CN111235511B - Preparation method of multi-element ceramic composite coating - Google Patents

Preparation method of multi-element ceramic composite coating Download PDF

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CN111235511B
CN111235511B CN202010178922.7A CN202010178922A CN111235511B CN 111235511 B CN111235511 B CN 111235511B CN 202010178922 A CN202010178922 A CN 202010178922A CN 111235511 B CN111235511 B CN 111235511B
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powder
oxide
silicon carbide
aluminum
coating
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CN111235511A (en
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杨勇
王彦伟
王晓龙
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
    • C23C4/02—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
    • C23C4/10—Oxides, borides, carbides, nitrides or silicides; Mixtures thereof
    • 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
    • C23C4/134—Plasma spraying

Abstract

The invention relates to a preparation method of a multi-element ceramic composite coating. The method comprises the following steps: first step, preparing oxide/silicon carbide/aluminum composite powder for thermal spraying: the oxide is 1-4 of zirconium oxide, titanium oxide, hafnium oxide, tantalum oxide, niobium oxide, vanadium oxide, chromium oxide, molybdenum oxide or tungsten oxide; secondly, pretreating the surface of the base material of the coating; and thirdly, spraying the oxide/silicon carbide/aluminum composite powder on the surface of the matrix material by adopting a thermal spraying method, thereby obtaining the multi-element ceramic composite coating through in-situ synthesis. The invention overcomes the defects of complex process, high cost, large pollution, low deposition efficiency, poor coating performance and unsuitability for large-scale industrial production in the prior art for preparing the multi-element ceramic composite coating.

Description

Preparation method of multi-element ceramic composite coating
Technical Field
The technical scheme of the invention relates to plating of carbide, silicide and oxide on materials, in particular to a preparation method of a multi-ceramic composite coating.
Background
The carbide has high melting point (3880 ℃), high hardness, good comprehensive performances of heat conduction, electric conduction, wear resistance, corrosion resistance and the like, and has important application value in the fields of machinery, metallurgy, aerospace, nuclear, military and the like. Among them, titanium carbide is a typical transition metal carbide, and titanium carbide is a most widely developed material among titanium, zirconium, and chromium transition metal carbides, and is widely applied in many fields such as machinery, electronics, chemical engineering, environmental protection, fusion reactors, national defense industry, and the like, and especially widely used as a protective coating for structural materials. Zirconium carbide, as a refractory metal carbide, has excellent characteristics of high melting point (3420 ℃), high hardness (25.5GPa), high thermal and electrical conductivity, high chemical stability and the like, and is widely applied to the fields of emitter surface coatings, nuclear fuel particle coatings, thermo-electro-optical radiator coatings, ultrahigh temperature refractory materials and the like. Niobium carbide has high melting point (3610 ℃), high hardness, high elastic modulus, high wear resistance, thermodynamic stability and other properties. Therefore, the niobium carbide coating is prepared on the surface of the metal workpiece substrate, the surface hardness of the niobium carbide coating can be greatly improved to be more than HV2800, and the working temperature of the workpiece is improved, so that the service life of the niobium carbide coating is prolonged, and the niobium carbide coating has important application value in the fields of machinery, metallurgy, aerospace, nuclear, military and the like. The tantalum carbide has a very high melting point (3985 ℃), and the tantalum carbide coating is an important high-temperature structural material with high strength, corrosion resistance and good chemical stability, has excellent high-temperature mechanical property, high-speed airflow scouring resistance and ablation resistance, and has good chemical compatibility and mechanical compatibility with graphite and carbon/carbon composite materials. Molybdenum carbide has high hardness, good thermal stability and corrosion resistance, can be used as a high-temperature material in a neutral or reducing atmosphere at a temperature of more than 2000 ℃, can resist corrosion of cold potassium hydroxide and sodium hydroxide solution, and has been applied in various mechanical fields with high temperature resistance, wear resistance and chemical corrosion resistance. Tungsten carbide, as a refractory metal carbide, has excellent characteristics of high melting point (2870 ℃), high hardness (2000HV), high thermal and electrical conductivity, high chemical stability and the like, is widely applied to the fields of emitter surface coatings, nuclear fuel particle coatings, thermophotovoltaic radiator coatings, ultrahigh temperature refractory materials and the like, is a main raw material for manufacturing hard alloys, has good chemical stability and thermal stability, and still has high thermal hardness in a 1000 ℃ working environment. The chromium carbide has the advantages of high-temperature hardness (HV 1500-2100), good wear resistance, good corrosion resistance, low density and the like, and particularly has a thermal expansion coefficient close to that of steel and good matching with a base body component. Chromium carbide is one of the most widely applied coating materials in the high-temperature (600-900 ℃) environment at present, and is widely applied to industries such as metallurgy, aviation, electric power, nuclear energy and the like. The chromium carbide phase increases the hardness of the coating, which can produce a dense protective film of chromium oxide at high temperatures. The chromium carbide has good wear resistance and corrosion resistance, and is widely applied to the protective coating of parts. Hafnium carbide has a very high melting point (3890 ℃), and is a good material for the lining of high melting point metal melting crucibles. Hafnium carbide has high hardness, can be used as an additive of hard alloy, and has been widely applied in the fields of cutting tools and dies; the material also has high elastic coefficient, good electric thermal conductivity, smaller thermal expansion coefficient and better impact property, is suitable for rocket nozzle materials, can be used for the nose cone part of a rocket, has important application in the field of aerospace, and also has important application in the aspects of spray pipes, high-temperature resistant linings, electric arcs or electrodes for electrolysis. The hafnium carbide has good solid phase stability and chemical corrosion resistance, and has great potential for being used in high temperature environment. In addition, the hafnium carbide film is evaporated on the surface of the carbon nanotube cathode, so that the field emission performance of the carbon nanotube cathode can be well improved; the introduction of hafnium carbide into the carbon/carbon composite material may improve its ablation resistance. Hafnium carbide has many excellent physical and chemical properties, which makes it very widely used in current ultra-high temperature materials.
