CN117658629A - Multi-element composite stable zirconia thermal barrier coating material and preparation method thereof - Google Patents
Multi-element composite stable zirconia thermal barrier coating material and preparation method thereof Download PDFInfo
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- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 title claims abstract description 50
- 239000000463 material Substances 0.000 title claims abstract description 45
- 239000002131 composite material Substances 0.000 title claims abstract description 35
- 239000012720 thermal barrier coating Substances 0.000 title claims abstract description 34
- 238000002360 preparation method Methods 0.000 title claims abstract description 13
- 229910002076 stabilized zirconia Inorganic materials 0.000 claims abstract description 28
- 229910001404 rare earth metal oxide Inorganic materials 0.000 claims abstract description 19
- 229910052761 rare earth metal Inorganic materials 0.000 claims abstract description 15
- 150000002910 rare earth metals Chemical class 0.000 claims abstract description 14
- 239000000126 substance Substances 0.000 claims abstract description 5
- 229910010413 TiO 2 Inorganic materials 0.000 claims abstract description 3
- 239000000843 powder Substances 0.000 claims description 40
- 230000004888 barrier function Effects 0.000 claims description 32
- 238000000498 ball milling Methods 0.000 claims description 26
- 238000001035 drying Methods 0.000 claims description 22
- 239000000919 ceramic Substances 0.000 claims description 20
- 229910010293 ceramic material Inorganic materials 0.000 claims description 18
- 238000005245 sintering Methods 0.000 claims description 17
- 239000008367 deionised water Substances 0.000 claims description 14
- 229910021641 deionized water Inorganic materials 0.000 claims description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 14
- 229910052751 metal Inorganic materials 0.000 claims description 13
- 239000002184 metal Substances 0.000 claims description 13
- 239000007921 spray Substances 0.000 claims description 13
- 238000000034 method Methods 0.000 claims description 12
- 238000002156 mixing Methods 0.000 claims description 12
- 239000000243 solution Substances 0.000 claims description 12
- 238000005406 washing Methods 0.000 claims description 12
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 10
- 239000002244 precipitate Substances 0.000 claims description 10
- 239000002243 precursor Substances 0.000 claims description 10
- 238000005507 spraying Methods 0.000 claims description 10
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 8
- 235000011114 ammonium hydroxide Nutrition 0.000 claims description 8
- 238000005469 granulation Methods 0.000 claims description 8
- 230000003179 granulation Effects 0.000 claims description 8
- 239000011259 mixed solution Substances 0.000 claims description 8
- 238000004448 titration Methods 0.000 claims description 8
- 238000007750 plasma spraying Methods 0.000 claims description 7
- 239000011268 mixed slurry Substances 0.000 claims description 6
- 230000007935 neutral effect Effects 0.000 claims description 6
- 239000002002 slurry Substances 0.000 claims description 6
- 239000006228 supernatant Substances 0.000 claims description 6
- 230000008569 process Effects 0.000 claims description 5
- 239000002202 Polyethylene glycol Substances 0.000 claims description 4
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 4
- 229920002125 Sokalan® Polymers 0.000 claims description 4
- 239000011324 bead Substances 0.000 claims description 4
- 238000005119 centrifugation Methods 0.000 claims description 4
- 239000002270 dispersing agent Substances 0.000 claims description 4
- 238000010285 flame spraying Methods 0.000 claims description 4
- 239000011521 glass Substances 0.000 claims description 4
- 239000004584 polyacrylic acid Substances 0.000 claims description 4
- 229920001223 polyethylene glycol Polymers 0.000 claims description 4
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 4
- 238000003756 stirring Methods 0.000 claims description 4
- 239000000758 substrate Substances 0.000 claims description 4
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 3
- 229910045601 alloy Inorganic materials 0.000 claims description 3
- 239000000956 alloy Substances 0.000 claims description 3
- 229910017604 nitric acid Inorganic materials 0.000 claims description 3
- QAOWNCQODCNURD-UHFFFAOYSA-N sulfuric acid Substances OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 3
