CN113025945A - Preparation method of high-temperature oxidation-resistant rare earth silicate thermal barrier coating on surface of titanium alloy composite material - Google Patents
Preparation method of high-temperature oxidation-resistant rare earth silicate thermal barrier coating on surface of titanium alloy composite material Download PDFInfo
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- 229910001069 Ti alloy Inorganic materials 0.000 title claims abstract description 100
- 239000012720 thermal barrier coating Substances 0.000 title claims abstract description 74
- 229910052761 rare earth metal Inorganic materials 0.000 title claims abstract description 51
- -1 rare earth silicate Chemical class 0.000 title claims abstract description 50
- 230000003647 oxidation Effects 0.000 title claims abstract description 33
- 238000007254 oxidation reaction Methods 0.000 title claims abstract description 33
- 238000002360 preparation method Methods 0.000 title claims abstract description 26
- 239000002131 composite material Substances 0.000 title claims abstract description 18
- 238000000576 coating method Methods 0.000 claims abstract description 30
- 239000000919 ceramic Substances 0.000 claims abstract description 19
- 239000000843 powder Substances 0.000 claims description 86
- 238000005507 spraying Methods 0.000 claims description 44
- 239000011159 matrix material Substances 0.000 claims description 40
- 238000000034 method Methods 0.000 claims description 26
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 24
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 22
- 238000000498 ball milling Methods 0.000 claims description 19
- 238000001035 drying Methods 0.000 claims description 19
- 239000007789 gas Substances 0.000 claims description 17
- 239000002002 slurry Substances 0.000 claims description 17
- 238000002156 mixing Methods 0.000 claims description 14
- 239000008367 deionised water Substances 0.000 claims description 13
- 229910021641 deionized water Inorganic materials 0.000 claims description 13
- 229910052786 argon Inorganic materials 0.000 claims description 12
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 12
- YWYZEGXAUVWDED-UHFFFAOYSA-N triammonium citrate Chemical compound [NH4+].[NH4+].[NH4+].[O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O YWYZEGXAUVWDED-UHFFFAOYSA-N 0.000 claims description 11
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 10
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 10
- 238000005469 granulation Methods 0.000 claims description 10
- 230000003179 granulation Effects 0.000 claims description 10
- 235000010489 acacia gum Nutrition 0.000 claims description 9
- 239000001785 acacia senegal l. willd gum Substances 0.000 claims description 9
- 238000005516 engineering process Methods 0.000 claims description 9
- 230000008569 process Effects 0.000 claims description 9
- 238000007873 sieving Methods 0.000 claims description 9
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 8
- 238000007750 plasma spraying Methods 0.000 claims description 8
- 239000000377 silicon dioxide Substances 0.000 claims description 8
- 238000004140 cleaning Methods 0.000 claims description 7
- 239000011812 mixed powder Substances 0.000 claims description 7
- 238000005488 sandblasting Methods 0.000 claims description 7
- 239000000126 substance Substances 0.000 claims description 7
- 229910052681 coesite Inorganic materials 0.000 claims description 6
- 229910052906 cristobalite Inorganic materials 0.000 claims description 6
- 229910052682 stishovite Inorganic materials 0.000 claims description 6
- 229910052905 tridymite Inorganic materials 0.000 claims description 6
- 229910052593 corundum Inorganic materials 0.000 claims description 3
- 239000010431 corundum Substances 0.000 claims description 3
- 239000004576 sand Substances 0.000 claims description 3
- 229920000642 polymer Polymers 0.000 claims 1
- 239000011248 coating agent Substances 0.000 abstract description 28
- 239000000758 substrate Substances 0.000 abstract description 18
- 239000000463 material Substances 0.000 abstract description 12
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 4
- 230000004048 modification Effects 0.000 abstract description 4
- 238000012986 modification Methods 0.000 abstract description 4
- 239000001301 oxygen Substances 0.000 abstract description 4
- 229910052760 oxygen Inorganic materials 0.000 abstract description 4
- 230000035699 permeability Effects 0.000 abstract description 3
- 230000015572 biosynthetic process Effects 0.000 abstract description 2
- 239000007769 metal material Substances 0.000 abstract description 2
- 230000035939 shock Effects 0.000 description 16
- 239000007921 spray Substances 0.000 description 16
- 239000001257 hydrogen Substances 0.000 description 7
- 229910052739 hydrogen Inorganic materials 0.000 description 7
- 238000010791 quenching Methods 0.000 description 5
- 230000000171 quenching effect Effects 0.000 description 5
- 238000002441 X-ray diffraction Methods 0.000 description 4
