CN114956811A - Scandium-cerium co-doped gadolinium zirconate thermal barrier coating material and preparation method thereof, and thermal barrier coating and preparation process thereof - Google Patents
Scandium-cerium co-doped gadolinium zirconate thermal barrier coating material and preparation method thereof, and thermal barrier coating and preparation process thereof Download PDFInfo
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- 239000012720 thermal barrier coating Substances 0.000 title claims abstract description 81
- 229910052688 Gadolinium Inorganic materials 0.000 title claims abstract description 80
- UIWYJDYFSGRHKR-UHFFFAOYSA-N gadolinium atom Chemical compound [Gd] UIWYJDYFSGRHKR-UHFFFAOYSA-N 0.000 title claims abstract description 80
- 239000000463 material Substances 0.000 title claims abstract description 69
- FEJWXSLFILQPBI-UHFFFAOYSA-N [Sc].[Ce] Chemical compound [Sc].[Ce] FEJWXSLFILQPBI-UHFFFAOYSA-N 0.000 title claims abstract description 48
- 238000002360 preparation method Methods 0.000 title claims abstract description 29
- 239000000203 mixture Substances 0.000 claims abstract description 21
- 229910010293 ceramic material Inorganic materials 0.000 claims abstract description 20
- 239000000126 substance Substances 0.000 claims abstract description 18
- WUKWITHWXAAZEY-UHFFFAOYSA-L calcium difluoride Chemical compound [F-].[F-].[Ca+2] WUKWITHWXAAZEY-UHFFFAOYSA-L 0.000 claims abstract description 6
- 239000010436 fluorite Substances 0.000 claims abstract description 6
- 239000000919 ceramic Substances 0.000 claims description 36
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- 239000000843 powder Substances 0.000 claims description 27
- 239000002244 precipitate Substances 0.000 claims description 22
- 239000000243 solution Substances 0.000 claims description 22
- 239000007921 spray Substances 0.000 claims description 15
- 229910052684 Cerium Inorganic materials 0.000 claims description 14
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 14
- 239000012265 solid product Substances 0.000 claims description 13
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 12
- 239000008367 deionised water Substances 0.000 claims description 11
- 229910021641 deionized water Inorganic materials 0.000 claims description 11
- 229910052751 metal Inorganic materials 0.000 claims description 11
- 239000002184 metal Substances 0.000 claims description 11
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- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonium chloride Substances [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 claims description 4
- QGZKDVFQNNGYKY-UHFFFAOYSA-N ammonia Natural products N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 4
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- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 239000003381 stabilizer Substances 0.000 description 1
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Abstract
The invention discloses a scandium-cerium co-doped gadolinium zirconate thermal barrier coating material and a preparation method thereof, and a thermal barrier coating and a preparation process thereof. The scandium-cerium co-doped gadolinium zirconate thermal barrier coating material is obtained by respectively and jointly doping Sc to Gd site and Ce to Zr site in a single gadolinium zirconate material, and has the chemical composition of (Gd) 0.925 Sc 0.075 ) 2 Zr 2‑x Ce x O 7 Wherein x is more than or equal to 0.15 and less than or equal to 0.60, and the material has a single-defect fluorite phase structure. The scandium-cerium co-doped gadolinium zirconate thermal barrier coating material prepared according to the invention has excellent high-temperature phase stability, low thermal conductivity and high fracture toughness, and a thermal barrier coating system prepared from the material has high fracture toughness which is improved by more than 30% compared with a single gadolinium zirconate thermal barrier coating. The thermal barrier coating ceramic material and the thermal barrier coating provided by the invention can be used as an alternative material of an ultrahigh-temperature thermal barrier coating of an aviation turbine engine.
Description
Technical Field
The invention belongs to the technical field of thermal barrier coatings, and particularly relates to a scandium-cerium co-doped gadolinium zirconate thermal barrier coating material and a preparation method thereof, and a thermal barrier coating and a preparation process thereof.