- 238000005303 weighing Methods 0.000 claims description 3
- CMIHHWBVHJVIGI-UHFFFAOYSA-N gadolinium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Gd+3].[Gd+3] CMIHHWBVHJVIGI-UHFFFAOYSA-N 0.000 claims description 2
- 229910044991 metal oxide Inorganic materials 0.000 claims description 2
- 150000004706 metal oxides Chemical class 0.000 claims description 2
- 238000012216 screening Methods 0.000 claims description 2
- 238000009413 insulation Methods 0.000 abstract description 6
- 229910017493 Nd 2 O 3 Inorganic materials 0.000 abstract description 3
- 238000010923 batch production Methods 0.000 abstract description 2
- 230000000052 comparative effect Effects 0.000 description 13
- 238000000576 coating method Methods 0.000 description 12
- 239000011248 coating agent Substances 0.000 description 11
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 7
- 239000007789 gas Substances 0.000 description 7
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- 238000005524 ceramic coating Methods 0.000 description 4
- 239000013078 crystal Substances 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- 229910052786 argon Inorganic materials 0.000 description 3
- 238000001816 cooling Methods 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 230000008018 melting Effects 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 229910000601 superalloy Inorganic materials 0.000 description 3
- 229910052777 Praseodymium Inorganic materials 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 238000007749 high velocity oxygen fuel spraying Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 230000002035 prolonged effect Effects 0.000 description 2
- 230000000630 rising effect Effects 0.000 description 2
- 238000001878 scanning electron micrograph Methods 0.000 description 2
- 230000035939 shock Effects 0.000 description 2
- 238000007873 sieving Methods 0.000 description 2
- LDXJRKWFNNFDSA-UHFFFAOYSA-N 2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-1-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]ethanone Chemical compound C1CN(CC2=NNN=C21)CC(=O)N3CCN(CC3)C4=CN=C(N=C4)NCC5=CC(=CC=C5)OC(F)(F)F LDXJRKWFNNFDSA-UHFFFAOYSA-N 0.000 description 1
- YLZOPXRUQYQQID-UHFFFAOYSA-N 3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-1-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]propan-1-one Chemical compound N1N=NC=2CN(CCC=21)CCC(=O)N1CCN(CC1)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F YLZOPXRUQYQQID-UHFFFAOYSA-N 0.000 description 1
- 229910002441 CoNi Inorganic materials 0.000 description 1
- 230000008859 change Effects 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
- 230000007547 defect Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 229910021645 metal ion Inorganic materials 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
- 238000004321 preservation Methods 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 230000009466 transformation Effects 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
- GBNDTYKAOXLLID-UHFFFAOYSA-N zirconium(4+) ion Chemical compound [Zr+4] GBNDTYKAOXLLID-UHFFFAOYSA-N 0.000 description 1
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- Compositions Of Oxide Ceramics (AREA)
- Coating By Spraying Or Casting (AREA)
Abstract
The invention discloses a multielement composite stable zirconia thermal barrier coating material and a preparation method thereof, comprising a thermal barrier coating material, wherein the chemical formula of the thermal barrier coating material is (Zr) 1‑x B x )O 2 ‑yA 2 O 3 Wherein x is the content of doped tetravalent B element, y is the mass percent of doped trivalent rare earth oxide, i.e. the mass percent of trivalent rare earth oxide is y%; wherein x is more than or equal to 0.1 and less than or equal to 0.3, y is more than or equal to 10 and less than or equal to 25; the trivalent rare earth oxide A 2 O 3 Is Gd 2 O 3 、Yb 2 O 3 、Nd 2 O 3 、Pr 2 O 3 、Sm 2 O 3 、Er 2 O 3 、Dy 2 O 3 Any four or five of (a); the tetravalent oxide BO 2 Is TiO 2 、HfO 2 、CeO 2 、MoO 2 Any two or three of (c). The composite rare earth stabilized zirconia thermal barrier coating material has the advantages of low thermal conductivity, high bonding strength, good heat insulation performance, long thermal cycle life and the like, is reliable in preparation process and stable in performance, is suitable for large-scale batch production, and has good popularization prospect in the heat insulation protection field of hot end components such as gas turbines, aeroengines and the like.
