CN115418596A - Eutectic toughening sintering-resistant alumina/rare earth doped zirconia ultrahigh-temperature thermal barrier coating spraying material, and preparation method and application thereof - Google Patents
Eutectic toughening sintering-resistant alumina/rare earth doped zirconia ultrahigh-temperature thermal barrier coating spraying material, and preparation method and application thereof Download PDFInfo
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- CN115418596A CN115418596A CN202211163960.0A CN202211163960A CN115418596A CN 115418596 A CN115418596 A CN 115418596A CN 202211163960 A CN202211163960 A CN 202211163960A CN 115418596 A CN115418596 A CN 115418596A
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- 239000000463 material Substances 0.000 title claims abstract description 85
- 238000005245 sintering Methods 0.000 title claims abstract description 55
- 238000005507 spraying Methods 0.000 title claims abstract description 42
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 title claims abstract description 40
- 229910052761 rare earth metal Inorganic materials 0.000 title claims abstract description 28
- 239000012720 thermal barrier coating Substances 0.000 title claims abstract description 28
- 150000002910 rare earth metals Chemical class 0.000 title claims abstract description 26
- 230000005496 eutectics Effects 0.000 title claims abstract description 20
- 238000002360 preparation method Methods 0.000 title claims abstract description 19
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 title claims abstract description 17
- 239000000843 powder Substances 0.000 claims abstract description 61
- 239000011248 coating agent Substances 0.000 claims abstract description 27
- 238000000576 coating method Methods 0.000 claims abstract description 27
- 239000011858 nanopowder Substances 0.000 claims abstract description 23
- 238000005054 agglomeration Methods 0.000 claims abstract description 19
- 238000007750 plasma spraying Methods 0.000 claims abstract description 18
- 229910001404 rare earth metal oxide Inorganic materials 0.000 claims abstract description 18
- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims abstract description 13
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 8
- 238000013329 compounding Methods 0.000 claims abstract description 3
- 239000007921 spray Substances 0.000 claims description 27
- 239000002244 precipitate Substances 0.000 claims description 24
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 claims description 23
- 239000002131 composite material Substances 0.000 claims description 22
- 238000000498 ball milling Methods 0.000 claims description 19
- 239000004793 Polystyrene Substances 0.000 claims description 16
- 229920002223 polystyrene Polymers 0.000 claims description 16
- 238000003756 stirring Methods 0.000 claims description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 14
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 13
- 239000012153 distilled water Substances 0.000 claims description 13
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 13
- 238000001816 cooling Methods 0.000 claims description 11
- 239000002002 slurry Substances 0.000 claims description 9
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 7
- 235000011114 ammonium hydroxide Nutrition 0.000 claims description 7
- 238000001035 drying Methods 0.000 claims description 7
- 238000010438 heat treatment Methods 0.000 claims description 7
- 238000000034 method Methods 0.000 claims description 7
- -1 aluminum ions Chemical class 0.000 claims description 6
- 239000007787 solid Substances 0.000 claims description 6
- OERNJTNJEZOPIA-UHFFFAOYSA-N zirconium nitrate Chemical compound [Zr+4].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O OERNJTNJEZOPIA-UHFFFAOYSA-N 0.000 claims description 4
- 238000009413 insulation Methods 0.000 claims description 3
- BNGXYYYYKUGPPF-UHFFFAOYSA-M (3-methylphenyl)methyl-triphenylphosphanium;chloride Chemical compound [Cl-].CC1=CC=CC(C[P+](C=2C=CC=CC=2)(C=2C=CC=CC=2)C=2C=CC=CC=2)=C1 BNGXYYYYKUGPPF-UHFFFAOYSA-M 0.000 claims description 2
- 229910052782 aluminium Inorganic materials 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 claims description 2
- UZLYXNNZYFBAQO-UHFFFAOYSA-N oxygen(2-);ytterbium(3+) Chemical compound [O-2].[O-2].[O-2].[Yb+3].[Yb+3] UZLYXNNZYFBAQO-UHFFFAOYSA-N 0.000 claims description 2
- 239000000725 suspension Substances 0.000 claims description 2
- 229910003454 ytterbium oxide Inorganic materials 0.000 claims description 2
- 229940075624 ytterbium oxide Drugs 0.000 claims description 2
- 229910052726 zirconium Inorganic materials 0.000 claims description 2
- 238000002485 combustion reaction Methods 0.000 claims 1
- 238000005516 engineering process Methods 0.000 abstract description 8
- 238000005469 granulation Methods 0.000 abstract description 7
- 230000003179 granulation Effects 0.000 abstract description 7
- 239000000203 mixture Substances 0.000 abstract description 3
- 239000011148 porous material Substances 0.000 abstract description 3
- 238000012216 screening Methods 0.000 abstract description 2