However, the great brittleness, poor thermal shock resistance and poor high temperature oxidation resistance of carbide ceramic coatings have limited further applications to some extent. Researches show that the ceramic composite coating can reduce the brittleness of a single-phase refractory carbide ceramic coating and improve the thermal shock resistance and high-temperature oxidation resistance of the single-phase refractory carbide ceramic coating, so that the multi-element ceramic composite coating is attracted by people as a high-temperature structural material. The silicide (zirconium silicide, titanium silicide, chromium silicide, hafnium silicide, niobium silicide, tantalum silicide, vanadium silicide, tungsten silicide, etc.) has low density, good thermal stability and strong oxidation resistance. The addition of silicide in carbide can not only reduce the brittleness of the carbide coating and improve the thermal shock resistance and high-temperature oxidation resistance of the carbide coating,the coating can also obtain the self-healing capability of cracks. When the coating generates cracks in the service process of high-temperature severe environment, silicide on the surfaces of the cracks and nearby the cracks can be quickly oxidized to generate silicon dioxide (SiO)2) And another oxide, SiO2The crack can be sealed as a mobile phase; on the other hand, the volume expansion of the oxidation reaction and the high thermal expansion coefficient of the silicide can make the crack under compressive stress, accelerate the healing of the crack, and thus the coating has better healing capability [ patent CN201410199003.2 ]. The silicide has a better oxidation resistance than the corresponding boride.
At present, the technical problems of preparing the multi-element ceramic composite coating are as follows:
(1) the disadvantages of chemical vapor deposition are: 1) the obtained coating has too small thickness, low deposition efficiency, low production efficiency and difficult preparation of thicker coatings; 2) it is difficult to deposit a thin film on a substrate locally or on a surface; 3) the reaction source participating in the deposition reaction and the residual gas after the reaction are mostly toxic, flammable and explosive gases, are dangerous to operate and pollute the environment; 4) the equipment requirements are strict, and the equipment is required to have corrosion resistance, so that the preparation cost is high.
(2) The disadvantages of the physical vapor deposition method are: 1) the deposition efficiency is low, and the production efficiency is low; 2) the film-base binding force is weak, the coated film is not wear-resistant, and chemical impurities are difficult to remove; 3) the method has complex equipment and large one-time investment.
(3) The disadvantages of the laser cladding method are: 1) the equipment has large one-time investment and high operation cost, and particularly, when large-area cladding is carried out, the probability of metallurgical defects is increased because the size of a light spot is small and a lapping process measure must be adopted; 2) in the process of laser cladding of the ceramic coating, the cracking phenomenon is easy to generate, so that the quality of the coating is reduced.
(4) The disadvantages of the slurry coating method are: 1) the slurry coating method is imperfect, and the coating thickness of the part is difficult to be uniform; 2) the coating properties depend to a large extent on the technical proficiency of the operator; under the condition of same thickness and same components, the slurry method coating has lower fracture resistance because of not compact; 3) the coating prepared by the method has poor bonding force with a matrix, poor thermal shock resistance, high sintering temperature and easy introduction of impurities.
(5) The disadvantages of the embedding method are: the embedding process usually needs to put the matrix material in a high-temperature environment for heat preservation (2000 ℃ -3000 ℃), so the defects of large heat damage to the matrix and high cost exist; meanwhile, the deposition and diffusion speeds of different elements are different, so that the thickness of the 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.
(6) The thermal spraying method is a method of heating a spray material to a molten or semi-molten state using a heat source and spray-depositing the spray material onto a pretreated substrate surface at a relatively high speed to form a coating layer. However, the problem of direct spray of multi-component ceramic powders by thermal spray processes to produce multi-component ceramic composite coatings is: 1) because the melting point of the refractory compounds (carbides and silicides) of the transition metals is very high, the residence time of the powder in the hot spraying high-temperature flame flow is short, the melting effect is not ideal, the deposition efficiency is low, and the porosity of the coating is high; 2) the carbide and the silicide are easily oxidized and decomposed by thermal spraying under the atmospheric condition or the oxidizing atmosphere; 3) the strong covalent bonding force in carbide and silicide crystals can cause that the diffusion sintering phenomenon is difficult to generate among particles during deposition in the thermal spraying process, so that the carbide and the silicide particles are isolated and not bonded with each other, are in a loose state and have high porosity of a coating.
Disclosure of Invention
The invention aims to provide a preparation method of a multi-element ceramic composite coating aiming at the defects in the prior art. The method is synthesized by adopting thermal spraying in-situ reaction, only oxide, silicon carbide and aluminum powder are mixed and then thermally sprayed, and the oxide, the silicon carbide and the aluminum react to generate carbide, silicide and alumina phases in situ in the thermal spraying process, so that the multi-element ceramic composite coating (the carbide-silicide-aluminum oxide composite coating) is obtained by the thermal spraying in-situ reaction. The invention overcomes the defects of complex process, high cost, large pollution, low deposition efficiency, poor coating performance and unsuitability for large-scale industrial production in the prior art for preparing the multi-element ceramic composite coating. Meanwhile, the invention also overcomes the defect that the high-temperature oxidation resistance is poor because no silicide or silicon carbide exists in the obtained coating because boron carbide is used as a raw material in the process of preparing the boride-carbide ceramic composite coating in the prior art.