Description
Technical Field
The invention relates to the technical field of path high-temperature thermal barrier materials, in particular to a multi-component composite stable zirconia thermal barrier coating material and a preparation method thereof.
Background
The inlet temperature of the turbine of the heavy gas turbine is high, the temperature reaches more than 1400 ℃, the gas temperature of the advanced military gas turbine even reaches 1500-1800 ℃, and the super-high temperature makes the operation environment of the hot end component of the gas turbine very bad. The nickel-based superalloy adopted by the common high-temperature component base material has the tolerance temperature limit of about 1100 ℃ and cannot meet the application requirements of the existing gas turbine or aeroengine. Thermal Barrier Coatings (TBCs) are composite coatings composed of a metallic bond coat and a ceramic layer with good heat resistance and thermal insulation. The surface temperature of the heated part is reduced mainly by isolating the heated substrate from the high-temperature medium, the preparation mode is not limited by the shape of the heated end component, and the mechanical property of the substrate material is hardly influenced. Therefore, preparing the thermal barrier coating on the surface of the high-temperature component is the first choice for improving the temperature tolerance of the component economically and effectively.
The thermal barrier coating material is required to be provided with: high melting point, high temperature phase stability, low thermal conductivity, high chemical stability, high thermal expansion coefficient, sintering resistance, etc. Zirconia ceramics have the advantages of relatively low thermal conductivity, high melting point, high thermal expansion coefficient and the like, and are therefore used as the preferred material of the thermal barrier ceramic layer. However, pure zirconia has three crystal structures, and the crystal structures are transformed at different temperatures, so that the volume change generates large internal stress, and the coating material generates cracks to fail. The research shows that the yttria partially stabilized zirconia (6% -8% YSZ) has good thermal cycle, high melting point, low thermal conductivity and other properties, and is considered to be the most ideal ceramic layer material at present. However, when the temperature is higher than 1200 ℃, the YSZ coating is easy to generate the problems of tetragonal phase-to-monoclinic phase transformation, sintering and the like, so that the coating falls off, fails and the like, and cannot meet the service requirement of higher temperature. Therefore, research and development of a novel high-performance zirconia thermal barrier ceramic coating material is needed, the thermal conductivity is further reduced, the phase stability and sintering resistance are improved, the service life is prolonged, and the higher-temperature service requirement of a hot end component of a gas turbine is met, so that a multi-element composite stable zirconia thermal barrier coating material is needed.
Disclosure of Invention
The invention aims to provide a multielement composite stable zirconia thermal barrier coating material with the advantages of low heat conductivity, stable high-temperature phase, long thermal cycle life and the like.
In order to achieve the above purpose, the invention is implemented according to the following technical scheme:
the thermal barrier coating material comprises tetravalent B element and trivalent rare earth oxide, and has a chemical formula of (Zr 1-x B x )O 2 -yA 2 O 3 2, wherein x is the content of doped tetravalent B element and y is doped trivalentThe mass percentage of rare earth oxide is that x is more than or equal to 0.1 and less than or equal to 0.3, y is more than or equal to 10 and less than or equal to 25, and the grain diameter of the thermal barrier coating material is 25-75 mu m. .
Further, the oxide BO of tetravalent B element 2 Is TiO 2 、HfO 2 、CeO 2 、MoO 2 Any two or more of (a) and (b).
Further, the trivalent rare earth oxide A2O3 is any four or more of Gd2O3, yb2O3, nd2O3, pr2O3, sm2O3, er2O3 and Dy2O 3.