Background
The gadolinium zirconate ceramic material is one of the materials with better comprehensive performance in the rare earth zirconate materials, has the advantages of good chemical stability, excellent sintering resistance, CMAS corrosion resistance, low thermal conductivity and the like, and is considered to be one of the most promising thermal barrier coating materials. However, compared with the traditional YSZ material of the thermal barrier coating, the single gadolinium zirconate material has poor fracture toughness, so that the service life and the application are limited. In addition, the next generation of high performance aircraft engine thermal barrier coating materials require more excellent thermal insulation effects, i.e., low thermal conductivity. Therefore, through rare earth doping modification treatment on a single gadolinium zirconate material, the heat insulation performance and the fracture toughness of the single gadolinium zirconate material are improved, and a novel alternative material of a super-high temperature thermal barrier coating is hopefully provided.
At present, researches on rare earth doping modification of a single gadolinium zirconate material are divided into Gd-site doping, Zr-site doping and double-site doping, most of the researches focus on the improvement of thermophysical properties, and few researches on mechanical properties of the gadolinium zirconate materials are carried out. CeO (CeO) 2 As a good structural stabilizer, the thermal expansion coefficient is high, the thermal conductivity is low, and the prior art isResearch generally utilizes good thermophysical properties of the doped silicon carbide as a doping component for improving the thermophysical properties. Wangcimei and Guo (international ceramics, 2015) and the like find that Sc doping can improve the fracture toughness of a single gadolinium zirconate material, and the material can obtain a larger thermal expansion coefficient under a specific proportion, but the research of the Sc doping only aims at Gd site doping, and the doping is single.
Disclosure of Invention
The invention aims to provide a scandium-cerium co-doped gadolinium zirconate thermal barrier coating material and a preparation method thereof, a thermal barrier coating and a preparation process thereof, solves the problem of low fracture toughness of a single gadolinium zirconate material, obtains lower thermal conductivity, and provides a novel alternative material of an ultrahigh-temperature thermal barrier coating.
According to the first aspect of the invention, a scandium-cerium co-doped gadolinium zirconate thermal barrier coating material is provided, the scandium-cerium co-doped gadolinium zirconate thermal barrier coating material is obtained by respectively co-doping Sc to Gd site and Ce to Zr site double-site rare earth in a single gadolinium zirconate material, and the chemical composition of the double-site rare earth co-doped gadolinium zirconate ceramic material is (Gd) 0.925 Sc 0.075 ) 2 Zr 2- x Ce x O 7 Wherein x is more than or equal to 0.15 and less than or equal to 0.60, and the fluorite phase structure with single defect is presented.
According to a second aspect of the present invention, a preparation method of the above scandium-cerium co-doped gadolinium zirconate ceramic material is provided, which includes the following steps: a1: sc is respectively weighed according to a certain molar ratio 2 O 3 、Gd 2 O 3 、ZrOCl 2 ·8H 2 O、 Ce(NO 3 ) 4 Then Sc is added 2 O 3 And Gd 2 O 3 Dissolved in dilute hydrochloric acid, ZrOCl 2 ·8H 2 O、Ce(NO 3 ) 4 Dissolving in deionized water, mixing to prepare a mixed solution, adding polyethylene glycol for dispersion, and magnetically stirring for 1-2 hours to obtain a clear and transparent solution to obtain a precursor solution; a2: dropwise adding the precursor solution obtained in the step A1 into an ammonia water solution, keeping the pH value at 10.0-11.0 to fully form a precipitate, standing and aging for 24-28 hours to obtain a colloidal precipitate, and then sequentially using the colloidal precipitateFiltering and washing with ionized water for 3 times, and washing with anhydrous ethanol for 2 times to obtain precipitate and filtered solution; a3: drying the precipitate obtained in the step A2 to obtain a solid product; a4: and D, carrying out heat treatment on the solid product obtained in the step A3, cooling to room temperature, and grinding to obtain scandium-cerium co-doped gadolinium zirconate ceramic material powder. A5: pressing the powder obtained in the step A4 into a ceramic block; a6: and D, sintering and densifying the ceramic block body obtained in the step A5 at a high temperature to obtain the scandium-cerium co-doped gadolinium zirconate ceramic.
