according to claim 1, wherein the metallic material substrate is steel, cast iron, aluminum alloy, copper alloy, titanium alloy, magnesium alloy, nickel-based superalloy, nickel-chromium alloy, cobalt-based superalloy, tantalum-based alloy, tungsten-based alloy, or intermetallic compound.
4. The method for preparing zirconium boride-zirconium carbide-silicon carbide composite coating according to claim 1, characterized in that the inorganic non-metallic material matrix is graphite, carbon/carbon composite, carbon/silicon carbide composite or silicon carbide/silicon carbide composite.
5. The method for preparing zirconium boride-zirconium carbide-silicon carbide composite coating according to claim 1, characterized in that the bonding layer material is: NiAl, NiCrAl, FeAl, NiCrAlY, CoCrAlY, CoNiCrAlY, NiCoCrAlYTa or NiCrBSi.
6. The method of preparing a zirconium boride-zirconium carbide-silicon carbide composite coating according to claim 1 wherein the powder feeding gas in the thermal spraying is argon gas.
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