CN113862598A - CMAS-resistant protective layer for TBCs or EBCs, preparation method thereof and protective structure obtained by CMAS-resistant protective layer - Google Patents
CMAS-resistant protective layer for TBCs or EBCs, preparation method thereof and protective structure obtained by CMAS-resistant protective layer Download PDFInfo
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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
- C23C4/04—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
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/009—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone characterised by the material treated
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/45—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements
- C04B41/52—Multiple coating or impregnating multiple coating or impregnating with the same composition or with compositions only differing in the concentration of the constituents, is classified as single coating or impregnation
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/80—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone of only ceramics
- C04B41/81—Coating or impregnation
- C04B41/89—Coating or impregnation for obtaining at least two superposed coatings having different compositions
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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
- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
- C23C14/08—Oxides
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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
- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
- C23C14/08—Oxides
- C23C14/083—Oxides of refractory metals or yttrium
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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
- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
- C23C14/14—Metallic material, boron or silicon
- C23C14/16—Metallic material, boron or silicon on metallic substrates or on substrates of boron or silicon
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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
- C23C4/04—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
- C23C4/11—Oxides
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- 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
- C23C4/129—Flame spraying
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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
- C23C4/134—Plasma spraying
Abstract
The invention relates to a CMAS-resistant protective coating for TBCs or EBCs, which is a rare earth aluminate compound Re4Al2O9Re is any one or two of Gd, Tb, Dy and Yb, the thickness of the anti-CMAS protective layer is 10-100 mu m, and the porosity of the anti-CMAS protective layer is 0.5-20%. The invention also relates toThe preparation method of the CMAS-resistant protective layer comprises the step of preparing the CMAS-resistant protective layer on the surfaces of TBCs or EBCs by using APS, PS-PVD or SPS. The invention further relates to a protective structure comprising a matrix layer, TBCs or EBCs and the above-mentioned anti-CMAS protective layer. According to the CMAS-resistant protective layer disclosed by the invention, the penetration of molten CMAS can be rapidly blocked within the working temperature range of 1200-1650 ℃, and the ultrahigh-temperature service stability and the thermal cycle life of the thermal barrier coating in the CMAS environment are improved.
Description
Technical Field
The present invention relates to high temperature resistant coatings, and more particularly to a CMAS resistant armor layer for TBCs or EBCs, a method of making the same, and protective structures made therefrom.
Background
Advanced aerospace, ships and energy power equipment put higher requirements on the working temperature, service life and comprehensive performance of two-machine high-temperature hot end components. At present, the turbine inlet temperature of the most advanced aviation engines around the world already exceeds 1800 ℃ and the turbine inlet temperature of heavy duty gas turbines approaches 1700 ℃. Nickel-cobalt-based superalloys are common structural materials for two-machine hot end parts, however, the operating temperature of the most advanced nickel-based single crystal superalloys is approximately 1120 ℃, which is close to its service temperature limit. Therefore, the development of advanced Thermal Barrier Coatings (TBCs) on the surface of the superalloy and the gradual adoption of Ceramic Matrix Composites (CMCs) instead of the superalloy in the high-temperature hot-end structural components of the two machines have become necessary approaches for developing two machines with high turbine inlet temperature, high fuel efficiency, low pollution emission, long service life and high performance.
The CMCs can be safely used at 1650 ℃ for a long time, but the degradation failure of the CMCs structural components can be accelerated by the water vapor and oxygen environment. Therefore, the development of advanced Environmental Barrier Coatings (EBCs) on the surfaces of CMCs is a necessary measure for solving the problem of long-time safe service at high temperature in the water-oxygen environment.