- 238000001816 cooling Methods 0.000 description 4
- 150000002431 hydrogen Chemical class 0.000 description 4
- 229910000883 Ti6Al4V Inorganic materials 0.000 description 3
- 239000000956 alloy Substances 0.000 description 3
- 230000003064 anti-oxidating effect Effects 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 238000001878 scanning electron micrograph Methods 0.000 description 3
- 238000003746 solid phase reaction Methods 0.000 description 3
- FIXNOXLJNSSSLJ-UHFFFAOYSA-N ytterbium(III) oxide Inorganic materials O=[Yb]O[Yb]=O FIXNOXLJNSSSLJ-UHFFFAOYSA-N 0.000 description 3
- 241000220479 Acacia Species 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 235000010643 Leucaena leucocephala Nutrition 0.000 description 2
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 2
- 238000007605 air drying Methods 0.000 description 2
- 230000004888 barrier function Effects 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000010220 ion permeability Effects 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 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 description 2
- 239000012071 phase Substances 0.000 description 2
- 238000012216 screening Methods 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 238000010532 solid phase synthesis reaction Methods 0.000 description 2
- 229940075624 ytterbium oxide Drugs 0.000 description 2
- 229910003454 ytterbium oxide Inorganic materials 0.000 description 2
- 238000002679 ablation Methods 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 238000005275 alloying Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000005524 ceramic coating Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000003801 milling Methods 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 150000002910 rare earth metals Chemical class 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 1
- 235000012239 silicon dioxide Nutrition 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 229910052727 yttrium Inorganic materials 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
- C23C4/12—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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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B33/00—Silicon; Compounds thereof
- C01B33/20—Silicates
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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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- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
- C01P2002/72—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
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Abstract
本发明涉及一种钛合金复合材料表面高温抗氧化稀土硅酸盐热障涂层的制备方法，属于金属材料表面改性技术领域。解决现有技术中钛合金热障涂层由于涂层与基体的热膨胀不匹配和界面处易形成热生长氧化物，导致热障涂层与基体的结合稳定性差，TBC易脱落，热震寿命不高的技术问题。本发明的制备方法采用新型稀土硅酸盐(如YxYb2‑xSiO5)作为热障涂层材料，所用的原料稀土硅酸盐的热膨胀系数与钛合金基底具有很好的匹配性，且具有高抗氧化性，低氧气渗透率，热膨胀系数介于NiCoCrAlY和钛合金之间。本发明制备的陶瓷层热障涂层具有良好的高温热稳定性、低热导率、良好的抗氧化能力，适合用作钛合金热端构件的高温热防护热障涂层。
The invention relates to a preparation method of a high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of a titanium alloy composite material, and belongs to the technical field of surface modification of metal materials. Solve the problem that the titanium alloy thermal barrier coating in the prior art has poor bonding stability between the thermal barrier coating and the substrate due to the mismatch of thermal expansion between the coating and the substrate and the easy formation of thermally grown oxides at the interface. high technical issues. The preparation method of the invention adopts a novel rare earth silicate (such as Y x Yb 2-x SiO 5 ) as the thermal barrier coating material, and the thermal expansion coefficient of the raw rare earth silicate used has good matching with the titanium alloy substrate, And it has high oxidation resistance, low oxygen permeability, and thermal expansion coefficient between NiCoCrAlY and titanium alloys. The ceramic layer thermal barrier coating prepared by the invention has good high temperature thermal stability, low thermal conductivity and good oxidation resistance, and is suitable for use as a high temperature thermal protection thermal barrier coating for titanium alloy hot end components.
Description
Technical Field
The invention belongs to the technical field of surface modification of metal materials, and particularly relates to a preparation method of a high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of a titanium alloy composite material.
Background
The titanium alloy material has the advantages of high strength, high hardness, high heat conductivity, low density and the like, and is one of candidate materials with the greatest application prospect on hot end members of aviation, aerospace and weaponry. However, titanium alloy materials are easily oxidized in high-temperature oxidation environments, which greatly limits their application in high-temperature oxidation environments. The anti-oxidation coating prepared on the surface of the titanium alloy can effectively improve the high-temperature anti-oxidation performance of the titanium alloy.