The technical scheme adopted by the invention for solving the technical problem is as follows:
a preparation method of a multi-element ceramic composite coating comprises the following steps:
first step, preparing oxide/silicon carbide/aluminum composite powder for thermal spraying:
mixing oxide powder, silicon carbide powder and aluminum powder into composite powder, and then mixing the composite powder with a binder to prepare oxide/silicon carbide/aluminum composite powder for thermal spraying;
wherein the silicon carbide powder accounts for 5-30% of the composite powder by mass, and the mass ratio of the oxide powder to the aluminum powder is 60-90: 10-40; the binder is used in a weight ratio of 100: 0.1-2, the oxide is any x of zirconium oxide, titanium oxide, hafnium oxide, tantalum oxide, niobium oxide, vanadium oxide, chromium oxide, molybdenum oxide or tungsten oxide, and x is 1,2,3 or 4;
the binder is polyvinyl alcohol or methyl cellulose;
the granularity of the oxide powder and the silicon carbide powder is 0.001-10 microns; the granularity of the aluminum powder is 0.1-10 microns;
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, performing sand blasting treatment, and then spraying a bonding layer on the surface of the metal base material subjected to the sand blasting treatment;
or, 2) when the base material is an inorganic non-metallic material base, adopting sand blasting or sand paper polishing treatment;
step three, preparing the multi-element ceramic composite coating:
spraying the oxide/silicon carbide/aluminum composite powder for thermal spraying prepared in the first step on the surface of the pretreated substrate material in the second step by adopting a thermal spraying method, so as to obtain a multi-element ceramic composite coating through in-situ synthesis;
the thickness of the coating is 200-500 microns;
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 30-40 KW, and the distance between the spray guns is 80-120 mm. The powder feeding gas is argon;
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 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 multi-element ceramic composite coating relates to raw materials which are commercially available, and the sand blasting process, the sand paper sanding process and the bonding layer spraying process are well known in the prior art.
According to the preparation method of the multi-element ceramic composite coating, when the oxide is any one of zirconium oxide, titanium oxide, hafnium oxide, tantalum oxide, niobium oxide, vanadium oxide, chromium oxide, molybdenum oxide or tungsten oxide, the prepared coating is mainly composed of carbide and silicide phases, wherein the carbide and the silicide are formed by in-situ reaction, each phase interface is pure, the interphase combination is tight, and the coating has high cohesive strength; the silicide formed in situ in the coating can not only improve the high-temperature resistance and the oxidation resistance of the coating, but also enable the coating to obtain the crack self-healing capability; when the raw material oxide powder is two or more oxides and is used simultaneously, carbides generated in situ in the prepared coating are solid-dissolved, the coating has high cohesive strength, and the hardness, the wear resistance, the corrosion resistance and the high-temperature resistance and the oxidation resistance of the coating are further improved.
The prominent substantive features of the invention are:
in the prior art, if a coating material with one component is prepared, the material with the one component is selected as a raw material for thermal spraying (or called spraying feed), for example, zirconium carbide, zirconium silicide and alumina powder are selected as spraying raw materials for obtaining a zirconium carbide-zirconium silicide-alumina composite coating; however, the carbide ceramic phase (with high melting point) has the characteristic of being refractory in the conventional spraying and the reason that the carbide and silicide can be oxidized in the spraying process, so that the preparation of the multi-ceramic composite coating by directly spraying the composite powder consisting of the carbide, the silicide and the aluminum oxide has difficulty.
The thermal spraying in-situ reaction of the invention adopts relatively cheap raw materials (such as the zirconium oxide, the silicon carbide and the aluminum of the invention), and utilizes the reaction of oxides (zirconium oxide, titanium oxide, hafnium oxide, tantalum oxide, niobium oxide, vanadium oxide, chromium oxide, molybdenum oxide or tungsten oxide), silicon carbide and aluminum under the high-temperature condition of thermal spraying flame flow to finally generate the multi-ceramic composite coating with main phases of carbide, silicide and aluminum oxide (such as zirconium carbide, zirconium silicide and aluminum oxide).
The invention has the following beneficial effects:
(1) the invention adopts the composite powder composed of thermal spraying oxide (zirconium oxide, titanium oxide, hafnium oxide, tantalum oxide, niobium oxide, vanadium oxide, chromium oxide, molybdenum oxide or tungsten oxide), silicon carbide and aluminum to react in situ to synthesize the multi-element ceramic composite coating, the selected raw material powder has rich resources and low price, and the thermal spraying technical process is adopted to prepare the multi-element ceramic composite coating by one-step forming, the preparation process is simple, the cost is low, and a novel method for preparing the multi-element ceramic composite coating is provided.
(2) The multi-element ceramic composite coating prepared by the method overcomes the defects that carbide and silicide particles are isolated from each other and are not bonded in a loose state, and each phase, namely the carbide, the silicide and the aluminum oxide, in the prepared multi-element ceramic composite coating is formed by in-situ reaction, the interface of each phase is pure, and the interphase bonding is tight; when two or more oxides are used as raw materials, carbides generated in situ in the prepared coating are solid-dissolved, and the coating has high cohesive strength.
(3) The multi-element ceramic composite coating prepared by the method has uniform components, wider element proportion adjusting space, high density, hardness, wear resistance, corrosion resistance and high temperature resistance and oxidation resistance; the existence of the silicide in the coating can not only improve the high-temperature resistance and the oxidation resistance of the coating, but also ensure that the coating can obtain the crack self-healing capability; when two or more than two oxides are used as raw materials, carbides generated in situ in the prepared coating are subjected to solid solution, so that the solid solution strengthening effect can be achieved, and the hardness, the wear resistance, the corrosion resistance and the high-temperature resistance and the oxidation resistance of the coating are further improved; the binary or multi-element solid solution phase can play a role in solid solution strengthening, so that the hardness, wear resistance, corrosion resistance and high-temperature resistance and oxidation resistance of the coating are further improved; the defects of complex process, high cost, large energy consumption, large pollution, low efficiency, low coating thickness, low coating density and poor coating performance of the multi-element ceramic composite coating prepared by the prior art are overcome.
(4) In order to obtain the multi-element ceramic composite coating with excellent performance, a raw material system is optimized, and after years of intensive research and hundreds of repeated experiments, the inventor group successfully adopts the method to prepare the multi-element ceramic composite coating.
Compared with the oxidation resistance and the ablation resistance of boride and carbide coatings prepared by the same process, the oxidation resistance (1000 ℃, 24 hours, mass weight gain percentage) of the multi-element ceramic composite coating prepared by the invention is improved by 40% at most compared with the oxidation resistance of coatings prepared by hot spraying zirconium carbide powder, zirconium boride-zirconium carbide composite powder, titanium carbide powder, zirconium/boron carbide composite powder and zirconium oxide/boron carbide/aluminum composite powder; the multi-element ceramic composite coating prepared by the invention has ablation resistance (heat flux of 4.02 MW/m) compared with coatings obtained by thermally spraying zirconium carbide powder, zirconium boride-zirconium carbide composite powder, titanium carbide powder, zirconium/boron carbide composite powder and zirconium oxide/boron carbide/aluminum composite powder240s mass ablation rate,%) increased by 6.68% at most.