- 230000002776 aggregation Effects 0.000 abstract 2
- 238000001694 spray drying Methods 0.000 abstract 1
- 239000000126 substance Substances 0.000 abstract 1
- 239000000919 ceramic Substances 0.000 description 20
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 11
- 238000005303 weighing Methods 0.000 description 10
- 238000001914 filtration Methods 0.000 description 5
- 230000001965 increasing effect Effects 0.000 description 5
- 239000002245 particle Substances 0.000 description 5
- 238000007873 sieving Methods 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
- 238000005406 washing Methods 0.000 description 5
- 229910001928 zirconium oxide Inorganic materials 0.000 description 5
- WXKDNDQLOWPOBY-UHFFFAOYSA-N zirconium(4+);tetranitrate;pentahydrate Chemical compound O.O.O.O.O.[Zr+4].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O WXKDNDQLOWPOBY-UHFFFAOYSA-N 0.000 description 5
- XNDZQQSKSQTQQD-UHFFFAOYSA-N 3-methylcyclohex-2-en-1-ol Chemical compound CC1=CC(O)CCC1 XNDZQQSKSQTQQD-UHFFFAOYSA-N 0.000 description 4
- QBAZWXKSCUESGU-UHFFFAOYSA-N yttrium(3+);trinitrate;hexahydrate Chemical compound O.O.O.O.O.O.[Y+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O QBAZWXKSCUESGU-UHFFFAOYSA-N 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 238000011160 research Methods 0.000 description 3
- 238000012876 topography Methods 0.000 description 3
- YUDXIXJILDPJEF-UHFFFAOYSA-N ytterbium(3+);trinitrate;hexahydrate Chemical compound O.O.O.O.O.O.[Yb+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O YUDXIXJILDPJEF-UHFFFAOYSA-N 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 2
- 229910010293 ceramic material Inorganic materials 0.000 description 2
- 238000009694 cold isostatic pressing Methods 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 238000003825 pressing Methods 0.000 description 2
- 229910002080 8 mol% Y2O3 fully stabilized ZrO2 Inorganic materials 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 238000005524 ceramic coating Methods 0.000 description 1
- 238000012512 characterization method Methods 0.000 description 1
- RKTYLMNFRDHKIL-UHFFFAOYSA-N copper;5,10,15,20-tetraphenylporphyrin-22,24-diide Chemical compound [Cu+2].C1=CC(C(=C2C=CC([N-]2)=C(C=2C=CC=CC=2)C=2C=CC(N=2)=C(C=2C=CC=CC=2)C2=CC=C3[N-]2)C=2C=CC=CC=2)=NC1=C3C1=CC=CC=C1 RKTYLMNFRDHKIL-UHFFFAOYSA-N 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 230000005764 inhibitory process Effects 0.000 description 1
- 230000000977 initiatory effect Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910002077 partially stabilized zirconia Inorganic materials 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 238000010290 vacuum plasma spraying Methods 0.000 description 1
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 description 1
- RUDFQVOCFDJEEF-UHFFFAOYSA-N yttrium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Y+3].[Y+3] RUDFQVOCFDJEEF-UHFFFAOYSA-N 0.000 description 1
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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
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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
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01D—NON-POSITIVE DISPLACEMENT MACHINES OR ENGINES, e.g. STEAM TURBINES
- F01D25/00—Component parts, details, or accessories, not provided for in, or of interest apart from, other groups
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01D—NON-POSITIVE DISPLACEMENT MACHINES OR ENGINES, e.g. STEAM TURBINES
- F01D25/00—Component parts, details, or accessories, not provided for in, or of interest apart from, other groups
- F01D25/005—Selecting particular materials
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T50/00—Aeronautics or air transport
- Y02T50/60—Efficient propulsion technologies, e.g. for aircraft
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Abstract
The invention relates to the technical field of thermal barrier coating materials, in particular to a eutectic toughening anti-sintering alumina/rare earth doped zirconia ultrahigh-temperature thermal barrier coating spraying material, a preparation method and application thereof, wherein the spraying powder material is prepared from (40-75) ZrO 2 ，(20‑35)(Y,Yb) 2 O 3 ，(5‑25)Al 2 O 3 Composition, first of all ZrO is prepared by chemical means 2 ‑(Y,Yb) 2 O 3 ‑Al 2 O 3 Compounding the nano powder material, then preparing nano agglomeration spraying powder containing a pore-forming agent by spray drying granulation, and obtaining the nano agglomeration spraying powder suitable for plasma spraying by screening. The nano-agglomerated spraying powder material of the alumina-zirconia-rare earth oxide prepared by the inventionThe material has uniform microstructure, is spherical and has good fluidity. The alumina-zirconia-rare earth oxide coating prepared by adopting the plasma spraying technology has a certain amount of eutectic structures and pores, effectively improves the fracture toughness and the high-temperature sintering resistance of the coating, and simultaneously reduces the thermal conductivity of the coating.