Preferably, in step A1, the Sc 2 O 3 、Gd 2 O 3 、ZrOCl 2 ·8H 2 O、Ce(NO 3 ) 4 The purity of (A) is 99.9% or more.
Preferably, in the step A2, the mass percentage concentration of the precipitant ammonia water is 25.0-28.0%.
Preferably, in the step A3, the precipitate obtained in the step A2 is put into an oven for drying at the temperature of 100-150 ℃ for 15-20 hours to obtain a solid product.
Preferably, in the step A4, the heat treatment temperature of the solid product obtained in the step A3 is 1100-1200 ℃, the time is 6-7 hours, and then the solid product is ground by a planetary ball mill at the speed of 400r/h for 8-12 hours.
Preferably, in the step a5, the powder obtained in the step a4 is subjected to compression molding by a micro isostatic press, wherein the preforming pressure is 10-15 MPa, the molding pressure is 250MPa, and the pressure maintaining time is 30 min.
Preferably, in the step A6, the ceramic block body obtained in the step A5 is sintered at high temperature for 40-48 hours in an air atmosphere at 1500-1550 ℃ to obtain the scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic.
According to a third aspect of the invention, a preparation process of a gadolinium zirconate based thermal barrier coating with high fracture toughness is provided, which comprises the following steps: b1: providing a scandium-cerium co-doped gadolinium zirconate thermal barrier coating material as described above;
b2: carrying out spray granulation and drying treatment on the scandium-cerium co-doped gadolinium zirconate thermal barrier coating material to prepare high-fluidity powder with the particle size of 30-75 microns as ceramic layer powder; b3: providing a nickel-based alloy substrate, and spraying NiCrAlY powder on the nickel-based alloy substrate to form a metal bonding layer; b4: and B, spraying the ceramic layer powder prepared in the step B2 on the metal bonding layer prepared in the step B3 by adopting a spraying process to form a ceramic layer, so as to obtain the thermal barrier coating.
Preferably, in step B2, the ceramic layer powder has a single defect fluorite phase structure, is in a hollow spherical shape, and has a rough and loose structure and pores on the surface.
Preferably, in step B3, the parameters in the preparation process of the metal bonding layer are: firstly, a spray gun is used for preheating a substrate to 350-450 ℃, then spraying is carried out, the spraying voltage is 55-65V, the spraying current is 400-600A, the moving speed of the spray gun is 450-550 mm/s, and the spraying distance is 50-150 mm.
Preferably, in step B4, the parameters of the ceramic layer preparation process are: firstly, a matrix is preheated to 380-500 ℃ by using a spray gun, then spraying is carried out, the spraying voltage is 55-65V, the spraying current is 500-700A, the moving speed of the spray gun is 100-200 mm/s, and the spraying distance is 60-100 mm.
Compared with the prior art, the invention has the advantages and beneficial effects that:
1) as a novel thermal barrier coating material, the invention adds two rare earth elements respectively by doping Sc to Gd site and Ce to Zr site in a single gadolinium zirconate material, improves the fracture toughness of the material, reduces the thermal conductivity on the basis of ensuring the high-temperature phase stability and higher thermal expansion coefficient, and provides a thermal barrier coating material with excellent mechanical property and thermal insulation property, wherein the chemical composition of the material is (Gd) 0.925 Sc 0.075 ) 2 Zr 2-x Ce x O 7 Wherein x is more than or equal to 0.15 and less than or equal to 0.60.
2) The preparation method of the doped modified ceramic material provided by the invention is simple and convenient to operate, low in cost, easy to control and suitable for industrial mass production.