Drawings
The invention is further illustrated with reference to the following figures and examples.
FIG. 1 is an XRD pattern of a multi-component ceramic composite coating (titanium carbide-titanium silicide-alumina composite coating) prepared in example 4.
FIG. 2 is an SEM photograph of the multi-component ceramic composite coating (titanium carbide-titanium silicide-alumina composite coating) obtained in example 4.
FIG. 3 is an XRD pattern of the multi-component ceramic composite coating (chrome carbide-chrome silicide-alumina composite coating) prepared in example 8.
FIG. 4 is an SEM photograph of the multi-component ceramic composite coating (chromium carbide-chromium silicide-alumina composite coating) obtained in example 8.
FIG. 5 is an XRD pattern of the multi-component ceramic composite coating (niobium carbide-niobium silicide-aluminum oxide composite coating) obtained in example 11.
FIG. 6 is an SEM photograph of a multi-component ceramic composite coating (niobium carbide-niobium silicide-aluminum oxide composite coating) prepared in example 11.
Detailed Description
Example 1
The first step, preparing zirconia/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing zirconia powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the silicon carbide powder accounts for 5% by mass of the total mass of the zirconia powder, the silicon carbide powder and the aluminum powder, the aluminum powder and the zirconia powder account for 95% by mass of the total mass of the zirconia powder, the silicon carbide powder and the aluminum powder, the mass ratio of the zirconia powder to the aluminum powder is 60: 40, and uniformly mixing a binder (methyl cellulose, the same as in examples 2-10) into the composite powder, wherein the weight ratio of the composite powder to the binder is 100: 0.1, so as to prepare the zirconia/silicon carbide/aluminum composite powder for thermal spraying;
secondly, preprocessing a base material:
the base material is Inconel 718 nickel-based high-temperature alloy, the pretreatment mode is sand blasting, and then a NiAl bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the nickel-based high-temperature alloy base material after the sand blasting;
step three, preparing the multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.36m3The arc power is 30KW, the distance of the spray gun is 80mm, and the powder feeding gas is argon (the same as the embodiment below); and spraying the zirconium oxide/silicon carbide/aluminum 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 multi-element ceramic composite coating with the thickness of 200 microns.
Example 2
The first step, preparing zirconia/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing zirconia powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the mass percent of the silicon carbide powder to the total mass of the zirconia powder, the silicon carbide powder and the aluminum powder is 10%, the mass percent of the aluminum powder and the zirconia powder to the total mass of the zirconia powder, the silicon carbide powder and the aluminum powder is 90%, the mass ratio of the zirconia powder to the aluminum powder is 85: 15, and uniformly mixing into a binder, wherein the weight ratio of the binder to the composite powder to the binder is 100: 1, so that the zirconia/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is TC4 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 TC4 titanium alloy base material after the sand blasting;
step three, preparing the multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.4m3And h, the electric arc power is 35KW, the distance between spray guns is 100mm, and the zirconium oxide/silicon carbide/aluminum composite powder for thermal spraying prepared in the first step is sprayed on the surface of the TC4 titanium alloy base material pretreated in the second step, so that the multi-ceramic composite coating with the thickness of 200 microns is formed.
Example 3
The first step, preparing zirconia/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing zirconia powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the silicon carbide powder accounts for 30% by mass of the total mass of the zirconia powder, the silicon carbide powder and the aluminum powder, the aluminum powder and the zirconia powder account for 70% by mass of the total mass of the zirconia powder, the silicon carbide powder and the aluminum powder, the mass ratio of the zirconia powder to the aluminum powder is 90: 10, and uniformly mixing the mixture into a binder, wherein the weight ratio of the binder to the composite powder is 100: 2, so that the zirconia/silicon carbide/aluminum 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;
step three, preparing the multi-element ceramic composite coating:
by adopting a plasma spraying method, the flow rate 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/silicon carbide/aluminum 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 multi-ceramic composite coating with the thickness of 200 microns is formed.
Example 4
The first step, preparing titanium oxide/silicon carbide/aluminum composite powder for thermal spraying:
titanium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns are uniformly mixed into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the titanium oxide powder, the silicon carbide powder and the aluminum powder is 5 percent, the mass percentage of the aluminum powder and the titanium oxide powder to the total mass of the titanium oxide powder, the silicon carbide powder and the aluminum powder is 95 percent, the mass ratio of the titanium oxide powder to the aluminum powder is 60: 40, and then a binder is uniformly mixed, wherein the use amount of the binder is that the weight ratio of the composite powder to the binder is 100: 0.1, so that the titanium oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is Inconel 718 nickel-based high-temperature alloy, the pretreatment mode is sand blasting, and then a NiAl bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the nickel-based high-temperature alloy base material after the sand blasting;
step three, preparing the multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.5m3And h, the electric arc power is 32KW, the distance of a spray gun is 100mm, and the titanium oxide/silicon carbide/aluminum 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 multi-ceramic composite coating with the thickness of 200 microns is formed.
Fig. 1 is an XRD pattern of the multi-component ceramic composite coating prepared in this example, from which it can be seen that the multi-component ceramic composite coating is mainly composed of titanium carbide, titanium silicide and alumina phases, and secondly a silicon carbide phase exists. It can be seen that the multi-element ceramic composite coating mainly comprising titanium carbide, titanium silicide and aluminum oxide can be successfully prepared by using the titanium oxide/silicon carbide/aluminum composite powder as a raw material and adopting a plasma spraying method.
Fig. 2 is an SEM image of the multi-ceramic composite coating prepared in this example. It can be seen that the thickness of the multi-element ceramic composite coating reaches more than 200 microns, the coating density is high, and the coating is well combined with a matrix.