In another aspect, a multi-component composite stabilized zirconia thermal barrier coating includes a metallic bond coat and a thermal barrier ceramic layer including a tetravalent element B and a trivalent rare earth oxide, the thermal barrier ceramic layer having the formula (Zr 1-x B x )O 2 -yA 2 O 3 Wherein x is the content of doped tetravalent B element, y is the mass percentage of doped trivalent rare earth oxide, namely the mass percentage of trivalent rare earth oxide is y, wherein x is more than or equal to 0.1 and less than or equal to 0.3, y is more than or equal to 10 and less than or equal to 25, the metal bonding layer comprises one or more of CoNi CrAlY, N iCoCrAlY or N iCoCrAl TaY, the thickness of the metal bonding layer is 100-200 mu m, and the metal bonding is prepared on an alloy substrate by adopting supersonic flame spraying; and adopting atmospheric plasma spraying to prepare the surface thermal barrier ceramic layer on the surface of the metal bonding layer.
Further, the atmospheric plasma spraying process parameters are as follows: the flow rate of argon is 35-45L/min, the flow rate of hydrogen is 8-15L/min, and the flow rate of nitrogen is 15-25L/min; the current is 500-650A, the working voltage is 60-80V, the spraying distance is 110-150 mm, the moving speed of the spray gun is 650-1000 mm/min, and the powder feeding speed is 30-50 g/min. The thickness of the surface thermal barrier zirconia ceramic layer is 300-1000 mu m.
In another aspect, a method of preparing a multi-component composite stabilized zirconia thermal barrier coating material includes the steps of:
1) Four or more rare earth oxides A 2 O 3 Two or more tetravalent metal oxides BO 2 With ZrOC l 2 ·8H 2 O is pressed(0.1-0.3): (10-25) weighing, dissolving oxide in diluted concentrated nitric acid or concentrated sulfuric acid, and adding ZrOCl 2 ·8H 2 O is dissolved in deionized water;
2) Mixing the two solutions, adding a polyethylene glycol dispersing agent, and stirring with a glass rod to obtain a clear mixed solution;
3) Under the ultrasonic vibration environment, reversely titrating the mixed solution into an ammonia water solution to form colloidal precipitate, keeping the PH value of the ammonia water solution to be more than or equal to 10 in the titration process, and standing for 24 hours after the titration is completed;
4) Centrifuging and washing the colloidal precipitate with deionized water at a centrifugal speed of 5000-8000 r/min until the pH value of the supernatant after centrifugation is neutral, washing with absolute ethyl alcohol, and drying in an oven to obtain precursor powder;
5) Sintering the precursor powder for 5-8 hours in an air environment at 1200-1400 ℃ to obtain the composite rare earth stabilized zirconia thermal barrier ceramic material;
6) Carrying out wet ball milling and crushing on the composite rare earth stabilized zirconia thermal barrier ceramic material to obtain slurry, wherein the ball milling medium is absolute ethyl alcohol, and the ball milling bead material is zirconia;
7) Placing the slurry into a drying box for drying to obtain powder, wherein the drying temperature is 80-100 ℃ and the drying time is 15-20 h;
8) Adding the dried powder into a ball mill for mixing to obtain mixed slurry;
9) Carrying out centrifugal spray granulation on the mixed slurry to obtain agglomerated powder;
10 And (3) sintering, crushing and screening the agglomerated powder to obtain the multi-component composite stable zirconia thermal barrier ceramic material spraying powder.
Further, in the step (6), the ball milling rotating speed is 400-600 r/min, and the ball milling time is 20-30 h.
Further, in the step (8), the rotation speed of the ball milling is 300-500 r/min, and the ball milling mixing time is 15-25 h.
Further, 15 to 30wt.% of deionized water and 3 to 6wt.% of polyacrylic acid and 2 to 5wt.% of polyvinyl alcohol are added in the step (8).
Further, in step (9), the centrifugal rotational speed at the time of centrifugal spray granulation: 15000-20000 rpm, air inlet temperature: 250-320 ℃, and the air outlet temperature is: 100-150 ℃, and the feeding rate is as follows: 30-45 rpm.
Further, in the step (10), the sintering temperature is 1200-1400 ℃, and the sintering heat preservation time is 2-6 h.