When the working temperature of TBCs or EBCs on the surfaces of the two-machine high-temperature hot-end components exceeds 1230 ℃ (the service temperature of the surfaces of the EBCs is up to 1482-1650 ℃), solid particles (the main chemical component is CaO-MgO-Al) such as volcanic ash, solid sand dust, ash and the like sucked from the air2O3-SiO2CMAS) will melt to form liquid CMAS adhering to the TBCs or EBCs surfaces. The liquid CMAS can locally dissolve the TBCs or EBCs and chemically react, chemically degrading and gradually destroying the original microstructure and thermo-mechanical properties of the TBCs and EBCs leading to spallation failure. On the other hand, during the cooling process of the two-machine thermal shock cycle, the residual liquid CMAS forms a glass phase after the reaction of penetrating into TBCs or EBCs through pores or cracks. The mismatch of the thermomechanical properties of the CMAS glass and the coating results in large internal residual stress, which aggravates the failure process of TBCs and EBCs under high-temperature and ultrahigh-temperature service heat-force-chemical interaction. Therefore, the development of a new material and a method for solving the corrosion degradation of 1230-grade TBCs and EBCs under the action of CMAS and the improvement of the high-temperature, ultrahigh-temperature and long-life service performance of two machines become a bottleneck problem to be solved urgently in advanced aerospace, ship and energy power equipment.
Disclosure of Invention
In order to solve the problems of corrosion degradation and the like of TBCs or EBCs at high temperature under the action of CMAS in the prior art, the invention provides a CMAS-resistant protective layer for TBCs or EBCs, a preparation method thereof and a protective structure obtained by the CMAS-resistant protective layer.
The CMAS-resistant protective layer for TBCs or EBCs according to the invention is a rare earth aluminate compound Re4Al2O9(ReMA), Re is any one or two of Gd, Tb, Dy and Yb, the thickness of the anti-CMAS protective layer is 10-100 mu m, and the porosity of the anti-CMAS protective layer is 0.5-20%.
Preferably, the thickness of the anti-CMAS protective layer is from 50 μm to 100 μm.
The preparation method of the CMAS-resistant protective layer comprises the steps of preparing the CMAS-resistant protective layer on the surfaces of TBCs or EBCs by using Atmospheric Plasma Spraying (APS), plasma spraying-physical vapor deposition (PS-PVD) or Suspension Plasma Spraying (SPS). In particular, the surface of the TBCs or EBCs has a certain roughness after the preparation, and the CMAS-resistant protective layer is directly prepared on the surface of the ceramic top layer of the TBCs or EBCs, so that the problems that the microstructure of the TBCs or EBCs is damaged and the coating is thinned due to sand blasting are avoided.
Preferably, firstly, synthesizing ceramic powder with the particle size of 40nm-2 mu m by a chemical method, and then agglomerating the ceramic powder into particles with the particle size of 10 mu m-100 mu m by spray granulation for atmospheric plasma spraying; 5-60 μm of agglomerated particles are used for plasma spraying-physical vapor deposition; the ceramic powder with the grain diameter less than or equal to 5 mu m is prepared into suspension for suspension plasma spraying.
Preferably, in the atmospheric plasma spraying, the plasma spraying-physical vapor deposition or the suspension plasma spraying, the working power of a plasma spray gun is 40-200kW, the spraying distance is 50-1000mm, the vacuum degree is 100Pa-1atm, the moving speed of the spray gun is 0-1000mm/s, and the plasma gas takes Ar as main gas and H as H2And He as a secondary gas, with a total flow rate of 45-250slpm (standard liters per minute). In a preferred embodiment, the spraying equipment is an Oerlikon Metco multicoat F4 plasma spray gun, and the powder agglomerate particle size range is 10-100 μm. In another preferred embodiment, the apparatus for spraying is O of Oerlikon Metco PS-PVD system3CP plasma spray gun. In a further preferred embodiment, the spraying equipment is a 100HE plasma spray gun and the ceramic powder has a particle size D50 of 40 nm. In a further preferred embodiment, the spraying equipment is an Oerlikon Metco Triplexpro210 plasma spray gun, and the particle size of the ceramic powder is 2 μm.