According to a fourth aspect of the present invention, there is provided a gadolinium zirconate based thermal barrier coating with high fracture toughness prepared according to the above preparation process, wherein the thermal barrier coating comprises: a substrate layer, a metal bonding layer and a ceramic layer; it is composed ofWherein the composition of the base layer is high-temperature nickel-based alloy K438, the composition of the metal bonding layer is NiCrAlY, and the chemical composition of the ceramic layer is (Gd) 0.925 Sc 0.075 ) 2 Zr 2-x Ce x O 7 Wherein x is more than or equal to 0.15 and less than or equal to 0.60, and the fluorite phase structure with single defect is presented.
Due to the complex formulation and preparation, the research on the double-site doping of a single gadolinium zirconate material in the prior art is far less than that of the single-site doping. The comprehensive research on the thermal physical property and the mechanical property of the material is firstly found that the heat-insulating property of a single gadolinium zirconate material can be improved and the fracture toughness of the single gadolinium zirconate material is remarkably improved by co-doping the Sc with the Gd site and the Ce with the Zr site double-site rare earth.
Compared with the prior art, the invention has the advantages and beneficial effects that:
1) as a novel thermal barrier coating material, the Sc-Gd-site and Ce-Zr-site are codoped with two rare earth elements in a single gadolinium zirconate material respectively, so that on the basis of ensuring high-temperature phase stability and high thermal expansion coefficient, the fracture toughness of the material is improved, the thermal conductivity is reduced, and the scandium-cerium-codoped gadolinium zirconate thermal barrier coating material with excellent fracture toughness and thermal insulation performance is provided, and has the chemical composition (Gd) 0.925 Sc 0.075 ) 2 Zr 2-x Ce x O 7 Wherein x is more than or equal to 0.15 and less than or equal to 0.60; the thermal barrier coating material can be suitable for the material of choice for the ultrahigh-temperature thermal barrier coating of the aircraft turbine engine.
2) The preparation method of the doped modified ceramic material provided by the invention is simple and convenient to operate, low in cost, easy to control, high in reliability and suitable for industrial mass production.
3) The invention also provides a thermal barrier coating prepared by the scandium-cerium co-doped gadolinium zirconate thermal barrier coating material and a preparation process thereof, the thermal barrier coating system has excellent fracture toughness, and compared with a single gadolinium zirconate thermal barrier coating material, the thermal barrier coating system is improved by more than 30%, and the problem of poor fracture toughness of gadolinium zirconate is solved.
Drawings
FIG. 1 is an X-ray diffraction diagram of the scandium-cerium co-doped gadolinium zirconate thermal barrier coating material prepared in examples 1-4;
FIG. 2 is a Raman spectrum of the scandium-cerium co-doped gadolinium zirconate thermal barrier coating material prepared in examples 1 to 4;
FIG. 3 is a thermal conductivity graph of the novel scandium-cerium co-doped gadolinium zirconate thermal barrier coating material prepared in examples 1 to 4 and a single gadolinium zirconate material at a temperature ranging from room temperature to 1000 ℃;
FIG. 4 is a fracture toughness diagram of the novel scandium-cerium co-doped gadolinium zirconate thermal barrier coating material and a single gadolinium zirconate material prepared in examples 1 to 4;
FIG. 5 is a cross-sectional orgraph chart of a thermal barrier coating prepared in example 5;
FIG. 6 is a graph of fracture toughness of the novel scandium-cerium co-doped gadolinium zirconate thermal barrier coating prepared in example 5 and a single gadolinium zirconate coating.
Detailed Description
The present invention will be further described with reference to the following specific examples. It should be understood that the following examples are illustrative only and are not intended to limit the scope of the present invention.