The beneficial effects of the invention are as follows:
compared with the prior art, the invention has the following technical effects:
the composite rare earth stabilized zirconia thermal barrier coating material has the advantages of low thermal conductivity, high bonding strength, good heat insulation performance, long thermal cycle life and the like, is reliable in preparation process and stable in performance, is suitable for large-scale batch production, and has good popularization prospect in the heat insulation protection field of hot end components such as gas turbines, aeroengines and the like.
Drawings
FIG. 1 is an XRD curve of a multi-component composite stabilized zirconia thermal barrier ceramic material prepared in example 1 and example 3 of the present invention.
FIG. 2 is an SEM image of a multi-component composite stabilized zirconia thermal barrier ceramic material powder prepared in example 1 of the present invention;
FIG. 3 is an SEM image of a multi-component composite stabilized zirconia thermal barrier ceramic material powder prepared in example 3 of the present invention;
Detailed Description
The invention is further described below in the following description of specific embodiments, which are presented for purposes of illustration and description, but are not intended to be limiting.
As shown in fig. 1, example 1:
(Zr 0.85 Ce 0.1 T i 0.05 )O 2 -5.2Gd 2 O 3 -5.6Yb 2 O 3 -4.8Nd 2 O 3 -4.5Pr 2 O 3 the thermal barrier ceramic material and the spraying powder comprise the following steps:
1) Pressing the buttonWeighing Ti and O according to stoichiometric ratio 2 (purity 99.99%), ceO 2 (purity 99.99%), gd 2 O 3 (purity 99.99%), yb 2 O 3 (purity 99.99%), nd 2 O 3 (99.99％)、Pr 2 O 3 (99.99%) is dissolved in diluted concentrated nitric acid and mixed and stirred evenly until clear, zrOCl is weighed according to the stoichiometric ratio 2 ·8H 2 O powder is dissolved in deionized water and stirred uniformly;
2) Mixing the two clear solutions, adding a polyethylene glycol dispersing agent, and stirring with a glass rod to obtain a clear mixed solution;
3) Under the ultrasonic vibration environment, reversely titrating the mixed solution into an ammonia water solution to form colloidal precipitate, keeping the PH value of the ammonia water solution to be more than or equal to 10 in the titration process, and standing for 24 hours after the titration is completed;
4) Centrifuging and washing the colloidal precipitate with deionized water at a centrifugal speed of 5000-8000 r/min until the pH value of the supernatant after centrifugation is neutral, washing with absolute ethyl alcohol, and drying in an oven to obtain precursor powder;
5) Centrifuging and washing the colloidal precipitate with deionized water at 8000r/min until the pH value of the supernatant is neutral, washing with absolute ethyl alcohol, and drying in an oven at 80deg.C to obtain precursor powder;
6) Heating the precursor powder to 1200 ℃ at a temperature rising speed of 5 ℃ for sintering, and keeping the sintering temperature for 6 hours to obtain (Zr) 0.85 Ce 0.1 T i 0.05 )O 2 -5.2Gd 2 O 3 -5.6Yb 2 O 3 -4.8Nd 2 O 3 -4.5Pr 2 O 3 A thermal barrier ceramic material.
7) The prepared (Zr) 0.85 Ce 0.1 T i 0.05 )O 2 -5.2Gd 2 O 3 -5.6Yb 2 O 3 -4.8Nd 2 O 3 -4.5Pr 2 O 3 The materials are subjected to wet ball milling and crushing, the ball milling medium is absolute ethyl alcohol, the ball milling beads are made of zirconia, the ball milling rotating speed is 450r/min, and the ball milling time is 24 hours.
8) And (3) placing the slurry obtained by ball milling in a drying box for drying, wherein the drying temperature is 180 ℃ and the drying time is 15 hours.
9) Adding 15wt.% of deionized water, 4wt.% of polyacrylic acid and 3wt.% of polyvinyl alcohol into the dried powder, placing the mixture into a ball mill for mixing, wherein the ball mill rotating speed is 400r/min, and the ball mill mixing time is 20h.