Preferably, in suspension plasma spraying, the suspension has a concentration of 10-30%, the liquid medium is ethanol or deionized water, and the suspension further comprises a surfactant. More preferably, the surfactant is at least one of polyvinylpyrrolidone, polyethylene glycol, polyethyleneimine, sodium polyacrylate, and polyvinyl alcohol. More preferably, the surfactant is added in an amount of ≦ 3.0 wt.%.
The protective structure comprises a matrix layer, TBCs or EBCs and an anti-CMAS protective layer, wherein the TBCs or EBCs are prepared on the surface of the matrix layer, and the anti-CMAS protective layer is prepared on the surface of the TBCs or EBCs.
Preferably, the substrate layer is Ni-based superalloy, TBCs are prepared on the surface of the Ni-based superalloy, and the rare earth aluminate compound resisting the CMAS protective layer is (Tb)xRe(1-x))4Al2O9Wherein x is more than or equal to 0.5 and less than or equal to 1.0, and Re is one of Gd, Dy and Yb. It should be understood that the coefficient of thermal expansion of nickel-base superalloys is-9-12 x 10-6K-1Chemical composition (Tb)xRe(1-x))4Al2O9Is obtained by adjusting according to the comprehensive consideration of CMAS corrosion resistance and thermal expansion coefficient matching. In a preferred embodiment, the rare earth aluminate compounds of the anti-CMAS protective layer are Tb4Al2O9，(Gd0.5Tb0.5)4Al2O9，(Tb0.7Yb0.3)4Al2O9。
Preferably, the substrate layer is directionally solidified nickel-base superalloy DZ125 and third generation nickel-base single crystal superalloy DD 10.
Preferably, the TBCs comprise a bond coat and a YSZ ceramic thermal barrier, wherein the bond coat is formed on a surface of the substrate layer and the YSZ ceramic thermal barrier is formed on a surface of the bond coat. In a preferred embodiment, the bonding layer is prepared by a supersonic flame spraying method or a low-pressure plasma spraying method or a PS-PVD method; the YSZ ceramic thermal barrier layer is prepared on the bonding layer by adopting an atmospheric plasma spraying and PS-PVD method.
Preferably, the thickness of the adhesive layer is 100 μm to 120 μm.
Preferably, the bonding layer is NiCoCrAlYHf bonding layer, NiCoCrAlYTa bonding layer or NiCoCrAlYSi bonding layer.
Preferably, the thickness of the YSZ ceramic thermal barrier layer is 150 μm to 300 μm.
Preferably, the YSZ ceramic thermal barrier layer is a YSZ columnar crystal thermal barrier coating.
Preferably, the TBCs further comprise a high temperature thermal barrier ceramic layer, wherein the high temperature thermal barrier ceramic layer is prepared on the surface of the YSZ ceramic thermal barrier layer.
Preferably, the high temperature thermal barrier ceramic layer has a thickness of 150 μm to 250 μm.
Preferably, the chemical composition of the high-temperature thermal barrier ceramic layer is LaMgAl11O19、Gd2Zr2O7、(Gd0.9Yb0.1)2Zr2O7、La2(Ce0.3Zr0.7)2O7And YSZ + xGd2O3+yYb2O3At least one of (1).
Preferably, the matrix layer is a ceramic matrix composite, the EBCs are prepared on the surface of the ceramic matrix composite, and the rare earth aluminate compound of the anti-CMAS protective layer is (Gd)yRe(1-y))4Al2O9Wherein y is more than or equal to 0.5 and less than or equal to 1.0, and Re is one of Tb, Dy and Yb. It should be understood that the ceramic matrix composite has a coefficient of thermal expansion of 5 to 8X 10-6K-1Chemical composition (Gd)yRe(1-y))4Al2O9Is obtained by adjusting according to the comprehensive consideration of CMAS corrosion resistance and thermal expansion coefficient matching. In a preferred embodiment, the rare earth aluminate compound of the anti-CMAS protective layer is Gd4Al2O9。
Preferably, the matrix layer is SiCf/SiC。
Preferably, the EBCs comprise a bond layer, 3Al2O3x 2SiO2Moyinaite layer and Yb2SiO5Layer, wherein the bonding layer is prepared on the surface of the ceramic matrix composite material, 3Al2O3x 2SiO2The Monaian stone layer is prepared on the surface of the bonding layer, Yb2SiO5Layer preparation in 3Al2O3x 2SiO2The surface of the mohnite layer. In a preferred embodiment, the adhesive layer has a thickness of 100 μm, 3Al2O3x 2SiO2The thickness of the moannaite layer was 75 μm, Yb2SiO5The thickness of the layer was 75 μm.