The service temperature of the titanium alloy is not obviously improved from the titanium alloy alloying technology to the alloy surface coating technology, the thermal barrier coating is the current advanced high-temperature thermal protection technology, and can prevent the high-temperature oxidation of the titanium alloy surface and the diffusion of nitrogen and oxygen elements into the titanium alloy when being applied to the titanium alloy surface, thereby enhancing the oxidation resistance of the titanium alloy, thereby obviously improving the service temperature of the titanium alloy and keeping the matrix structure stable for a long time, and the literature reports [ Journal of thermal Spray Technology,2011,20(4):948-957 the YSZ/NiCoCrAlY thermal barrier coating is prepared on the surface of the titanium alloy by adopting an Atmospheric Plasma Spraying (APS) technology, however, the thermal expansion of the YSZ/NiCoCrAlY coating and the titanium alloy substrate is not matched, so that the interface stability of the coating and the titanium alloy substrate is poor, the coating is still easy to fall off, and the thermal shock life of the coating needs to be further improved.
Disclosure of Invention
The invention provides a preparation method of a high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of a titanium alloy composite material, aiming at solving the technical problems that the thermal expansion mismatch between a coating and a substrate and Thermal Growth Oxide (TGO) is easily formed at an interface of a YSZ/MCrAlY (M is Ni and Co) thermal barrier coating in the prior art, so that the bonding stability of the thermal barrier coating and the substrate is poor, TBC is easily shed, and the thermal shock service life is low.
In order to solve the technical problems, the technical scheme of the invention is as follows:
the invention provides a preparation method of a high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of a titanium alloy composite material, which comprises the following steps: and spraying rare earth silicate powder on the titanium alloy matrix to prepare the high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of the titanium alloy composite material.
In the above technical solution, it is preferable that: the rare earth silicate powder has a chemical formula of YxYb2-xSiO5Wherein x is 0-0.6.
In the above technical solution, it is further preferable that: x is 0, 0.2, 0.4 or 0.6.
In the above technical solution, it is preferable that: one specific embodiment of the preparation method is as follows: the method comprises the following steps:
the method comprises the following steps: preparing rare earth silicate powder;
step two: mixing the rare earth silicate powder obtained in the step one with deionized water, ammonium citrate and Arabic gum to obtain rare earth silicate slurry; performing ball milling, sieving and granulation on the rare earth silicate slurry to obtain rare earth silicate spraying powder;
step three: pretreating the titanium alloy matrix to obtain a pretreated titanium alloy matrix;
step four: preparation of coatings using APS technology
And (4) putting the rare earth silicate spraying powder obtained in the step two into a plasma spraying powder feeder, and spraying a rare earth silicate ceramic layer on the pretreated titanium alloy matrix obtained in the step three to obtain the high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of the titanium alloy composite material.
In the above technical solution, it is preferable that: when the rare earth silicate powder has a chemical formula of YxYb2-xSiO5The specific steps of the first step are as follows:
yb is mixed according to the molar ratio of the chemical formula2O3Powder, Y2O3Powder and SiO2Mixing the powders, adding water and zirconia balls into the mixed powder, and placing on a ball millBall milling is carried out for 6-12 h, the obtained slurry is dried, centrifugally ball milled and sieved, the obtained product reacts for 10-12 h at 1400-1500 ℃, and Y is obtainedxYb2-xSiO5And (3) powder.
In the above technical solution, it is preferable that: the ball milling time in the second step is 72 hours; said Y isxYb2-xSiO5The mass ratio of the powder to the deionized water to the ammonium citrate to the arabic gum is 100: (100-150): (0.4-0.8): (1-2).
In the above technical solution, it is further preferable that: said Y isxYb2-xSiO5The mass ratio of the powder to the deionized water to the ammonium citrate to the arabic gum is 100:150:0.8: 2.
in the above technical solution, it is preferable that: the pretreatment process in the third step comprises the following steps: carrying out sand blasting treatment on the surface of the titanium alloy matrix by using corundum sand, then cleaning the titanium alloy matrix in an ultrasonic cleaner by using ethanol, and drying to obtain the pretreated titanium alloy matrix.
In the above technical solution, it is preferable that: in the fourth step, the spraying current is 500-700A, the spraying power is 30-40 kW, the plasma gas is argon gas and hydrogen gas, the argon gas flow is 30-40 SLPM, the hydrogen gas flow is 10-20 SLPM, and the spraying distance is 90-110 mm.
In the above technical solution, it is preferable that: spraying Y in the four stepsxYb2-xSiO5The thickness of the ceramic layer is 100 to 300 μm.