10 And (3) carrying out centrifugal spray granulation on the obtained mixed slurry to obtain agglomerated powder. Centrifugal rotational speed at centrifugal spray granulation: 18000 rpm, inlet air temperature: 300 ℃, air outlet temperature: 100 ℃, feeding rate: 32rpm.
11 Sintering the agglomerated powder at 1400 ℃ for 3 hours. Then crushing and sieving to obtain the (Zr) 0.85 Ce 0.1 T i 0.05 )O 2 -5.2Gd 2 O 3 -5.6Yb 2 O 3 -4.8Nd 2 O 3 -4.5Pr 2 O 3 Spraying powder with particle size of 25-75 microns.
Example 2
(Zr) 0.85 Ce 0.1 T i 0.05 )O 2 -5.2Gd 2 O 3 -5.6Yb 2 O 3 -4.8Nd 2 O 3 -4.5Pr 2 O 3 The thermal barrier coating comprises a metal bonding layer and a thermal barrier ceramic layer.
And spraying a N i Co17Cr12A l 0.5Y metal bonding layer on the GH4145 nickel-based superalloy plate by adopting supersonic flame spraying HVOF, wherein the thickness of the coating is 100 mu m.
Preparation of the (Zr) on the surface of the metallic bond layer by atmospheric plasma spraying 0.85 Ce 0.1 T i 0.05 )O 2 -5.2Gd 2 O 3 -5.6Yb 2 O 3 -4.8Nd 2 O 3 -4.5Pr 2 O 3 The surface thermal barrier ceramic layer comprises the following technical parameters of atmospheric plasma spraying: argon flow is 40L/min, hydrogen flow is 10L/min, and nitrogen flow is 15L/min; the current is 580A, the working voltage is 72V, the spraying distance is 120mm, the moving speed of the spray gun is 800mm/min, the powder feeding speed is 40g/min, the thickness of the thermal barrier zirconia ceramic layer is 500 mu m,
example 3:
low-thermal-conductivity long-life composite rare earth stabilized zirconia thermal barrier ceramic material (Zr) 0.89 Hf 0.06 T i 005 )-4.9La 2 O 3 -4.5Sm 2 O 3 -5.3Er 2 O 3 -5.2Dy 2 O 3 The method comprises the following steps:
1) Weighing HfO according to stoichiometric ratio 2 (purity 99.99%), T iO 2 (purity 99.99%), la 2 O 3 (purity 99.99%), nd 2 O 3 (purity 99.99%), sm 2 O 3 (purity 99.99%), er 2 O 3 (99.99％)、Dy 2 O 3 (99.99%) is dissolved in concentrated sulfuric acid and mixed and stirred uniformly until clear, zrOC l is weighed according to the stoichiometric ratio 2 ·8H 2 O powder is dissolved in deionized water and stirred uniformly;
2) Mixing the two clear solutions, adding a polyethylene glycol dispersing agent, and stirring with a glass rod to obtain a clear mixed solution;
3) Under the ultrasonic vibration environment, reversely titrating the mixed solution into an ammonia water solution to form colloidal precipitate, keeping the PH value of the ammonia water solution to be more than or equal to 10 in the titration process, and standing for 24 hours after the titration is completed;
4) Centrifuging and washing the colloidal precipitate with deionized water at a centrifugal speed of 5000-8000 r/min until the pH value of the supernatant after centrifugation is neutral, washing with absolute ethyl alcohol, and drying in an oven to obtain precursor powder;
5) Centrifuging and washing the colloidal precipitate with deionized water at 8000r/min until the pH value of the supernatant is neutral, washing with absolute ethyl alcohol, and drying in an oven at 80deg.C to obtain precursor powder;
6) Heating the precursor powder to 1200 ℃ at a temperature rising speed of 5 ℃ for sintering, and keeping the sintering temperature for 6 hours to obtain (Zr) 0.89 Hf 0.06 T i 005 )-4.9La 2 O 3 -4.5Sm 2 O 3 -5.3Er 2 O 3 -5.2Dy 2 O 3 Composite rare earth stabilized zirconiaA thermal barrier ceramic material.