Description
Technical Field
The invention relates to the technical field of thermal barrier coating materials, in particular to a eutectic toughening anti-sintering alumina/rare earth doped zirconia ultrahigh-temperature thermal barrier coating spraying material, a preparation method and application thereof.
Background
Thermal barrier coating technology has been widely applied to hot end components of gas turbine engines, significantly reduces the working temperature of the surface of the hot end component, improves the thermal efficiency of the engine and prolongs the service life of the engine in complex environments. Thermal barrier coating technology has become one of the indispensable key scientific technologies of high performance gas turbine engines. With the development of high heat efficiency, low oil consumption and long service life of the engine, the temperature of the front inlet of the turbine of the engine is continuously increased, and more severe requirements are provided for thermal barrier coating materials. The most classical and widely used thermal barrier coating at present is (6 to 8,wt.%) yttria partially stabilized zirconia (abbreviated as 8 YSZ). However, 8YSZ is in service in an environment higher than 1200 ℃ for a long time, and phenomena such as transformation from a tetragonal phase to a monoclinic phase, high-temperature sintering, high oxygen transmission rate, and aggravated surface deposit corrosion occur. Therefore, there is a need to research a novel ultra-high temperature thermal barrier coating with high temperature resistance, low thermal conductivity and sintering resistance to meet the urgent requirements of the next generation of high performance gas turbine engine.
The rare earth doped zirconium dioxide is an effective way for improving the heat insulation performance and the high-temperature phase stability, and is also one of the research hotspots of the ultrahigh-temperature thermal barrier coating. The rare earth doped zirconium dioxide has low thermal conductivity due to the existence of more oxygen vacancies in the crystal structure, but the oxygen vacancies migrate during high-temperature long-time sintering to accelerate the sintering of the coating. Meanwhile, the rare earth doped zirconium dioxide coating has the defects of poor fracture toughness, insufficient crack initiation and expansion inhibition capability and the like, and is easy to cause brittle fracture of the coating in the thermal cycle process, so that the thermal cycle life of the coating is shortened. Therefore, while maintaining the original excellent properties of the rare earth doped zirconium dioxide coating, such as low thermal conductivity, good high temperature phase stability, etc., it is imperative to improve the fracture toughness and the high temperature sintering resistance.
In view of the above-mentioned drawbacks, the inventors of the present invention have finally obtained the present invention through a long period of research and practice.
Disclosure of Invention
The invention aims to solve the problem of how to improve the fracture toughness and the high-temperature sintering resistance of a rare earth doped zirconium dioxide coating while keeping the original excellent properties of low thermal conductivity, good high-temperature phase stability and the like of the rare earth doped zirconium dioxide coating, and provides a eutectic toughened sintering-resistant aluminum oxide/rare earth doped zirconium oxide ultrahigh-temperature thermal barrier coating spraying material, a preparation method and application thereof.
In order to achieve the aim, the invention discloses a eutectic toughening sintering-resistant alumina/rare earth doped zirconia ultrahigh-temperature thermal barrier coating spraying material which comprises the following components: zrO (zirconium oxide) 2 Rare earth oxide RE 2 O 3 、Al 2 O 3 Of said ZrO 2 Rare earth oxide RE 2 O 3 、Al 2 O 3 The molar ratio of (A) to (B) is 40-75: 20 to 35:5 to 25.