Example 5
The first step, preparing titanium oxide/silicon carbide/aluminum composite powder for thermal spraying:
titanium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns are uniformly mixed into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the titanium oxide powder, the silicon carbide powder and the aluminum powder is 10%, the mass percentage of the aluminum powder and the titanium oxide powder to the total mass of the titanium oxide powder, the silicon carbide powder and the aluminum powder is 90%, the mass ratio of the titanium oxide powder to the aluminum powder is 85: 15, and then the titanium oxide powder, the silicon carbide powder and the aluminum powder are uniformly mixed into a binder, wherein the weight ratio of the composite powder to the binder is 100: 1, so that the titanium oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is 1Cr18Ni9Ti steel, 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 1Cr18Ni9Ti steel base material after the sand blasting;
step three, preparing the multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.5m3And h, the electric arc power is 36KW, the distance between spray guns is 110mm, and the titanium oxide/silicon carbide/aluminum composite powder for thermal spraying prepared in the first step is sprayed on the surface of the 1Cr18Ni9Ti steel substrate material pretreated in the second step, so that the multi-element ceramic composite coating with the thickness of 200 microns is formed.
Example 6
The first step, preparing titanium oxide/silicon carbide/aluminum composite powder for thermal spraying:
titanium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns are uniformly mixed into composite powder, wherein the silicon carbide powder accounts for 30% of the total mass of the titanium oxide powder, the silicon carbide powder and the aluminum powder, the aluminum powder and the titanium oxide powder account for 70% of the total mass of the titanium oxide powder, the silicon carbide powder and the aluminum powder, the mass ratio of the titanium oxide powder to the aluminum powder is 90: 10, and then the titanium oxide powder, the silicon carbide powder and the aluminum powder are uniformly mixed into a binder, the weight ratio of the composite powder to the binder is 100: 2, so that the titanium oxide/silicon carbide/aluminum 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;
step three, preparing the multi-element ceramic composite coating:
by adopting a plasma spraying method, the flow rate of the powder feeding gas is 0.6m3And h, the electric arc power is 40KW, the distance between spray guns is 120mm, and the titanium oxide/silicon carbide/aluminum 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 multi-ceramic composite coating with the thickness of 200 microns is formed.
Example 7
The first step, preparing the chromium oxide/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing chromium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the silicon carbide powder accounts for 5 mass percent of the total mass of the chromium oxide powder, the silicon carbide powder and the aluminum powder, the aluminum powder and the chromium oxide powder account for 95 mass percent of the total mass of the chromium oxide powder, the silicon carbide powder and the aluminum powder, the mass ratio of the chromium oxide powder to the aluminum powder is 60: 40, and uniformly mixing the mixture into a binder, wherein the weight ratio of the binder to the composite powder is 100: 0.1, so that the chromium oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is Inconel 718 nickel-based high-temperature alloy, the pretreatment mode is sand blasting, and then a NiAl bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the nickel-based high-temperature alloy base material after the sand blasting;
step three, preparing the multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.4m3And h, the electric arc power is 33KW, the distance between spray guns is 90mm, and the chromium oxide/silicon carbide/aluminum 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 multi-ceramic composite coating with the thickness of 200 microns is formed.
Example 8
The first step, preparing the chromium oxide/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing chromium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the silicon carbide powder accounts for 20 mass percent of the total mass of the chromium oxide powder, the silicon carbide powder and the aluminum powder, the aluminum powder and the chromium oxide powder account for 80 mass percent of the total mass of the chromium oxide powder, the silicon carbide powder and the aluminum powder, the mass ratio of the chromium oxide powder to the aluminum powder is 78: 22, and uniformly mixing the mixture into a binder, wherein the weight ratio of the binder to the composite powder is 100: 1, so that the chromium oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is TC4 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 multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.5m3H, arc power is 38KW, spray gun distance is 110, the chromium oxide/silicon carbide/aluminum composite powder prepared in the first step for thermal spraying is sprayed on the second stepAnd (3) forming a multi-element ceramic composite coating with the thickness of 200 microns on the surface of the pretreated titanium alloy base material.
Fig. 3 is an XRD pattern of the multi-component ceramic composite coating prepared in this example, from which it can be seen that the multi-component ceramic composite coating is mainly composed of phases of chromium carbide, chromium silicide and alumina, and secondly, phases of chromium oxide and silicon carbide exist. Therefore, the multi-element ceramic composite coating with the main components of chromium carbide, chromium silicide and aluminum oxide can be successfully prepared by using the chromium oxide/silicon carbide/aluminum composite powder as the raw material and adopting a plasma spraying method.
Fig. 4 is an SEM image of the multi-ceramic composite coating prepared in this example. It can be seen that the thickness of the multi-element ceramic composite coating reaches more than 200 microns, the coating density is high, and the coating is well combined with a matrix.
Example 9
The first step, preparing the chromium oxide/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing chromium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the silicon carbide powder accounts for 30% by mass of the total mass of the chromium oxide powder, the silicon carbide powder and the aluminum powder, the aluminum powder and the chromium oxide powder account for 70% by mass of the total mass of the chromium oxide powder, the silicon carbide powder and the aluminum powder, the mass ratio of the chromium oxide powder to the aluminum powder is 90: 10, and uniformly mixing the mixture into a binder, wherein the weight ratio of the binder to the composite powder is 100: 2, so that the chromium oxide/silicon carbide/aluminum 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;
step three, preparing the multi-element ceramic composite coating:
by adopting a plasma spraying method, the flow rate of the powder feeding gas is 0.6m3H, arc power is 40KW, spray gun distance is 120mm, will go upAnd spraying the chromium oxide/silicon carbide/aluminum composite powder prepared in the first step for thermal spraying on the surface of the graphite base material pretreated in the second step to form a multi-element ceramic composite coating with the thickness of 200 microns.