According to the CMAS-resistant protective layer for TBCs or EBCs, the preparation method thereof and the protective structure obtained by the preparation method, the CMAS-resistant protective layer is used for CMAS corrosion degradation-resistant protection of the TBCs ceramic top surface of the nickel-based superalloy component of the aeroengine and the gas turbine, or CMAS corrosion degradation-resistant protection of the EBCs ceramic top surface of the CMCs component of the aeroengine and the gas turbine. Specifically, the anti-CMAS protective layer can rapidly block the penetration of molten CMAS within the working temperature range of 1200-1650 ℃, the corrosion degradation of CMAS only occurs on the surface of ReMA, the chemical components, the microstructure and the thermo-mechanical properties of inner TBCs or EBCs are protected, and the ultra-high temperature service stability and the thermal cycle life of the thermal barrier coating in the CMAS environment are greatly improved. Particularly, ReMA has good thermo-mechanical and chemical compatibility with the ceramic top layer of TBCs or EBCs, and can especially meet the CMAS protection requirement under 1300-1650 ℃ ultra-high temperature service; the ReMA coating material has higher chemical reaction activity with the molten CMAS, allows the ReMA coating to rapidly crystallize and solidify the liquid-phase CMAS within the range of 0.5-20% of larger porosity and 1230-1650 ℃, and protects TBCs or EBCs on the surface of high-temperature hot-end components of aeroengines and gas turbines for high-temperature long-life service; the ReMA coating can be prepared by selecting various spraying modes according to different service working conditions, and the preparation and processing cost of the TBCs or EBCs surfaces of the aeroengine and the gas turbine can be greatly reduced.
Drawings
FIG. 1 is a high purity Gd synthesized according to example 4 of the present invention after a high temperature reaction at 1600 ℃ for 12h4Al2O9Ceramic powder XRD atlas;
FIG. 2 is Gd according to example 4 high temperature solid phase synthesis of the present invention4Al2O9A scanning electron microscope topography of the ceramic powder;
FIG. 3 is Gd in example 4 according to the invention4Al2O9And (3) a section micrograph of the surface of the layer after CMAS is corroded and degraded for 100 hours at 1260 ℃. Gd (Gd)4Al2O9The layer effectively blocks penetration of molten CMAS at 1260 ℃, and surface corrosion products are distributed in a multilayer way;
FIG. 4 is a flowchart of example 4 according to the present inventionGd4Al2O9Section micrograph of CMAS corrosion degraded for 100h at 1350 deg.C on layer surface, Gd4Al2O9The layer effectively blocks the penetration of molten CMAS at 1350 ℃, and surface corrosion products are distributed in a multilayer way;
FIG. 5 is Gd in example 4 according to the invention4Al2O9Cross section micrograph of CMAS corrosion degraded for 100h at 1500 deg.C on the surface of the layer, Gd4Al2O9The layer effectively blocks penetration of molten CMAS at 1500 ℃, and surface corrosion products are distributed in a double layer.
Detailed Description
The preferred embodiments of the present invention will be described in detail below with reference to the accompanying drawings.