The rare earth oxide RE 2 O 3 Is one or the combination of two of yttrium oxide and ytterbium oxide.
The invention also discloses a preparation method of the eutectic toughening sintering-resistant alumina/rare earth doped zirconia ultrahigh-temperature thermal barrier coating spraying material, which comprises the following steps:
s1: preparing the composite nano powder material of the alumina-zirconia-rare earth oxide: mixing aluminum nitrate, zirconium nitrate and rare earth oxide, adding distilled water to prepare a solution, heating while stirring until a transparent solution is formed, then cooling to room temperature, dropwise adding the transparent solution containing aluminum ions, zirconium ions and rare earth ions into ammonia water while stirring until white precipitates are completely formed, and sintering the white precipitates to obtain ZrO 2 -RE 2 O 3 -Al 2 O 3 Compounding nano powder material;
s2: preparing the nano-agglomeration spraying powder material of the alumina-zirconia-rare earth oxide: is reacted with ZrO 2 -RE 2 O 3 -Al 2 O 3 Composite nano powder material, polyvinyl alcohol solution with mass fraction of 10%, polystyrene powder and distilled waterAnd (3) ball-milling the water and the n-butyl alcohol to obtain uniform slurry, performing spray granulation and drying to obtain a nano-agglomeration spraying powder material of alumina-zirconia-rare earth oxide containing a polystyrene pore-forming agent, and screening the nano-agglomeration spraying powder through a screen to obtain the spraying material.
The concentration of the solution prepared in the step S1 is 0.5-1 mol/L.
In the step S1, the sintering temperature is 1000-1100 ℃, and the sintering time is 2-4 h.
In the step S2, the mass fraction of polyvinyl alcohol in the polyvinyl alcohol solution is 10%.
In the step S2, the ball milling speed is 360-400 r/min, and the ball milling time is 3-5 h.
ZrO added to the slurry of the step S2 2 -RE 2 O 3 -Al 2 O 3 The composite nano powder material accounts for 30-40% of the solid content by mass, the polyvinyl alcohol solution accounts for 2-4% of the solid content by mass, the polystyrene accounts for 5-10% of the solid content by mass, and the volume of the added n-butyl alcohol is 3-5 mL.
The invention also discloses application of the eutectic toughening anti-sintering aluminum oxide/rare earth doped zirconium oxide ultrahigh-temperature thermal barrier coating spraying material to a hot end part of a turbine engine which is fired in advance, and the aluminum oxide/rare earth doped zirconium oxide ultrahigh-temperature thermal barrier coating is prepared by spraying the spraying powder material by using a plasma spraying technology.
The plasma spraying technology comprises atmospheric plasma spraying, vacuum plasma spraying, low-pressure plasma spraying and suspension plasma spraying.
Compared with the prior art, the invention has the beneficial effects that:
1. the nano-agglomerated spraying powder material of the alumina-zirconia-rare earth oxide prepared by the invention has uniform microstructure, is spherical and has good fluidity;
2. the alumina-zirconia-rare earth oxide heat-insulating coating prepared by the atmospheric plasma spraying technology has a certain amount of eutectic structures and pores, effectively improves the fracture toughness and the high-temperature sintering resistance of the coating, simultaneously reduces the heat conductivity of the coating, and is beneficial to enhancing the heat-insulating capability of the coating.
Drawings
FIG. 1 shows the preparation of ZrO 2 -Y 2 O 3 -Al 2 O 3 A morphology of the composite nano-agglomerate spray powder material;
FIG. 2 shows atmospheric plasma spraying of 40ZrO 2 -35Yb 2 O 3 -25Al 2 O 3 Sintering the surface topography of the coating at 1400 ℃ for different times;
FIG. 3 is 50ZrO 2 -16Y 2 O 3 -10Yb 2 O 3 -24Al 2 O 3 Sintering the ceramic blocks at 1400 ℃ for different time to obtain surface topography maps;
FIG. 4 is 71.5ZrO 2 -16Y 2 O 3 -10Yb 2 O 3 -2.5Al 2 O 3 And sintering the ceramic blocks at 1400 ℃ for different time to obtain surface topography maps.