Example 1
In this example, the chemical composition (Gd) was selected 0.925 Sc 0.075 ) 2 Zr 1.85 Ce 0.15 O 7 The scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic material is a preferred object. Sc with a purity of 99.9% 2 O 3 、Gd 2 O 3 、ZrOCl 2 ·8H 2 O、Ce(NO 3 ) 4 As raw material, according to the molar ratio Sc 2 O 3 ：Gd 2 O 3 ：ZrOCl 2 ·8H 2 O： Ce(NO 3 ) 4 8.41: 0.68: 16.82: 1.36 weight percent, Sc 2 O 3 And Gd 2 O 3 ZrOCl dissolved in dilute hydrochloric acid 2 ·8H 2 O and Ce (NO) 3 ) 4 Dissolving in deionized water, mixing the prepared solutions, adding polyethylene glycol for dispersion, and magnetically stirring for 1 hour to obtain a clear and transparent solution. The precursor solution is added dropwise to the diluted ammoniaIn aqueous solution, and the pH was kept at 10.5, sufficient to form a precipitate. After aging in the stock solution for 24 hours, the obtained precipitate is washed with deionized water for 3 times and then with absolute ethyl alcohol for 2 times to obtain a solid product. And calcining the precipitate in an air atmosphere at 1100 ℃ for 7 hours, cooling to room temperature, and grinding for 8 hours at 400r/h by using a planetary ball mill to obtain the required material powder. And pressing and molding the powder by using a micro isostatic pressing machine, wherein the preforming pressure is 10-15 MPa, the molding pressure is 250MPa, and the pressure is maintained for 30min to obtain the ceramic block. Sintering the obtained ceramic block at the high temperature of 1550 ℃ for 48 hours in the air atmosphere to obtain the scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic with the chemical composition of (Gd) 0.925 Sc 0.075 ) 2 Zr 1.85 Ce 0.15 O 7 。
As shown in fig. 3 to 4, the thermal conductivity of the prepared scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic material at 1000 ℃ is 1.422W/mK; the fracture toughness is 1.195 MPa.m 1/2 。
Example 2
In this example, the chemical composition (Gd) was selected 0.925 Sc 0.075 ) 2 Zr 1.70 Ce 0.30 O 7 The scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic material is a preferred object. Sc with a purity of 99.9% 2 O 3 、Gd 2 O 3 、 ZrOCl 2 ·8H 2 O、Ce(NO 3 ) 4 As raw material, according to the molar ratio Sc 2 O 3 ：Gd 2 O 3 ：ZrOCl 2 ·8H 2 O： Ce(NO 3 ) 4 8.41: 0.68: 15.45: 2.73 weight portions and Sc 2 O 3 And Gd 2 O 3 Dissolved in dilute hydrochloric acid, ZrOCl 2 ·8H 2 O and Ce (NO) 3 ) 4 Dissolving in deionized water, mixing the prepared solutions, adding polyethylene glycol for dispersion, and magnetically stirring for 1 hour to obtain a clear and transparent solution. The precursor solution was added dropwise to the diluted aqueous ammonia solution, and the pH was maintained at 10.5, to sufficiently form a precipitate. Aging in stock solution for 24 hr, washing the obtained precipitate with deionized water for 3 times, and washing with anhydrous ethanol for 2 times to obtain solid product. And calcining the precipitate in an air atmosphere at 1100 ℃ for 7 hours, cooling to room temperature, and grinding for 8 hours at 400r/h by using a planetary ball mill to obtain the required material powder. And (3) performing compression molding on the powder by using a micro isostatic pressing machine, wherein the preforming pressure is 10-15 MPa, the molding pressure is 250MPa, and the pressure is maintained for 30min to obtain the ceramic block. Sintering the obtained ceramic block at the high temperature of 1550 ℃ for 48 hours in the air atmosphere to obtain the scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic with the chemical composition of (Gd) 0.925 Sc 0.075 ) 2 Zr 1.70 Ce 0.30 O 7 。
As shown in fig. 3 to 4, the thermal conductivity of the prepared scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic material at 1000 ℃ is 1.284W/mK; the fracture toughness is 1.230 MPa.m 1/2 。
Example 3