The invention has the beneficial effects that:
the invention provides a preparation method of a high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of a titanium alloy composite material, which adopts novel rare earth silicate (such as Y)xYb2-xSiO5) As thermal barrier coating material, rare earth silicate (such as Y) is used as raw materialxYb2-xSiO5X is 0-0.6), has high oxidation resistance and low oxygen permeability, and has a thermal expansion coefficient between NiCoCrAlY and titanium alloy. Thus converting rare earth silicates (e.g. Y)xYb2- xSiO5) As the titanium alloy surface thermal barrier coating, the problem of poor bonding stability of the TBC and the titanium alloy substrate interface caused by the mismatching of the thermal expansion of the coating and the substrate is effectively solved, so that the bonding strength of the titanium alloy surface TBC and the high-temperature thermal shock service life are remarkably improved.
The invention firstly adopts a solid-phase reaction method to synthesize YxYb2-xSiO5Spray granulation of the synthetic powder followed by preparation of Y by APS techniquexYb2-xSiO5And (4) coating. The rare earth silicate material is synthesized by a solid phase method, and is used as a novel anti-oxidation and anti-ablation thermal protection coating on the surface of the titanium alloy to remarkably improve the bonding strength of a TBC (titanium alloy) on the surface of the titanium alloy, and simultaneously, the 800 ℃ high-temperature water quenching thermal shock service life of the rare earth silicate material is improved by about 35% compared with that of a traditional YSZ/NiCoCrAlY thermal barrier coating and is improved by about 38% compared with that of a single YSZ thermal barrier coating, and experimental results show that the novel rare earth silicate material has important application value for the surface thermal protection of the titanium alloy (Ti6Al4V/TC 4.
The ceramic layer thermal barrier coating prepared by the invention has good high-temperature thermal stability, low thermal conductivity and good oxidation resistance, and is suitable for being used as a high-temperature thermal protection thermal barrier coating of a titanium alloy hot end component.
Drawings
The present invention will be described in further detail with reference to the accompanying drawings and specific embodiments.
FIG. 1 Synthesis of silicate Y by the solid phase method of example 10.4Yb1.6SiO5XRD spectrum and SEM picture of the titanium alloy surface thermal barrier coating.
FIG. 2 is a scanning electron microscope photograph of a thermal barrier coating on the surface of a titanium alloy prepared in example 2 of the present invention, wherein (a) a YSZ/NiCoCrAlY thermal barrier coating; (b) YSZ thermal barrier coating.
FIG. 3 is an XRD pattern of the ceramic powder of the thermal barrier coating prepared in example 3 of the present invention and a scanning electron microscope photograph of the thermal barrier coating prepared on the surface of the titanium alloy, wherein (a) is Yb2SiO5/Y0.2Yb1.8SiO5/Y0.6Yb1.4SiO5XRD pattern of (b) Yb2SiO5Scanning electron microscope photograph of (c)) Is Y0.2Yb1.8SiO5Scanning electron micrograph, and (d) is Y0.6Yb1.4SiO5Scanning electron micrographs.
FIG. 4 is a photograph of the failure of the titanium alloy thermal barrier coating sample in the 800 ℃ water quenching thermal shock test, wherein (a) is YSZ + NiCoCrAlY, (b) is YSZ, and (c) is Yb2SiO5And (d) is Y0.2Yb1.8SiO5And (e) is Y0.4Yb1.6SiO5(f) is Y0.6Yb1.4SiO5。
FIG. 5 is a photograph of a failure cross-section of a titanium alloy thermal barrier coating sample in a 800 ℃ water quenched thermal shock test, wherein (a) is a YSZ/NiCoCrAlY coating, (b) is a YSZ coating, and (c) is a Y coating0.4Yb1.6SiO5And (4) coating.
Detailed Description
The invention provides a preparation method of a high-temperature oxidation-resistant rare earth silicate Thermal Barrier Coating (TBC) on the surface of a titanium alloy (Ti6Al4V/TC4) composite material, which comprises the following steps: and spraying rare earth silicate powder on the titanium alloy matrix to prepare the high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of the titanium alloy composite material.
The chemical formula of the rare earth silicate powder is YxYb2-xSiO5(x is 0 to 0.6) as an example, the preparation process of the preparation method is explained in detail.