FIG. 5 is a plasma sprayed 75ZrO 2 -25Y 2 O 3 The cross-sectional shape of the coating before and after sintering for 100 hours at 1400 ℃.
Detailed Description
The above and further features and advantages of the present invention are described in more detail below with reference to the accompanying drawings.
Example 1
Step 1: preparation of 75ZrO 2 -20Y 2 O 3 -5Al 2 O 3 (mol.%) composite nanopowder material:
weighing 150g of aluminum nitrate nonahydrate, 1288g of zirconium nitrate pentahydrate and 612.8g of yttrium nitrate hexahydrate powder material in a clean beaker, adding 8000mL of distilled water to prepare a solution with the concentration of 0.5mol/L, heating and stirring to form a transparent solution, and then cooling to room temperature; then dropwise adding the transparent solution into sufficient ammonia water while stirring until white precipitate is completely formed, testing that the pH value of the solution containing the white precipitate is more than 9, and then filtering and washing for three times to obtain white precipitate; finally, sintering the white precipitate in a muffle furnace at 1100 ℃ for 3h to prepare the composite nano powder material;
step 2: preparation of 75ZrO 2 -20Y 2 O 3 -5Al 2 O 3 Nano-agglomeration spraying powder material:
weighing 500g of the composite nano powder material prepared in the step 1, 15g of a polyvinyl alcohol solution with the mass fraction of 10%, 25g of polystyrene powder, 1650g of distilled water and 3mL of n-butanol in a ball milling tank, and then placing the ball milling tank in a planetary ball mill to ball mill for 4 hours at the speed of 400r/min to obtain uniform slurry. Preparing 75ZrO containing polystyrene pore forming agent by adopting spray granulation drying process 2 -20Y 2 O 3 -5Al 2 O 3 Nano-agglomeration spraying powder material; finally, sieving the nano-aggregate spray powder to screen to obtain powder material with the particle size of 15-60 mu m for plasma spraying.
The nano-agglomerated spray powder prepared above was subjected to microstructure characterization using a scanning electron microscope, as shown in fig. 1. As can be seen from the figure, 75ZrO was produced 2 -20Y 2 O 3 -5Al 2 O 3 Most of the nano-agglomerated spraying powder material is spherical, and a small part of the nano-agglomerated spraying powder material is in an apple shape, and the surface tissue of the powder is uniform. The flowability of the nano-agglomeration spraying powder material is 55s/50g through a Hall flow meter.
Example 2
Step 1: preparation of 40ZrO 2 -35Yb 2 O 3 -25Al 2 O 3 (mol.%) composite nanopowder material:
weighing 750g of aluminum nitrate nonahydrate, 687g of zirconium nitrate pentahydrate and 1308g of ytterbium nitrate hexahydrate powder material in a clean beaker, preparing a solution with the concentration of 1mol/L by 4000mL of distilled water, heating and stirring to form a transparent solution, and then cooling to room temperature; then dropwise adding the transparent solution into sufficient ammonia water while stirring until white precipitate is completely formed, testing that the pH value of the solution containing the white precipitate is more than 9, and then filtering and washing for three times to obtain white precipitate; finally, sintering the white precipitate in a muffle furnace at 1050 ℃ for 4 hours to prepare a composite nano powder material;
step 2: preparation of 40ZrO 2 -35Yb 2 O 3 -25Al 2 O 3 Nano-agglomeration spraying powder material:
weighing 500g of the composite nano powder material prepared in the step 1, 20g of a polyvinyl alcohol solution with the mass fraction of 10%, 40g of polystyrene powder, 1428g of distilled water and 4mL of n-butanol in a ball milling tank, and then placing the ball milling tank in a planetary ball mill to ball mill for 5 hours at the speed of 360r/min to obtain uniform slurry. Preparing 40ZrO containing polystyrene pore-forming agent by adopting spray granulation drying process 2 -35Y 2 O 3 -25Al 2 O 3 Nano-agglomeration spraying powder material; finally, sieving the nano-aggregate spray powder to screen to obtain powder material with the particle size of 15-60 mu m for plasma spraying.