Example 1
The directional solidification nickel-based superalloy DZ125 is used as a matrix and is processed into the nickel-based superalloy by linear cutting, grinding and polishing
The wafer is subjected to sand blasting treatment on the surface of a sample by adopting 60-mesh corundum under compressed air, and then ultrasonic cleaning is sequentially carried out by using acetone and absolute alcohol, so that stains on the surface of the sample or adhered fine corundum sand grains are removed, and the sample is fully dried. A NiCoCrAlYHf bonding layer is prepared on the surface of the DZ125 high-temperature alloy substrate by adopting a supersonic flame spraying or low-pressure plasma spraying method, and the thickness is 120 mu m. Then, preparing a 150 μm thick YSZ ceramic thermal barrier layer on the bonding layer by atmospheric plasma spraying, and preparing a 150 μm thick novel high-temperature thermal barrier ceramic layer (chemical component is LaMgAl) on the surface of YSZ layer11O19、Gd2Zr2O7、(Gd0.9Yb0.1)2Zr2O7、La2(Ce0.3Zr0.7)2O7、YSZ+xGd2O3+yYb2O3Etc., without being limited to these). Finally, preparing Tb on the surface of the novel high-temperature thermal barrier coating by adopting atmospheric plasma spraying4Al2O9(TbAM) anti-CMAS anti-A covering layer having a thickness of 50 μm and a porosity of 20%. The equipment for spraying is an Oerlikon metco multicoat F4 plasma spray gun, the powder agglomeration particle size range is 10-100 μm, the spraying distance is 110mm, the working power of the spray gun is 40kW, the plasma gas is Ar-40slpm, H25slpm, a lance movement speed of 700 mm/s.
The TbAM protective coating prepared on the surface of the novel double-ceramic-layer high-temperature thermal barrier coating can rapidly block the penetration of molten CMAS within the working temperature range of 1200-1650 ℃ (preferably 1230-1500 ℃); CMAS corrosion degradation only occurs on the surface of the TbAM protective layer, and chemical components, microstructure and thermal mechanical properties of the novel high-temperature thermal barrier coating on the inner layer are well protected; greatly improves the ultra-high temperature service stability and the thermal cycle life of the thermal barrier coating in the CMAS environment.
Example 2
The third generation nickel-based single crystal superalloy DD10 is used as a substrate and is processed into the nickel-based single crystal superalloy by linear cutting, grinding and polishing
The wafer is prepared by polishing the surface of a sample by using sand paper until the roughness Ra is less than or equal to 1 mu m, then sequentially carrying out ultrasonic cleaning by using acetone and absolute alcohol, removing stains on the experimental surface or fine corundum sand grains adhered to the surface, and fully drying. A NiCoCrAlYTa bonding layer is prepared on a DD10 high-temperature alloy substrate by adopting a PS-PVD method, and the thickness of the bonding layer is 100 mu m. Then, a columnar crystal YSZ ceramic thermal barrier layer with the thickness of 300 mu m is prepared on the bonding layer by adopting a PS-PVD method respectively, and then a layer (Gd) is prepared on the surface of the YSZ ceramic thermal barrier layer0.5Tb0.5)4Al2O9(GdTBAM) anti-CMAS overcoat with a thickness of 100 μm and a porosity of 0.5%. An Oerlikon Metco PS-PVD system and an O3CP plasma spray gun are adopted, the spraying distance is 1000mm, the working power of the spray gun is 130kW, the plasma gas is Ar-110slpm and He-20slpm, the preheating temperature is 900 ℃, the vacuum degree is 100Pa, and the powder feeding rate is 8 g/min.
The example is prepared on the surface of YSZ high-temperature thermal barrier coating (Gd)0.5Tb0.5)4Al2O9The protective coating is at 1200-1650 deg.C (preferably 1230-1500 deg.C)DEG C) can rapidly block the penetration of the molten CMAS; CMAS corrosion degradation only occurs on the GdTBAM surface, and the chemical components, the microstructure and the thermal mechanical property of the inner YSZ columnar crystal thermal barrier coating are well protected; the thermal cycle life of the thermal barrier coating in the CMAS service environment is greatly prolonged.