Example 10
First, preparing niobium oxide/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing niobium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the niobium oxide powder, the silicon carbide powder and the aluminum powder is 5%, the mass percentage of the aluminum powder and the niobium oxide powder to the total mass of the niobium oxide powder, the silicon carbide powder and the aluminum powder is 95%, the mass ratio of the niobium oxide powder to the aluminum powder is 60: 40, and uniformly mixing the mixture into a binder, wherein the use amount of the binder is that the weight ratio of the composite powder to the binder is 100: 0.1, so that the niobium oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is Inconel 718 nickel-based high-temperature alloy, the pretreatment mode is sand blasting, and then a NiAl bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the nickel-based high-temperature alloy base material after the sand blasting;
step three, preparing the multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.6m3And h, the electric arc power is 40KW, the distance between spray guns is 120mm, and the niobium oxide/silicon carbide/aluminum 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 multi-ceramic composite coating with the thickness of 200 microns is formed.
Example 11
First, preparing niobium oxide/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing niobium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the niobium oxide powder, the silicon carbide powder and the aluminum powder is 13%, the mass percentage of the aluminum powder and the niobium oxide powder to the total mass of the niobium oxide powder, the silicon carbide powder and the aluminum powder is 87%, the mass ratio of the niobium oxide powder to the aluminum powder is 75: 25, and uniformly mixing the mixture into a binder (polyvinyl alcohol, the same as the following embodiment), wherein the weight ratio of the binder to the composite powder is 100: 1, so that the niobium oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is TC4 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 multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.5m3And h, the electric arc power is 37KW, the distance between spray guns is 110mm, and the niobium oxide/silicon carbide/aluminum 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 a multi-ceramic composite coating with the thickness of 200 microns is formed.
Fig. 5 is an XRD pattern of the multi-component ceramic composite coating obtained in this example, from which it can be seen that the multi-component ceramic composite coating is mainly composed of niobium carbide, niobium silicide and alumina phases, and secondly niobium oxide and silicon carbide phases exist. It can be seen that the multi-element ceramic composite coating mainly comprising niobium carbide, niobium silicide and aluminum oxide can be successfully prepared by using the niobium oxide/silicon carbide/aluminum composite powder as a raw material and adopting a plasma spraying method.
Fig. 6 is an SEM image of the multi-ceramic composite coating layer prepared in this example. It can be seen that the thickness of the multi-element ceramic composite coating reaches more than 200 microns, the coating density is high, and the coating is well combined with a matrix.
Example 12
First, preparing niobium oxide/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing niobium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the niobium oxide powder, the silicon carbide powder and the aluminum powder is 30%, the mass percentage of the aluminum powder and the niobium oxide powder to the total mass of the niobium oxide powder, the silicon carbide powder and the aluminum powder is 70%, the mass ratio of the niobium oxide powder to the aluminum powder is 90: 10, and uniformly mixing the mixture into a binder, wherein the weight ratio of the binder to the composite powder to the binder is 100: 2, so that the niobium oxide/silicon carbide/aluminum 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;
step three, preparing the multi-element ceramic composite coating:
by adopting a plasma spraying method, the flow rate of the powder feeding gas is 0.3m3And h, the electric arc power is 30KW, the distance between spray guns is 80mm, and the niobium oxide/silicon carbide/aluminum 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 multi-element ceramic composite coating with the thickness of 200 microns is formed.
Example 13
The first step, preparing hafnium oxide/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing hafnium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the three raw materials of the hafnium oxide powder, the silicon carbide powder and the aluminum powder is 5%, the mass percentage of the aluminum powder and the hafnium oxide powder to the total mass of the three raw materials of the hafnium oxide powder, the silicon carbide powder and the aluminum powder is 95%, the mass ratio of the hafnium oxide powder to the aluminum powder is 60: 40, and uniformly mixing the mixture into a binder, wherein the use amount of the binder is that the weight ratio of the composite powder to the binder is 100: 0.1, so that the hafnium oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is Inconel 718 nickel-based high-temperature alloy, the pretreatment mode is sand blasting, and then a NiAl bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the nickel-based high-temperature alloy base material after the sand blasting;
step three, preparing the multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.6m3And h, the electric arc power is 40KW, the distance between spray guns is 120mm, and the hafnium oxide/silicon carbide/aluminum 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 multi-ceramic composite coating is formed. The thickness of the prepared multi-element ceramic composite coating reaches 200 microns, the coating density is high, and the coating and a matrix are well combined.
Example 14
The first step, preparing hafnium oxide/silicon carbide/aluminum composite powder for thermal spraying:
evenly mixing hafnium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the three raw materials of the hafnium oxide powder, the silicon carbide powder and the aluminum powder is 20%, the mass percentage of the aluminum powder and the hafnium oxide powder to the total mass of the three raw materials of the hafnium oxide powder, the silicon carbide powder and the aluminum powder is 80%, the mass ratio of the hafnium oxide powder to the aluminum powder is 75: 25, and then evenly mixing into a binder, wherein the use amount of the binder is that the weight ratio of the composite powder to the binder is 100: 1, so that the hafnium oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is TC4 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 multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.3m3And h, the electric arc power is 30KW, the distance between spray guns is 80mm, and the hafnium oxide/silicon carbide/aluminum 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 multi-ceramic composite coating is formed. The thickness of the prepared multi-element ceramic composite coating reaches 200 microns, the coating density is high, and the coating and a matrix are well combined.
Example 15
The first step, preparing hafnium oxide/silicon carbide/aluminum composite powder for thermal spraying:
evenly mixing hafnium oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the three raw materials of the hafnium oxide powder, the silicon carbide powder and the aluminum powder is 30%, the mass percentage of the aluminum powder and the hafnium oxide powder to the total mass of the three raw materials of the hafnium oxide powder, the silicon carbide powder and the aluminum powder is 70%, the mass ratio of the hafnium oxide powder to the aluminum powder is 90: 10, and then evenly mixing into a binder, wherein the use amount of the binder is that the weight ratio of the composite powder to the binder is 100: 2, so that the hafnium oxide/silicon carbide/aluminum 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;
step three, preparing the multi-element ceramic composite coating:
by adopting a plasma spraying method, the flow rate of the powder feeding gas is 0.4m3And h, the electric arc power is 34KW, the distance between spray guns is 90mm, and the hafnium oxide/silicon carbide/aluminum 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 multi-ceramic composite coating with the thickness of 200 microns is formed.