40ZrO prepared by adopting atmospheric plasma spraying technology 2 -35Yb 2 O 3 -25Al 2 O 3 The nano-agglomeration spraying powder material is prepared into the ceramic heat-insulation coating. Respectively sintering the prepared coating at 1400 ℃ for 10h, 50h, 100h and 200h, then cooling to room temperature along with the furnace, and taking out. The sintered ceramic coating was characterized using SEM and it was found that the grain size of the coating surface remained almost unchanged with increasing sintering time at 1400 ℃, showing excellent high temperature sintering resistance as shown in figure 2.
Example 3
Step 1: preparation of 50ZrO 2 -16Y 2 O 3 -10Yb 2 O 3 -24Al 2 O 3 (mol.%) composite nanopowder material:
weighing 540g of aluminum nitrate nonahydrate, 644g of zirconium nitrate pentahydrate, 368g of yttrium nitrate hexahydrate and 280g of ytterbium nitrate hexahydrate powder material in a clean beaker, adding 4000mL of distilled water to prepare a solution with the concentration of 0.75mol/L, heating and stirring to form a transparent solution, and then cooling to room temperature; then dropwise adding the transparent solution into sufficient ammonia water while stirring until white precipitate is completely formed, testing the pH value of the solution containing the white precipitate to be 10, and then filtering and washing for three times to obtain white precipitate; finally, sintering the white precipitate in a muffle furnace at 1100 ℃ for 4h to prepare the composite nano powder material;
step 2: preparation of 50ZrO 2 -16Y 2 O 3 -10Yb 2 O 3 -24Al 2 O 3 Nano-agglomeration spraying powder material:
and (3) weighing 750g of the composite nano powder material prepared in the step (1), 30g of a polyvinyl alcohol solution with the mass fraction of 10%, 40g of polystyrene powder, 1700g of distilled water and 4mL of n-butanol in a ball milling tank, and then placing the ball milling tank in a planetary ball mill to perform ball milling for 5 hours at the speed of 380r/min to obtain uniform slurry. Adopting a spray granulation drying process to prepare 50ZrO containing polystyrene pore-forming agent 2 -16Y 2 O 3 -10Yb 2 O 3 -24Al 2 O 3 Nano-agglomeration spraying powder material; finally, sieving the nano-aggregate spray powder to screen to obtain powder material with the particle size of 15-60 mu m for plasma spraying.
And pressing the nano agglomerated powder into a ceramic green body with the diameter of 15mm by using a powder tablet press, carrying out cold isostatic pressing on the ceramic green body, and sintering at 1500 ℃ for 5 hours to prepare the ceramic block. Respectively sintering the ceramic blocks at 1400 ℃ for 75h, 150h and 300h, then cooling to room temperature along with the furnace and taking out. The sintered ceramic block was characterized by SEM and it was found that the grain size and fracture toughness of the ceramic material remained almost unchanged with increasing sintering time at 1400 ℃, showing excellent high temperature sintering resistance, as shown in fig. 3.
Comparative example 1:
comparative example 1 was identical to the experimental procedure of example 3, except that the composition of the powders was different. The powder composition of example 4 was: 71.5ZrO 2 -16Y 2 O 3 -10Yb 2 O 3 -2.5Al 2 O 3 (mol.％)。
Step 1: preparation of 71.5ZrO 2 -16Y 2 O 3 -10Yb 2 O 3 -2.5Al 2 O 3 (mol.%) composite nanopowder material:
weighing 56.3g of aluminum nitrate nonahydrate, 921g of zirconium nitrate pentahydrate, 368g of yttrium nitrate hexahydrate and 280g of ytterbium nitrate hexahydrate powder material in a clean beaker, adding 4000mL of distilled water to prepare a solution with the concentration of 0.75mol/L, heating and stirring to form a transparent solution, and then cooling to room temperature; then dropwise adding the transparent solution into sufficient ammonia water while stirring until white precipitate is completely formed, testing the pH value of the solution containing the white precipitate to be 10, and then filtering and washing for three times to obtain white precipitate; finally, sintering the white precipitate in a muffle furnace at 1100 ℃ for 4 hours to prepare a composite nano powder material;
and 2, step: preparation of 71.5ZrO 2 -16Y 2 O 3 -10Yb 2 O 3 -2.5Al 2 O 3 (mol.%) nanoagglomerated spray powder material:
and (3) weighing 750g of the composite nano powder material prepared in the step (1), 30g of a polyvinyl alcohol solution with the mass fraction of 10%, 40g of polystyrene powder, 1700g of distilled water and 4mL of n-butanol in a ball milling tank, and then placing the ball milling tank in a planetary ball mill to perform ball milling for 5 hours at the speed of 380r/min to obtain uniform slurry. Adopting spray granulation drying process to prepare 71.5ZrO containing polystyrene pore-forming agent 2 -16Y 2 O 3 -10Yb 2 O 3 -2.5Al 2 O 3 (mol.%) nanoagglomerated spray-coated powder material; finally, sieving the nano-aggregate spray powder to screen to obtain powder material with the particle size of 15-60 mu m for plasma spraying.