Example 3
Taking directionally solidified nickel-based superalloy DZ125 as a substrate, performing wire cutting and polishing to obtain a sample with the thickness of 30mm multiplied by 3mm, performing sand blasting treatment on the surface of the sample by adopting 120-mesh corundum sand under compressed air, then sequentially placing the sample in acetone and absolute alcohol for ultrasonic cleaning, and drying after fully removing pollution impurities and corundum fine sand remained on the surface of the sample; preparing a NiCoCrAlYSi bonding layer with the thickness of 120 mu m on a DZ125 alloy substrate by adopting supersonic flame spraying or low-pressure plasma spraying, preparing a YSZ thermal barrier layer with the thickness of 150 mu m on the surface of a metal bonding layer by adopting atmospheric plasma spraying, and then preparing a novel high-temperature thermal barrier ceramic coating with the thickness of 250 mu m on the surface of YSZ, wherein the chemical component is LaMgAl11O19、Gd2Zr2O7、(Gd0.9Yb0.1)2Zr2O7、La2(Ce0.3Zr0.7)2O7Etc. (not limited to these). Then, high-purity (Tb) with a thickness of 50 μm was prepared on the outermost layer by suspension plasma spraying0.7Dy0.3)4Al2O9(TbDyAM) coating: (Tb)0.7Dy0.3)4Al2O9The particle diameter of the powder is D50 ═ 40nm, the suspension concentration is 10 wt.%, the surfactant is polyvinylpyrrolidone, and the addition amount is 3 wt.%. The flow rate of the suspension injected into the plasma jet is 50g/min, the spraying distance is 50mm, and the moving speed of the spray gun is 1000 mm/s. A100 HE (Progressive Surface, Grand Rapids, MI) plasma spray gun was used, with a spray power of 200 kW. Flow rate of plasma gas flow Ar-88slpm, H2-75slpm，N2-87slpm。
The embodiment is prepared on the surface of the high-temperature thermal barrier coating (Tb)0.7Yb0.3)4Al2O9The protective coating can rapidly block the penetration of the molten CMAS within the working temperature range of 1200-1650 ℃ (preferably 1230-1500 ℃); CMAS corrosion degradation only occurs on the surface of the TbDyAM protective layer, and the chemical components, the microstructure and the thermal mechanical properties of the inner double-ceramic-layer thermal barrier coating are well protected; the thermal cycle life of the thermal barrier coating in the CMAS service environment is greatly prolonged.
Example 4
With SiCfThe method comprises the following steps of cutting a/SiC CMCs (carbon nano tubes) serving as a substrate into samples of 30mm multiplied by 5mm, carrying out sand blasting treatment on the surfaces of the samples by adopting 36-mesh corundum sand under compressed air, then sequentially placing the samples into acetone and absolute alcohol for ultrasonic cleaning, and drying after fully removing pollution impurities and corundum fine sand remained on the surfaces of the samples; sequentially spraying Si-based intermediate bonding layers with the thickness of 100 mu m and 3Al with the thickness of 75 mu m on the surfaces of CMCs by adopting atmospheric plasma spraying2O3x 2SiO2A layer of mullite and Yb 75 μm thick2SiO5EBCs. Plasma spraying of suspensions on Yb2SiO5Gd with the thickness of 75 mu m is sprayed on the surface of the layer4Al2O9(GdMA) CMAS corrosion protection layer: gd (Gd)4Al2O9The particle size of the powder is D50 ═ 2 μm, the suspension concentration is 30 wt.%, the surfactant is polyethylene glycol, and the addition amount is 2 wt.%. The flow rate of the suspension injected into the plasma jet is 40g/min, the spraying distance is 70mm, and the moving speed of the spray gun is 1000 mm/s. An Oerlikon Metco Triplexpro210 plasma spray gun is adopted, the working power of the spray gun is 45kW, Ar45slpm and H2-8slpm。
The XRD pattern of the CMAS corrosion-resistant protective layer is shown in figure 1, the topography of a scanning electron microscope is shown in figure 2, and the section micrographs of the CMAS after corrosion degradation at 1260 ℃, 1350 ℃ and 1500 ℃ for 100h are shown in figures 3-5. Therefore, Gd prepared on the surface of the high-temperature thermal barrier coating in the embodiment4Al2O9The protective coating can rapidly block the penetration of the molten CMAS within the working temperature range of 1200-1650 ℃ (preferably 1230-1500 ℃); CMAS corrosion degradation only occurs on the surface of the protective layer, and chemical components, microstructure and thermal mechanical properties of the EBCs on the inner layer are well protected; greatly improve the ultra-high temperature service of the EBCsResistance to corrosion degradation by CMAS.