Example 16
Firstly, preparing tantalum oxide/silicon carbide/aluminum composite powder for thermal spraying:
tantalum oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns are uniformly mixed into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the tantalum oxide powder, the silicon carbide powder and the aluminum powder is 5%, the mass percentage of the aluminum powder and the tantalum oxide powder to the total mass of the tantalum oxide powder, the silicon carbide powder and the aluminum powder is 95%, the mass ratio of the tantalum oxide powder to the aluminum powder is 60: 40, and then the composite powder is uniformly mixed with a binder, wherein the use amount of the binder is that the weight ratio of the composite powder to the binder is 100: 0.1, so that the tantalum oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is Inconel 718 nickel-based high-temperature alloy, the pretreatment mode is sand blasting, and then a NiAl bonding bottom layer with the thickness of 50 microns is sprayed on the surface of the nickel-based high-temperature alloy base material after the sand blasting;
step three, preparing the multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.5m3And h, the electric arc power is 33KW, the distance between spray guns is 110mm, and the tantalum oxide/silicon carbide/aluminum 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 multi-ceramic composite coating is formed. The thickness of the prepared multi-element ceramic composite coating reaches 200 microns, the coating density is high, and the coating and a matrix are well combined.
Example 17
Firstly, preparing tantalum oxide/silicon carbide/aluminum composite powder for thermal spraying:
tantalum oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns are uniformly mixed into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the tantalum oxide powder, the silicon carbide powder and the aluminum powder is 20%, the mass percentage of the aluminum powder and the tantalum oxide powder to the total mass of the tantalum oxide powder, the silicon carbide powder and the aluminum powder is 80%, the mass ratio of the tantalum oxide powder to the aluminum powder is 75: 25, and then the mixture is uniformly mixed into a binder, the use amount of the binder is that the weight ratio of the composite powder to the binder is 100: 1, so that the tantalum oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is TC4 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 multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.5m3And h, the electric arc power is 38KW, the distance between spray guns is 120mm, and the tantalum oxide/silicon carbide/aluminum 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 multi-ceramic composite coating is formed. The thickness of the prepared multi-element ceramic composite coating reaches 200 microns, the coating density is high, and the coating and a matrix are well combined.
Example 18
Firstly, preparing tantalum oxide/silicon carbide/aluminum composite powder for thermal spraying:
tantalum oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns are uniformly mixed into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the tantalum oxide powder, the silicon carbide powder and the aluminum powder is 30%, the mass percentage of the aluminum powder and the tantalum oxide powder to the total mass of the tantalum oxide powder, the silicon carbide powder and the aluminum powder is 70%, the mass ratio of the tantalum oxide powder to the aluminum powder is 90: 10, and then a binder is uniformly mixed, the use amount of the binder is that the weight ratio of the composite powder to the binder is 100: 2, so that the tantalum oxide/silicon carbide/aluminum 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;
step three, preparing the multi-element ceramic composite coating:
by adopting a plasma spraying method, the flow rate of the powder feeding gas is 0.5m3And h, the electric arc power is 40KW, the distance between spray guns is 120mm, and the tantalum oxide/silicon carbide/aluminum 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 multi-ceramic composite coating with the thickness of 200 microns is formed.
Example 19
First step, preparing oxide/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the silicon carbide powder accounts for 5% by mass of the total mass of all the raw material powders, the aluminum powder and the oxide powder account for 95% by mass of the total mass of all the raw material powders, and the mass ratio between the oxide powder and the aluminum powder is 60: 40, wherein the oxide comprises niobium oxide, titanium oxide, chromium oxide and zirconium oxide, each of which accounts for 25%, and uniformly mixing the mixture into a binder, wherein the weight ratio of the binder to the composite powder is 100: 0.1, so as to prepare the oxide/silicon carbide/aluminum 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 multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.3m3And h, the electric arc power is 30KW, the distance between spray guns is 80mm, and the oxide/silicon carbide/aluminum 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 multi-ceramic composite coating with the thickness of 200 microns is formed.
Example 20
First step, preparing oxide/silicon carbide/aluminum composite powder for thermal spraying:
uniformly mixing oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the silicon carbide powder accounts for 13% of the total mass of all the raw material powders, the aluminum powder and the oxide powder account for 87% of the total mass of all the raw material powders, and the mass ratio between the oxide powder and the aluminum powder is 75: 25, wherein the oxide comprises niobium oxide, titanium oxide, chromium oxide and zirconium oxide, each of which accounts for 25%, and uniformly mixing the mixture into a binder, wherein the weight ratio of the binder to the composite powder is 100: 1, so that the oxide/silicon carbide/aluminum composite powder for thermal spraying is prepared;
secondly, preprocessing a base material:
the base material is TC4 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 multi-element ceramic composite coating:
the air plasma spraying method is adopted, and the flow rate of the powder feeding gas is 0.6m3H, arc power of 40KW, spray gun distance of 120mm, spraying the oxide/silicon carbide/aluminum composite powder prepared in the first step for thermal spraying on the surface of the titanium alloy base material pretreated in the second step, thereby forming a multi-element ceramic composite coating with the thickness of 200 microns.