In this example, the chemical composition (Gd) was selected 0.925 Sc 0.075 ) 2 Zr 1.55 Ce 0.45 O 7 The scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic material is a preferred object. Sc with a purity of 99.9% 2 O 3 、Gd 2 O 3 、 ZrOCl 2 ·8H 2 O、Ce(NO 3 ) 4 As raw material, according to the molar ratio Sc 2 O 3 ：Gd 2 O 3 ：ZrOCl 2 ·8H 2 O： Ce(NO 3 ) 4 8.41: 0.68: 14.09: 4.09 weight percent, Sc 2 O 3 And Gd 2 O 3 ZrOCl dissolved in dilute hydrochloric acid 2 ·8H 2 O and Ce (NO) 3 ) 4 Dissolving in deionized water, mixing the prepared solutions, adding polyethylene glycol for dispersion, and magnetically stirring for 1 hour to obtain a clear and transparent solution. The precursor solution was added dropwise to the diluted aqueous ammonia solution, and the pH was maintained at 10.5, to sufficiently form a precipitate. After aging in the stock solution for 24 hours, the obtained precipitate is washed with deionized water for 3 times and then with absolute ethyl alcohol for 2 times to obtain a solid product. And calcining the precipitate in an air atmosphere at 1100 ℃ for 7 hours, cooling to room temperature, and grinding by a planetary ball mill at 400r/h for 8 hours to obtain the required material powder. Pressing the powder by a micro isostatic pressAnd (3) performing and forming, wherein the preforming pressure is 10-15 MPa, the forming pressure is 250MPa, and the pressure is maintained for 30min to obtain the ceramic block. Sintering the obtained ceramic block at the high temperature of 1550 ℃ for 48 hours in the air atmosphere to obtain the scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic with the chemical composition of (Gd) 0.925 Sc 0.075 ) 2 Zr 1.55 Ce 0.45 O 7 。
As shown in fig. 3 to 4, the thermal conductivity of the prepared scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic material at 1000 ℃ is 1.228W/mK; the fracture toughness is 1.340 MPa.m 1/2 。
Example 4
In this example, the chemical composition (Gd) was selected 0.925 Sc 0.075 ) 2 Zr 1.60 Ce 0.40 O 7 The scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic material is a preferred object. Sc with a purity of 99.9% 2 O 3 、Gd 2 O 3 、 ZrOCl 2 ·8H 2 O、Ce(NO 3 ) 4 As raw material, according to the molar ratio Sc 2 O 3 ：Gd 2 O 3 ：ZrOCl 2 ·8H 2 O： Ce(NO 3 ) 4 8.41: 0.68: 12.73: 5.45 weight percent, Sc 2 O 3 And Gd 2 O 3 ZrOCl dissolved in dilute hydrochloric acid 2 ·8H 2 O and Ce (NO) 3 ) 4 Dissolving in deionized water, mixing the prepared solutions, adding polyethylene glycol for dispersion, and magnetically stirring for 1 hour to obtain a clear and transparent solution. The precursor solution was added dropwise to the diluted aqueous ammonia solution, and the pH was maintained at 10.5, to sufficiently form a precipitate. And aging in the stock solution for 24 hours, washing the obtained precipitate with deionized water for 3 times, and then washing with absolute ethyl alcohol for 2 times to obtain a solid product. And calcining the precipitate in an air atmosphere at 1100 ℃ for 7 hours, cooling to room temperature, and grinding by a planetary ball mill at 400r/h for 8 hours to obtain the required material powder. And pressing and molding the powder by using a micro isostatic pressing machine, wherein the preforming pressure is 10-15 MPa, the molding pressure is 250MPa, and the pressure is maintained for 30min to obtain the ceramic block. Sintering the obtained ceramic block at 1550 ℃ for 48 hours in an air atmosphere at a high temperature to obtain the scandium-cerium co-polymerGadolinium zirconate doped thermal barrier coating ceramic with chemical composition of (Gd) 0.925 Sc 0.075 ) 2 Zr 1.40 Ce 0.60 O 7 。
As shown in fig. 3 to 4, the thermal conductivity of the prepared scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic material at 1000 ℃ is 1.169W/mK; the fracture toughness is 1.446 MPa.m 1/2 。
Example 5