And pressing the nano agglomerated powder into a ceramic green body with the diameter of 15mm by using a powder tablet press, carrying out cold isostatic pressing on the ceramic green body, and sintering at 1500 ℃ for 5 hours to prepare the ceramic block. Sintering the ceramic blocks at 1400 ℃ for 75h, 150h and 300h respectively, and then cooling the ceramic blocks to room temperature along with a furnace and taking out the ceramic blocks. The sintered ceramic block was characterized by SEM, and it was found that the grain size of the ceramic material significantly increased with the increase of sintering time at 1400 ℃, showing poor high temperature sintering resistance, as shown in fig. 4.
Comparative example 2:
step 1: preparation of 75ZrO 2 -25Y 2 O 3 (mol.%) composite nano powder material
Weighing 1288g of pentahydrate zirconium nitrate powder material and 766.02g of hexahydrate yttrium nitrate powder material in a clean beaker, adding 8000mL of distilled water to prepare a solution with the concentration of 0.5mol/L, heating and stirring to form a transparent solution, and then cooling to room temperature; then dropwise adding the transparent solution into sufficient ammonia water while stirring until white precipitate is completely formed, testing that the pH value of the solution containing the white precipitate is more than 9, and then filtering and washing for three times to obtain white precipitate; finally, sintering the white precipitate in a muffle furnace at 1100 ℃ for 3 hours to prepare a composite nano powder material;
step 2: preparation of 75ZrO 2 -25Y 2 O 3 Nano-agglomeration spraying powder material:
weighing 500g of the composite nano powder material prepared in the step 1, 15g of a polyvinyl alcohol solution with the mass fraction of 10%, 25g of polystyrene powder, 1650g of distilled water and 3mL of n-butyl alcohol in a ball milling tank, and then placing the ball milling tank in a planetary ball mill to perform ball milling for 4 hours at the speed of 400r/min to obtain uniform slurry. 75ZrO prepared by adopting spray granulation drying process and containing polystyrene pore-forming agent 2 -25Y 2 O 3 Nano-agglomeration spraying powder material; finally, sieving the nano-aggregate spray powder to screen to obtain powder material with the particle size of 15-60 mu m for plasma spraying.
The 75ZrO is sprayed by atmosphere plasma 2 -25Y 2 O 3 And preparing a ceramic heat-insulating coating by nano-agglomeration spraying powder material, sintering the prepared ceramic heat-insulating coating at 1400 ℃ for 100 hours, cooling the ceramic heat-insulating coating along with a furnace to room temperature, and taking out the ceramic heat-insulating coating. The sintered ceramic thermal barrier coating was characterized using a Scanning Electron Microscope (SEM) (as shown in fig. 5). Plasma spraying 75ZrO from FIG. 5 2 -25Y 2 O 3 The cross section appearance of the coating after being sintered for 100 hours at 1400 ℃ can be seen, and the plasma spraying is carried out on 75ZrO after being sintered 2 -25Y 2 O 3 The interface between the layers of the coating disappears, the size of columnar crystal is obviously increased, and severe sintering occurs, which shows that 75ZrO 2 -25Y 2 O 3 The coating prepared by nano-agglomeration spraying powder material does not have good sintering resistance at high temperature.
The foregoing is illustrative of the preferred embodiments of the present invention, which is set forth only, and not to be taken as limiting the invention. It will be appreciated by those skilled in the art that many variations, modifications, and equivalents may be made thereto without departing from the spirit and scope of the invention as defined in the claims.