Example 21
The first step, preparing the complex oxide/silicon carbide/aluminum composite powder for thermal spraying: uniformly mixing multi-component oxide powder with the particle size range of 0.001-10 microns, silicon carbide powder with the particle size range of 0.001-10 microns and aluminum powder with the particle size range of 0.1-10 microns into composite powder, wherein the mass percentage of the silicon carbide powder to the total mass of the three raw material powders of the multi-component oxide powder, the carbide powder and the aluminum powder is 15%, the mass percentage of the aluminum powder and the multi-component oxide powder to the total mass of the three raw material powders of the multi-component oxide powder, the silicon carbide powder and the aluminum powder is 85%, the mass ratio of the multi-component oxide powder to the aluminum powder is 68: 32, and the oxide powder is ZrO2、TiO2、Nb2O5And V2O5The mass ratio of the powder to the multi-component oxide powder is 25:25:25: 25; uniformly mixing the powder and the binder in a weight ratio of 100: 0.1 to prepare the multi-element oxide/silicon carbide/aluminum composite powder for thermal spraying;
secondly, preprocessing the surface of the base material:
the base material is 1Cr18Ni9Ti steel, 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 1Cr18Ni9Ti steel base material after the sand blasting;
thirdly, preparing the high-entropy ceramic-alumina composite coating:
and spraying the multi-element composite powder for thermal spraying prepared in the first step on the surface of the 1Cr18Ni9Ti steel matrix material pretreated in the second step by adopting a thermal spraying method, so as to synthesize the multi-element ceramic composite coating with the thickness of 300 microns in situ.
The preparation method of the multi-element ceramic composite coating adopts the thermal spraying method, and the technological parameters are as follows:the flow of the powder feeding gas is 0.5m3The arc power was 35kW and the lance distance was 110 mm.
In the above examples, the raw materials are commercially available, and the sand blasting process, the sand sanding process, and the process of spraying the bonding layer are well known in the art.
Compared with the oxidation resistance and the ablation resistance of boride and carbide coatings prepared by the same process, the oxidation resistance (1000 ℃, 24h, mass weight gain percent) of coatings obtained by thermally spraying zirconium carbide powder, zirconium boride-zirconium carbide composite powder, titanium carbide powder, zirconium/boron carbide composite powder and zirconium oxide/boron carbide/aluminum composite powder is 58, 56, 47, 65, 38 and 36 respectively, while the oxidation resistance of coatings of example 4 (titanium carbide-titanium silicide-aluminum oxide composite coating), example 8 (chromium carbide-chromium silicide-aluminum oxide composite coating) and example 11 (niobium carbide-niobium silicide-aluminum oxide composite coating) is 30, 25 and 31 respectively; ablation resistance (heat flux 4.02 MW/m) of coatings obtained by thermal spraying of zirconium carbide powder, zirconium boride-zirconium carbide composite powder, titanium carbide powder, zirconium/boron carbide composite powder and zirconium oxide/boron carbide/aluminum composite powder240s mass ablation (%) was 8.16, 7.81, 6.33, 10.15, 4.99 and 4.74, while the coatings of example 4 of the present invention (titanium carbide-titanium silicide-alumina composite coating), example 8 (chromium carbide-chromium silicide-alumina composite coating) and example 11 (niobium carbide-niobium silicide-alumina composite coating) had ablation resistances of 3.59, 3.47 and 3.62, respectively. It can be seen that the multi-element ceramic composite coating prepared by the method has more excellent performances (including oxidation resistance and ablation resistance) than the corresponding boride and carbide coatings.
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; zirconium carbide powder is sprayed on the surface of the pretreated TC4 titanium alloy base material, and the parameters of the thermal spraying process are as follows: the flow of the powder feeding gas is 0.3m3H, electricityThe arc power is 35KW, the distance of the spray gun is 100mm, and the powder feeding gas is argon; thereby synthesizing a zirconium carbide coating having a thickness of 300 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; zirconium boride powder is sprayed on the surface of the pretreated TC4 titanium alloy base material, and 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; thus synthesizing a zirconium boride coating having a thickness of 300 microns.
Comparative example 3
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; zirconium boride-zirconium carbide powder is sprayed on the surface of the pretreated TC4 titanium alloy base material, and 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 a zirconium boride-zirconium carbide coating having a thickness of 300 μm.
Comparative example 4
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; titanium carbide powder is sprayed on the surface of the pretreated TC4 titanium alloy base material, and 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 a titanium carbide coating having a thickness of 300 microns.
Comparative example 5
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, and performing thermal spraying process parametersThe method comprises the following steps: 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 300 microns.
Comparative example 6
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 300 microns.
The invention is not the best known technology.

Claims (5)

1. A preparation method of a multi-element ceramic composite coating is characterized by comprising the following steps:
first step, preparing oxide/silicon carbide/aluminum composite powder for thermal spraying:
mixing oxide powder, silicon carbide powder and aluminum powder into composite powder, and then mixing the composite powder with a binder to prepare oxide/silicon carbide/aluminum composite powder for thermal spraying;
wherein the silicon carbide powder accounts for 5-30% of the composite powder by mass, and the mass ratio of the oxide powder to the aluminum powder is 60-90: 10-40; the binder is used in a weight ratio of 100: 0.1-2, the oxide is any x of zirconium oxide, titanium oxide, hafnium oxide, tantalum oxide, niobium oxide, vanadium oxide, chromium oxide, molybdenum oxide or tungsten oxide, and x is 1,2,3 or 4;
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, performing sand blasting treatment, and then spraying a bonding layer on the surface of the metal base material subjected to the sand blasting treatment;
or, 2) when the base material is an inorganic non-metallic material base, adopting sand blasting or sand paper polishing treatment;
step three, preparing the multi-element ceramic composite coating:
spraying the oxide/silicon carbide/aluminum composite powder for thermal spraying prepared in the first step on the surface of the pretreated substrate material in the second step by adopting a thermal spraying method, so as to obtain a multi-element ceramic 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 30-40 KW, and the distance between spray guns is 80-120 mm;
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 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.
2. The method for preparing the multi-element ceramic composite coating according to claim 1, wherein the particle sizes of the oxide powder and the silicon carbide powder are 0.001-10 microns; the granularity of the aluminum powder is 0.1-10 microns.
3. The method of claim 1, wherein the thickness of the coating layer in the third step is 200-500 μm.
4. The method of claim 1, wherein the powder-feeding gas is argon gas.
5. The method of claim 1, wherein the bonding layer material is: NiAl, NiCrAl, FeAl, NiCrAlY, CoCrAlY, CoNiCrAlY, NiCoCrAlYTa or NiCrBSi.
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