In this example, a gadolinium zirconate based thermal barrier coating sample with high fracture toughness was prepared by a conventional atmospheric plasma spray coating method. The chemical composition obtained by the chemical coprecipitation method of example 4 was (Gd) 0.925 Sc 0.075 ) 2 Zr 1.40 Ce 0.60 O 7 The scandium-cerium co-doped gadolinium zirconate material powder is prepared into high-fluidity powder with the particle size of 30-75 micrometers as ceramic layer powder through spray granulation and drying treatment. The materials of the substrate and the bonding layer are high-temperature nickel-based alloy K438 and NiCrAlY respectively. And preheating the substrate to 400 ℃ by using a spray gun, and spraying NiCrAlY powder to prepare the metal bonding layer. The spraying voltage and current were 60V and 500A, respectively, the moving speed of the spray gun was set to 500mm/s, and the spraying distance was 120 mm. And for the ceramic layer, the substrate is preheated to 400 ℃ by using a spray gun, the spraying voltage is 60V, the current is 600A, the moving speed of the spray gun is set to 150mm/s, and the spraying distance is 80mm, so that the novel scandium-cerium co-doped gadolinium zirconate thermal barrier coating is obtained.
As shown in fig. 5, the cross-sectional texture of the thermal barrier coating is shown. As shown in FIG. 6, the fracture toughness of the prepared novel scandium-cerium co-doped gadolinium zirconate thermal barrier coating is 1.415W/mK, which is improved by 34.5% compared with that of a single gadolinium zirconate thermal barrier coating material.
The results prove that compared with a single gadolinium zirconate material, the scandium-cerium co-doped gadolinium zirconate thermal barrier coating ceramic material provided by the invention has the advantages of low thermal conductivity, high fracture toughness, low preparation cost, simple preparation method and easiness in industrial production and application; the prepared novel scandium-cerium co-doped gadolinium zirconate thermal barrier coating has high fracture toughness, and is improved by more than 30% compared with a single gadolinium zirconate thermal barrier coating. The scandium-cerium co-doped gadolinium zirconate ceramic material and the thermal barrier coating provided by the invention can be used for an alternative technology of an ultrahigh-temperature thermal barrier coating of an aviation turbine engine.
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 (12)
1. The scandium-cerium co-doped gadolinium zirconate thermal barrier coating material is characterized in that a scandium-cerium co-doped gadolinium zirconate ceramic material is obtained by respectively co-doping Sc to Gd site and Ce to Zr site double-site rare earth in a single gadolinium zirconate material, and the scandium-cerium co-doped gadolinium zirconate ceramic material has a chemical composition of (Gd site) 0.925 Sc 0.075 ) 2 Zr 2-x Ce x O 7 Wherein x is more than or equal to 0.15 and less than or equal to 0.60, and the single-defect fluorite phase structure is presented.
2. The preparation method of the scandium-cerium co-doped gadolinium zirconate thermal barrier coating material as claimed in claim 1, characterized by comprising the following steps:
a1: sc is respectively weighed according to a certain molar ratio 2 O 3 、Gd 2 O 3 、ZrOCl 2 ·8H 2 O、Ce(NO 3 ) 4 Then Sc is added 2 O 3 And Gd 2 O 3 ZrOCl dissolved in dilute hydrochloric acid 2 ·8H 2 O、Ce(NO 3 ) 4 Dissolving in deionized water, mixing to prepare a mixed solution, adding polyethylene glycol for dispersion, and magnetically stirring for 1-2 hours to obtain a clear and transparent solution to obtain a precursor solution;
a2: dropwise adding the precursor solution obtained in the step A1 into an ammonia water solution, keeping the pH value at 10.0-11.0 to fully form a precipitate, standing and aging for 24-28 hours to obtain a colloidal precipitate, and then sequentially filtering and washing with deionized water and absolute ethyl alcohol to obtain a precipitate and a filtered solution;
a3: drying the precipitate obtained in the step A2 to obtain a solid product;
a4: c, cooling the solid product obtained in the step A3 to room temperature after heat treatment, and grinding to obtain scandium-cerium co-doped gadolinium zirconate ceramic material powder;
a5: pressing the powder obtained in the step A4 into a ceramic block;
a6: and C, sintering and densifying the ceramic block obtained in the step A5 at a high temperature to obtain the scandium-cerium co-doped gadolinium zirconate thermal barrier coating material.