7) The prepared (Zr) 0.89 Hf 0.06 T i 005 )-4.9La 2 O 3 -4.5Sm 2 O 3 -5.3Er 2 O 3 -5.2Dy 2 O 3 The materials are subjected to wet ball milling and crushing, the ball milling medium is absolute ethyl alcohol, the ball milling beads are made of zirconia, the ball milling rotating speed is 450r/min, and the ball milling time is 24 hours.
8) And (3) placing the slurry obtained by ball milling in a drying box for drying, wherein the drying temperature is 180 ℃ and the drying time is 15 hours.
9) Adding 15wt.% of deionized water, 4wt.% of polyacrylic acid and 3wt.% of polyvinyl alcohol into the dried powder, placing the mixture into a ball mill for mixing, wherein the ball mill rotating speed is 400r/min, and the ball mill mixing time is 20h.
10 And (3) carrying out centrifugal spray granulation on the obtained mixed slurry to obtain agglomerated powder. Centrifugal rotational speed at centrifugal spray granulation: 18000 rpm, inlet air temperature: 300 ℃, air outlet temperature: 100 ℃, feeding rate: 32rpm.
11 Sintering the agglomerated powder at 1400 ℃ for 3 hours. Then crushing and sieving to obtain the (Zr) 0.89 Hf 0.06 T i 005 )-4.9La 2 O 3 -4.5Sm 2 O 3 -5.3Er 2 O 3 -5.2Dy 2 O 3 Spraying powder with particle size of 25-75 microns.
Example 4:
(Zr) 0.89 Hf 0.06 T i 005 )-4.9La 2 O 3 -4.5Sm 2 O 3 -5.3Er 2 O 3 -5.2Dy 2 O 3 The thermal barrier coating comprises a metal bonding layer and a thermal barrier ceramic layer.
And spraying a N i Co17Cr12A l 0.5Y metal bonding layer on the GH4145 nickel-based superalloy plate by adopting supersonic flame spraying HVOF, wherein the thickness of the coating is 100 mu m.
Preparation of the (Zr) on the surface of the metallic bond layer by atmospheric plasma spraying 0.89 Hf 0.06 T i 005 )-4.9La 2 O 3 -4.5Sm 2 O 3 -5.3Er 2 O 3 -5.2Dy 2 O 3 The surface thermal barrier ceramic layer comprises the following technical parameters of atmospheric plasma spraying: argon flow is 40L/min, hydrogen flow is 10L/min, and nitrogen flow is 15L/min; the current is 580A, the working voltage is 75V, the spraying distance is 120mm, the moving speed of the spray gun is 850mm/min, the powder feeding speed is 42g/min, the thickness of the thermal barrier zirconia ceramic layer is 500 mu m,
comparative example 1:
with ZrO available on the market 2 -8Y 2 O 3 The rare earth stabilized zirconia ceramic powder material is tested for thermal conductivity and thermal expansion coefficient.
Comparative example 2:
using example 1ZrO 2 -8Y 2 O 3 Rare earth stabilized zirconia ceramic powder, 500 μm thick ZrO was prepared by the method of example 2 2 -8Y 2 O 3 Rare earth stabilized zirconia thermal barrier ceramic coatings.