The invention provides a preparation method of a high-temperature oxidation-resistant rare earth silicate Thermal Barrier Coating (TBC) on the surface of a titanium alloy (Ti6Al4V/TC4) composite material, which comprises the following steps:
the method comprises the following steps: preparation of YxYb2-xSiO5A powder, wherein x is 0-0.6;
step two: y obtained in the step onexYb2-xSiO5Mixing the powder with deionized water, ammonium citrate, and acacia to obtain YxYb2-xSiO5Slurry of YxYb2-xSiO5Ball-milling, sieving and granulating the slurry to obtain YxYb2-xSiO5Spraying powder;
step three: pretreating the titanium alloy matrix to obtain a pretreated titanium alloy matrix;
step four: preparing coating by APS technology, and mixing Y obtained in the second stepxYb2-xSiO5Putting the spraying powder into a plasma spraying powder feeder, and spraying Y on the pretreated titanium alloy matrix obtained in the step threexYb2-xSiO5And (5) a ceramic layer is formed to obtain the high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of the titanium alloy composite material.
According to the invention, Y is first preparedxYb2-xSiO5Powder of preparation YxYb2-xSiO5The preferable specific steps of the powder are as follows:
yb of2O3Powder, Y2O3Powder and SiO2Mixing the powder according to a molar ratio, adding water and zirconia balls into the mixed powder, carrying out ball milling on the mixed powder for 6-12 h in a ball mill, drying, carrying out centrifugal ball milling and sieving on the obtained slurry, and reacting the obtained product for 10-12 h at 1400-1500 ℃ to obtain Y0.4Yb1.6SiO5Powder; most preferably Yb2O3Powder, Y2O3Powder and SiO2The molar ratio of the powders was 4:1: 5.
According to the invention, Y is obtainedxYb2-xSiO5Mixing the powder with deionized water, ammonium citrate, and acacia to obtain YxYb2-xSiO5Slurry of YxYb2-xSiO5Ball milling is carried out on the slurry, the ball milling time is preferably 72 hours, the slurry passes through a 120 mu m sieve, the sieved slurry is sent into a spray dryer at 100-125 ℃ for spray granulation, so as to obtain spherical powder with good fluidity, the spray dried powder is sieved through a vibrating sieve, and the spray granulated powder with the particle size of 32-100 mu m is selected as APS spraying powder. Preferably said Y is0.4Yb1.6SiO5The mass ratio of the powder to the deionized water to the ammonium citrate to the arabic gum is 100: (100-150): (0.4-0.8): (1-2), most preferably 100:150:0.8: 2.
According to the invention, the titanium alloy substrate is pretreated before sprayingSo that the sprayed coating effect can reach the best, the working requirement under the high-temperature oxidation atmosphere is met, and the pretreatment process specifically comprises the following steps: the surface of the titanium alloy substrate is made of corundum sand (Al) with the granularity of 36 meshes2O3) Carrying out sand blasting treatment, wherein the sand blasting time is preferably 2-5 seconds, so that the surface of the matrix is roughened, and the effect of improving the bonding strength of the coating is achieved; and after sand blasting treatment, cleaning the titanium alloy matrix in an ultrasonic cleaner by using ethanol, removing oil stains and residual fine particle impurities on the surface, naturally drying, and then putting into a drying oven for drying for later use.
According to the invention, Y obtained as described above is used to prepare a coating using APS technologyxYb2-xSiO5Respectively putting the sprayed powder into a plasma spraying powder feeder, and firstly spraying Y on the pretreated titanium alloy matrixxYb2-xSiO5The thickness of the ceramic layer is preferably 100-300 mu m, more preferably 260-286 mu m, and the high-temperature oxidation-resistant thermal barrier coating on the surface of the titanium alloy composite material is obtained.
According to the invention, in the spraying process, the spraying current is 500-700A, the spraying power is 30-40 kW, and the plasma gas is argon (Ar)2) And hydrogen (H)2) Wherein the flow rate of argon gas is 30-40 SLPM, the flow rate of hydrogen gas is 10-20 SLPM, and the spraying distance is 90-110 mm.
According to the invention, the rare earth silicate YxYb2-xSiO5The thermal expansion coefficient of the titanium alloy substrate is about 6.99 ppm/DEG C, has good matching property with the titanium alloy substrate, and has high oxidation resistance and low oxygen permeability. Thus designing a novel YxYb2-xSiO5The oxidation-resistant thermal barrier coating with the ceramic layer structure effectively solves the problem that the coating and the matrix fall off due to thermal expansion mismatch and poor bonding strength, obviously prolongs the thermal shock service life of the thermal barrier coating, and ensures that the coating is not easy to fall off. Meanwhile, the components and the proportion of the coating material can be freely adjusted, the damage degree of the spraying process to the substrate material is lower, and the method is very suitable for the preparation of the high-melting-point ceramic coating and the industrial mass production.