3. The method according to claim 2, wherein in step A1, the Sc is 2 O 3 、Gd 2 O 3 、ZrOCl 2 ·8H 2 O、Ce(NO 3 ) 4 The purity of the product is more than 99.9 percent.
4. The method according to claim 2, wherein in step A2, the concentration of the aqueous ammonia solution is 25.0 to 28.0% by mass.
5. The preparation method according to claim 2, wherein in the step A3, the precipitate obtained in the step A2 is dried in an oven at a temperature of 100-150 ℃ for 15-20 hours to obtain a solid product.
6. The method according to claim 2, wherein in step A4, the solid product obtained in step A3 is heat treated at 1100-1200 ℃ for 6-7 hours, and then ground by a planetary ball mill at a speed of 300-500 r/h for 8-12 hours.
7. The preparation method according to claim 2, wherein in the step A5, the powder obtained in the step A4 is subjected to compression molding by a micro isostatic press, the pressure of the pre-molding is 10-15 MPa, the molding pressure is 250MPa, and the pressure maintaining time is 30 min.
8. The preparation method of claim 2, wherein in the step A6, the ceramic block obtained in the step A5 is sintered at a high temperature of 1500-1550 ℃ in an air atmosphere for 40-48 hours to obtain the scandium-cerium co-doped gadolinium zirconate thermal barrier coating material.
9. A preparation process of a gadolinium zirconate-based thermal barrier coating with high fracture toughness is characterized by comprising the following steps:
b1: providing a scandium-cerium co-doped gadolinium zirconate thermal barrier coating material according to claim 1;
b2: carrying out spray granulation and drying treatment on the scandium-cerium co-doped gadolinium zirconate thermal barrier coating material to prepare high-fluidity powder with the particle size of 30-75 microns as ceramic layer powder;
b3: providing a nickel-based alloy substrate, and spraying NiCrAlY powder on the nickel-based alloy substrate to form a metal bonding layer;
b4: and B, spraying the ceramic layer powder prepared in the step B2 on the metal bonding layer prepared in the step B3 by adopting a spraying process to form a ceramic layer, so that the gadolinium zirconate-based thermal barrier coating with high fracture toughness can be obtained.
10. The process of claim 9, wherein in step B3, the parameters of the metal bonding layer preparation process are: firstly, a spray gun is used for preheating a substrate to 350-450 ℃, then spraying is carried out, the spraying voltage is 55-65V, the spraying current is 400-600A, the moving speed of the spray gun is 450-550 mm/s, and the spraying distance is 50-150 mm.
11. The spraying process according to claim 9, wherein in step B4, the parameters of the ceramic layer preparation process are: firstly, a matrix is preheated to 380-500 ℃ by using a spray gun, then spraying is carried out, the spraying voltage is 55-65V, the spraying current is 500-700A, the moving speed of the spray gun is 100-200 mm/s, and the spraying distance is 60-100 mm.
12. A high-breaking polymer prepared by the preparation process according to any one of claims 9 to 11A tough gadolinium zirconate-based thermal barrier coating, characterized in that the thermal barrier coating comprises: a substrate layer, a metal bonding layer and a ceramic layer; wherein the composition of the basal layer is high-temperature nickel-based alloy K438, the composition of the metal bonding layer is NiCrAlY, and the chemical composition of the ceramic layer is (Gd) 0.925 Sc 0.075 ) 2 Zr 2-x Ce x O 7 Wherein x is more than or equal to 0.15 and less than or equal to 0.60, and the fluorite phase structure with single defect is presented.
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