Claims (10)
1. The eutectic toughening sintering-resistant alumina/rare earth doped zirconia ultrahigh-temperature thermal barrier coating spraying material is characterized by comprising the following components: zrO (ZrO) 2 Rare earth oxide RE 2 O 3 、Al 2 O 3 Said ZrO 2 Rare earth oxide RE 2 O 3 、Al 2 O 3 The molar ratio of (A) to (B) is 40-75: 20 to 35:5 to 25.
2. The eutectic toughened and sintering-resistant alumina/rare earth doped zirconia super-high temperature thermal barrier coating spray material as claimed in claim 1, wherein the rare earth oxide RE is 2 O 3 Is one or the combination of two of yttrium oxide and ytterbium oxide.
3. A method for preparing the eutectic toughened anti-sintering alumina/rare earth doped zirconia ultra-high temperature thermal barrier coating spray material according to claim 1 or 2, which is characterized by comprising the following steps:
s1, preparing an alumina-zirconia-rare earth oxide composite nano powder material: mixing aluminum nitrate, zirconium nitrate and rare earth oxide, adding distilled water to prepare a solution, heating and stirring the solution until a transparent solution is formed, then cooling the solution to room temperature, dropwise adding the transparent solution containing aluminum ions, zirconium ions and rare earth ions into ammonia water while stirring the solution until white precipitates are completely formed, and sintering the white precipitates to obtain ZrO 2 -RE 2 O 3 -Al 2 O 3 Compounding nanometer powder material;
s2, preparing the nano-agglomeration spraying powder material of the alumina-zirconia-rare earth oxide: zrO 2 is mixed with 2 -RE 2 O 3 -Al 2 O 3 Ball milling the composite nano powder material, 10 mass percent of polyvinyl alcohol solution, polystyrene powder, distilled water and n-butyl alcohol to obtain uniform slurry, and spray granulating and drying to obtain the polystyrene-containing pore-forming materialThe nano-agglomeration spraying powder material of the agent alumina-zirconia-rare earth oxide is screened by a screen to obtain the spraying material.
4. The preparation method of the eutectic toughening sintering-resistant alumina/rare earth doped zirconia ultrahigh temperature thermal barrier coating spraying material according to claim 3, wherein the concentration of the solution prepared in the step S1 is 0.5-1 mol/L.
5. The method for preparing the eutectic toughened sintering-resistant alumina/rare earth doped zirconia ultrahigh temperature thermal barrier coating spraying material according to claim 3, wherein in the step S1, the sintering temperature is 1000-1100 ℃, and the sintering time is 2-4 h.
6. The method for preparing the eutectic toughened sintering-resistant alumina/rare earth doped zirconia ultrahigh temperature thermal barrier coating spraying material according to claim 3, wherein the mass fraction of polyvinyl alcohol in the polyvinyl alcohol solution in the step S2 is 10%.
7. The preparation method of the eutectic toughening sintering-resistant alumina/rare earth doped zirconia ultrahigh temperature thermal barrier coating spray material according to claim 3, wherein in the step S2, the ball milling speed is 360-400 r/min, and the ball milling time is 3-5 h.
8. The method for preparing the eutectic toughening sintering-resistant alumina/rare earth doped zirconia ultrahigh temperature thermal barrier coating spraying material according to claim 3, wherein ZrO added into the slurry in the step S2 is ZrO 2 -RE 2 O 3 -Al 2 O 3 The composite nano powder material accounts for 30-40% of the solid content by mass, the polyvinyl alcohol solution accounts for 2-4% of the solid content by mass, the polystyrene accounts for 5-10% of the solid content by mass, and the volume of the added n-butyl alcohol is 3-5 mL.
9. The use of the eutectic toughened and sintering-resistant alumina/rare earth doped zirconia ultrahigh temperature thermal barrier coating spray material as claimed in claim 1 or 2 on the hot end part of an advanced combustion turbine engine, characterized in that the alumina/rare earth doped zirconia ultrahigh temperature thermal insulation coating is prepared by spraying the spray powder material by using a plasma spraying technique.
10. The use of the eutectic toughened anti-sintering alumina/rare earth doped zirconia ultrahigh temperature thermal barrier coating spray material as claimed in claim 9, wherein the plasma spray technique comprises atmospheric plasma spray, vacuum plasma spray, low pressure plasma spray, suspension plasma spray.
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