In order to more clearly illustrate the present invention, the following examples are given to further illustrate the present invention, but the present invention is not limited to the following examples.
Example 1
Ytterbium oxide (Yb) is taken according to a molar ratio of 4:1:52O3) Powder, yttrium oxide (Y)2O3) Powder and Silica (SiO)2) Mixing the powder, adding deionized water and zirconia balls into the mixed powder, performing roll ball milling for 12h, taking out the balls after ball milling, drying slurry in a drying oven at 100 ℃, performing rapid centrifugal ball milling on the powder obtained after drying for 10min, and sieving by a 120-micron sieve. The obtained uniformly mixed Yb2O3、Y2O3And SiO2The raw material powder is subjected to solid phase reaction for 12 hours at the high temperature of 1400 ℃ to synthesize high-purity Y0.4Yb1.6SiO5And (3) powder.
Mixing the prepared Y according to the mass ratio0.4Yb1.6SiO5Powder: deionized water: ammonium citrate: mixing Arabic gum at a ratio of 100:150:0.8:2, ball milling for 72h, and sieving with a 120 μm sieve; and (3) carrying out spray granulation on the screened slurry at the temperature of 100 ℃, screening the spray granulation powder by using a vibration sample separation screen, and selecting the spray granulation powder with the particle size of 32-100 mu m as plasma spraying powder.
Carrying out surface sand blasting treatment on the titanium alloy matrix, placing the treated titanium alloy matrix in an ultrasonic cleaner, ultrasonically cleaning the titanium alloy matrix with ethanol, taking out the titanium alloy matrix after cleaning, naturally drying the titanium alloy matrix after air drying, placing the titanium alloy matrix in a 60 ℃ drying oven, and drying the titanium alloy matrix for later use.
The prepared Y is0.4Yb1.6SiO5The powder is fed into high-temperature plasma flame flow generated by a plasma spray gun, and a layer of Y with the thickness of 280 mu m is sprayed on the surface of a substrate0.4Yb1.6SiO5Coating, and naturally cooling to room temperature.
In the spraying process, the spraying current is 550A, the spraying power is 30kW, and the plasma gas used for spraying is argon (Ar)2) And hydrogen (H)2) Wherein the gas flow of argon is 30SLPM, the gas flow of hydrogen is 10SLPM, and the spraying distance is 90 mm.
FIG. 1 shows a ceramic powder Y for a thermal barrier coating prepared in example 1 of the present invention0.4Yb1.6SiO5XRD pattern of the ceramic powder phase and scanning electron microscope photograph of the thermal barrier coating prepared on the surface of the titanium alloy, from which the composition of the ceramic powder phase is Y0.4Yb1.6SiO5And the product is pure; the prepared thermal barrier coating is uniformly distributed, is tightly combined with the matrix, and has a compact ceramic layer structure.
Example 2
Respectively putting the purchased YSZ powder and NiCoCrAlY powder into a plasma spraying powder feeder, firstly, selecting NiCoCrAlY powder, feeding the NiCoCrAlY powder into high-temperature plasma flame flow generated by a plasma spray gun, spraying a NiCoCrAlY coating with the thickness of 100 mu m on the surface of a matrix, and then naturally cooling to room temperature. And then, selecting YSZ powder to be sent into high-temperature plasma flame flow generated by a plasma spray gun, spraying a layer of YSZ coating with the thickness of 280 mu m on the surface of the substrate, and naturally cooling to room temperature.
In the spraying process, the spraying current is 550A, the spraying power is 30kW, and the plasma gas used for spraying is argon (Ar)2) And hydrogen (H)2) Wherein the gas flow of argon is 30SLPM, the gas flow of hydrogen is 10SLPM, and the spraying distance is 90 mm.
The preparation method of the single YSZ thermal barrier coating sample is the same as that of the YSZ thermal barrier coating in example 2.
FIG. 2 is a scanning electron micrograph of a thermal barrier coating on the surface of a titanium alloy prepared in example 2 of the present invention (a) a YSZ/NiCoCrAlY thermal barrier coating; (b) the YSZ thermal barrier coating can be found from the figure that the prepared thermal barrier coating is uniformly distributed, is tightly combined with a substrate and has a compact ceramic layer structure.