The above embodiments are merely preferred embodiments of the present invention, which are not intended to limit the scope of the present invention, and various changes may be made in the above embodiments of the present invention. All simple and equivalent changes and modifications made according to the claims and the content of the specification of the present application fall within the scope of the claims of the present patent application. The invention has not been described in detail in order to avoid obscuring the invention.
Claims (10)
1. An anti-CMAS protective layer for TBCs or EBCs, characterized in that the anti-CMAS protective layer is a rare earth aluminate compound Re4Al2O9Re is any one or two of Gd, Tb, Dy and Yb, the thickness of the anti-CMAS protective layer is 10-100 mu m, and the porosity of the anti-CMAS protective layer is 0.5-20%.
2. The method of claim 1, comprising applying atmospheric plasma spray, plasma spray-physical vapor deposition or suspension plasma spray to the surface of the TBCs or EBCs to form the CMAS-resistant protective coating.
3. The preparation method of claim 2, wherein ceramic powder with a particle size of 40nm-2 μm is synthesized by a chemical method, and then the ceramic powder is agglomerated into particles with a particle size of 10 μm-100 μm by spray granulation for atmospheric plasma spraying; 5-60 μm of agglomerated particles are used for plasma spraying-physical vapor deposition; the ceramic powder with the grain diameter less than or equal to 5 mu m is prepared into suspension for suspension plasma spraying.
4. The method according to claim 2, wherein in the atmospheric plasma spraying, the plasma spraying-physical vapor deposition or the suspension plasma spraying, the operating power of the plasma torch is 40 to 200kW, the spraying distance is 50 to 1000mm, the degree of vacuum is 100Pa to 1atm, the moving speed of the torch is 0 to 1000mm/s, and the plasma gas mainly contains Ar and mainly contains H2And He as an assist gas, with a total flow rate of 45-250 slpm.
5. The method according to claim 2, wherein the suspension has a concentration of 10 to 30% and the liquid medium is ethanol or deionized water, and the suspension further comprises a surfactant.
6. A protective structure comprising a substrate layer, TBCs or EBCs and an anti-CMAS protective layer according to claim 1, wherein the TBCs or EBCs are formed on the surface of the substrate layer and the anti-CMAS protective layer is formed on the surface of the TBCs or EBCs.
7. The protective structure according to claim 6, wherein the substrate layer is a nickel-base superalloy, the TBCs are prepared on the surface of the nickel-base superalloy, and the rare earth aluminate compound resistant to the CMAS protective layer is (Tb)xRe(1-x))4Al2O9Wherein x is more than or equal to 0.5 and less than or equal to 1.0, and Re is one of Gd, Dy and Yb.
8. The protective structure of claim 7, wherein the TBCs comprise a bond coat and a YSZ ceramic thermal barrier, wherein the bond coat is formed on a surface of the substrate layer and the YSZ ceramic thermal barrier is formed on a surface of the bond coat.
9. The protective structure of claim 8, wherein the TBCs further comprise a high temperature thermal barrier ceramic layer, wherein the high temperature thermal barrier ceramic layer is prepared on the surface of the YSZ ceramic thermal barrier layer.
10. The protective structure of claim 6, wherein the matrix layer is a ceramic matrix composite, the EBCs are prepared on the surface of the ceramic matrix composite, and the rare earth aluminate compound for resisting the CMAS protective layer is (Gd)yRe(1-y))4Al2O9Wherein y is more than or equal to 0.5 and less than or equal to 1.0, and Re is one of Tb, Dy and Yb.
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