Example 3
Ytterbium oxide (Yb) is taken according to the molar ratio of 7:3:102O3) Powder, yttrium oxide (Y)2O3) Powder and Silica (SiO)2) Mixing the powder, adding deionized water and zirconia balls into the mixed powder, performing roll ball milling for 12h, taking out the balls after ball milling, drying slurry in a drying oven at 100 ℃, performing rapid centrifugal ball milling on the powder obtained after drying for 10min, and sieving by a 120-micron sieve. The obtained uniformly mixed Yb2O3、Y2O3And SiO2The raw material powder is in 14High-temperature solid-phase reaction at 00 ℃ for 12h to synthesize high-purity Y0.6Yb1.4SiO5And (3) powder.
Mixing the prepared Y according to the mass ratio0.6Yb1.4SiO5Powder: deionized water: ammonium citrate: mixing Arabic gum at a ratio of 100:150:0.8:2, ball milling for 72h, and sieving with a 120 μm sieve; and (3) carrying out spray granulation on the screened slurry at the temperature of 100 ℃, screening the spray granulation powder by using a vibration sample separation screen, and selecting the spray granulation powder with the particle size of 32-100 mu m as plasma spraying powder.
Carrying out surface sand blasting treatment on the titanium alloy matrix, placing the treated titanium alloy matrix in an ultrasonic cleaner, ultrasonically cleaning the titanium alloy matrix with ethanol, taking out the titanium alloy matrix after cleaning, naturally drying the titanium alloy matrix after air drying, placing the titanium alloy matrix in a 60 ℃ drying oven, and drying the titanium alloy matrix for later use.
The prepared Y is0.6Yb1.4SiO5The powder is fed into high-temperature plasma flame flow generated by a plasma spray gun, and a layer of Y with the thickness of 280 mu m is sprayed on the surface of a substrate0.6Yb1.4SiO5Coating, and naturally cooling to room temperature.
In the spraying process, the spraying current is 550A, the spraying power is 30kW, and the plasma gas used for spraying is argon (Ar)2) And hydrogen (H)2) Wherein the gas flow of argon is 30SLPM, the gas flow of hydrogen is 10SLPM, and the spraying distance is 90 mm.
Two other kinds of thermal barrier ceramic powder (Yb)2SiO5/Y0.2Yb1.8SiO5Powder) preparation method and Y in example 30.6Yb1.4SiO5The powders were prepared in the same manner except that the molar ratio of the reactants added was varied according to the product composition. The preparation method of the titanium alloy surface thermal barrier coating is the same as that of the example 3.
FIG. 3 is a thermal barrier coating ceramic powder (Yb) prepared in example 3 of the present invention2SiO5/Y0.2Yb1.8SiO5/Y0.6Yb1.4SiO5) XRD pattern of the titanium alloy and scanning electron microscope photograph of the thermal barrier coating prepared on the surface of the titanium alloy, and the pure synthesized thermal barrier ceramic powder product can be found from the imageCleaning; the prepared thermal barrier coating is uniformly distributed, is tightly combined with the matrix, and has a compact ceramic layer structure.
The YSZ/NiCoCrAlY, YSZ and Y are respectively prepared on the surface of the titanium alloy by using the embodiment methodxYb2- xSiO5(x is 0/0.2/0.4/0.6) oxidation-resistant thermal barrier coating (samples are correspondingly named as a-f), the prepared titanium alloy surface thermal barrier coating is heated at 800 ℃ for 5min and then subjected to water quenching thermal shock test, the experimental result is shown in table 1, and the sample photo and the section electron microscope photo after thermal shock are shown in fig. 4 and 5.
Table 1 shows the results of the thermal shock life of different thermal barrier coatings on the surface of the titanium alloy composite material after water quenching at 800 ℃ for thermal shock
| a:YSZ+NiCoCrAlY | b:YSZ | c:Yb2SiO5 | d:Y0.2Yb1.8SiO5 | e:Y0.4Yb1.6SiO5 | f:Y0.6Yb1.4SiO5 |
| 210 times | 205 times (x) | 253 times (a) | 269 times | 283 times (twice) | 259 times |
The thermal shock test results prove that: as can be found from fig. 5, the rare earth silicate material as a novel high temperature resistant and oxidation resistant thermal barrier coating material on the surface of the titanium alloy has better high temperature resistance and oxidation ion permeability resistance than a conventional YSZ/NiCoCrAlY thermal barrier coating, reduces the generation of an oxide layer on the surface of the titanium alloy, and has excellent high temperature oxidation resistance and protection performance on the surface of the titanium alloy, and the 800 ℃ water quenching thermal shock life results show that the thermal barrier coatings of the rare earth silicate material have a longer thermal shock life than the conventional thermal barrier coating, although the conventional thermal barrier coating does not fall off, it can be found through the sectional electron microscope photographs of experimental samples that a large number of cracks are generated on the surface of the coating to cause failure of the coating, as shown in fig. 5 and table 1; compared with the traditional YSZ/NiCoCrAlY and single YSZ thermal barrier coatings, the thermal barrier coating using the rare earth silicic acid as the titanium alloy surface has better high temperature resistance, oxidation ion permeability resistance and thermal shock resistance life, the thermal shock life of the optimal silicate material thermal barrier coating is improved by about 35% compared with the traditional YSZ/NiCoCrAlY thermal barrier coating, and is improved by about 38% compared with the single YSZ thermal barrier coating, and the method using the rare earth silicate as the titanium alloy surface thermal protection is an effective method.
It should be understood that the above examples are only for clarity of illustration and are not intended to limit the embodiments. Other variations and modifications will be apparent to persons skilled in the art in light of the above description. And are neither required nor exhaustive of all embodiments. And obvious variations or modifications therefrom are within the scope of the invention.
Claims (10)
1. A preparation method of a high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of a titanium alloy composite material is characterized by comprising the following steps: the method comprises the following steps: and spraying rare earth silicate powder on the titanium alloy matrix to prepare the high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of the titanium alloy composite material.
2. The method according to claim 1, wherein the rare earth silicate powder has a chemical formula of YxYb2-xSiO5Wherein x is 0-0.6.
3. The method of claim 2, wherein x is 0, 0.2, 0.4, or 0.6.
4. The method for preparing a polymer according to any one of claims 1 to 3, comprising the steps of:
the method comprises the following steps: preparing rare earth silicate powder;
step two: mixing the rare earth silicate powder obtained in the step one with deionized water, ammonium citrate and Arabic gum to obtain rare earth silicate slurry; performing ball milling, sieving and granulation on the rare earth silicate slurry to obtain rare earth silicate spraying powder;
step three: pretreating the titanium alloy matrix to obtain a pretreated titanium alloy matrix;
step four: preparation of coatings using APS technology
And (4) putting the rare earth silicate spraying powder obtained in the step two into a plasma spraying powder feeder, and spraying a rare earth silicate ceramic layer on the pretreated titanium alloy matrix obtained in the step three to obtain the high-temperature oxidation-resistant rare earth silicate thermal barrier coating on the surface of the titanium alloy composite material.
5. The method according to claim 4, wherein the rare earth silicate powder has a chemical formula of YxYb2- xSiO5The specific steps of the first step are as follows:
yb is mixed according to the molar ratio of the chemical formula2O3Powder, Y2O3Powder and SiO2Mixing the powder, adding water and zirconia balls into the mixed powder, carrying out ball milling on the mixed powder for 6-12 h in a ball mill, drying, carrying out centrifugal ball milling on the obtained slurry, and sieving to obtain a product, reacting the product for 10-12 h at 1400-1500 ℃ to obtain YxYb2-xSiO5And (3) powder.
6. The preparation method according to claim 5, wherein the ball milling time in the second step is 72 hours; said Y isxYb2-xSiO5The mass ratio of the powder to the deionized water to the ammonium citrate to the arabic gum is 100: (100-150): (0.4-0.8): (1-2).
7. The method according to claim 6, wherein Y isxYb2-xSiO5The mass ratio of the powder to the deionized water to the ammonium citrate to the arabic gum is 100:150:0.8: 2.
8. the preparation method according to claim 5, wherein the pretreatment process in step three is as follows: carrying out sand blasting treatment on the surface of the titanium alloy matrix by using corundum sand, then cleaning the titanium alloy matrix in an ultrasonic cleaner by using ethanol, and drying to obtain the pretreated titanium alloy matrix.
9. The preparation method of claim 5, wherein in the spraying process in the fourth step, the spraying current is 500-700A, the spraying power is 30-40 kW, the plasma gas is argon gas and hydrogen gas, the argon gas flow is 30-40 SLPM, the hydrogen gas flow is 10-20 SLPM, and the spraying distance is 90-110 mm.
10. The method of claim 5, wherein Y is sprayed in step fourxYb2-xSiO5The thickness of the ceramic layer is 100 to 300 μm.
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