Comparative example 3:
the difference from example 1 is that a two-element rare earth oxide stabilized zirconia material will be prepared using the method of example 1: zrO (ZrO) 2 -4.8％Nd 2 O 3 -4.5％Pr 2 O 3 Ceramic material and spray powder;
comparative example 4:
the difference from example 2 is that a two-element rare earth oxide stabilized zirconia coating will be prepared using the method of example 2: zrO (ZrO) 2 -4.8％Nd 2 O 3 -4.5％Pr 2 O 3 A ceramic coating;
comparative example 5:
the difference from example 3 is that a four-element rare earth oxide stabilized zirconia material ZrO will be prepared by the method of example 3 2 -4.9La 2 O3-4.5Sm 2 O 3 -5.3Er 2 O 3 -5.2Dy 2 O 3 Ceramic material and spray powder;
comparative example 6:
the difference from example 4 is that the method of example 4 is used to prepare four-element rare earth oxygenA carbide stabilized zirconia coating: zrO (ZrO) 2 -4.9La 2 O3-4.5Sm 2 O 3 -5.3Er 2 O 3 -5.2Dy 2 O 3 A ceramic coating;
as shown in fig. 2 and 3, the rare earth stabilized zirconia ceramic materials prepared in the above examples and comparative examples were tested for thermal conductivity at 1100 c, thermal expansion coefficient, and water-cooling thermal cycle life of the coating, and the results are shown in table 1. It can be seen that A prepared by the present invention 3+ 、B 4+ The thermal conductivity of the multi-element composite rare earth stabilized zirconia ceramic material is less than or equal to 1.0W/(m.times.K), which is far lower than that of comparative examples 1, 3 and 5, and the thermal expansion coefficient is more than 11.0.times.10 -6 K -1 Is greater than comparative 1, comparative 3 and comparative 5. Meanwhile, the water-cooling thermal cycle life of the thermal barrier coating is also longer than that of comparative examples 2, 4 and 6. The comprehensive data indicate A 3+ 、B 4+ The multielement composite stable zirconia greatly reduces the thermal conductivity of the zirconia, increases the thermal expansion coefficient of the material, is closer to that of the Ni high-temperature alloy of the matrix material, and is beneficial to prolonging the thermal cycle life of the material.
Table 1 shows the thermal conductivities, thermal expansion coefficients, and the numbers of water-cooling thermal cycles at 1100℃of examples 1 to 4 and comparative examples 1 to 6.
According to the invention, the ZrO2 crystal lattice is distorted by doping trivalent rare earth elements to form more point defects, so that the bond length of X-O bonds is increased, the population is reduced, the crystal lattice vibration frequency is reduced, phonon scattering is aggravated, the thermal diffusion coefficient of the material is reduced, the thermal conductivity is reduced, and the heat insulation performance of the coating material is improved. However, the length of the X-O bond becomes larger, which causes the reduction of the thermal expansion coefficient and reduces the thermal shock resistance of the coating. For this purpose, the strength of the X-O bond is lowered by substituting a tetravalent metal ion equivalent to the zirconium ion, therebyThe thermal expansion coefficient is improved, the thermal shock resistance of the coating is enhanced, and the service life of the material is prolonged. The A is 3+ 、B 4+ The thermal conductivity of the multi-element composite stable zirconia thermal barrier ceramic material at 1100 ℃ is less than or equal to 1.0W/(m.times.K), and the thermal expansion coefficient is more than 11.0 multiplied by 10 -6 K -1 。
The foregoing description of the preferred embodiments of the invention is not intended to limit the invention to the precise form disclosed, and any such modifications, equivalents, and alternatives falling within the spirit and scope of the invention are intended to be included within the scope of the invention.
Claims (10)
1. A multi-element composite stable zirconia thermal barrier coating material is characterized in that the thermal barrier coating material comprises tetravalent B element and trivalent rare earth oxide, and the chemical formula of the thermal barrier coating material is (Zr) 1-x B x )O 2 -yA 2 O 3 And 2, wherein x is the content of doped tetravalent B element, y is the mass percentage of doped trivalent rare earth oxide, x is more than or equal to 0.1 and less than or equal to 0.3, y is more than or equal to 10 and less than or equal to 25, and the grain size of the thermal barrier coating material is 25-75 mu m.
2. The multi-component composite stabilized zirconia thermal barrier coating material according to claim 1, wherein said oxide BO of tetravalent B element 2 Is TiO 2 、HfO 2 、CeO 2 、MoO 2 Any two or more of (a) and (b).
3. The multi-component composite stabilized zirconia thermal barrier coating material and the preparation method thereof according to claim 1, wherein the trivalent rare earth oxide A2O3 is any four or more of Gd2O3, yb2O3, nd2O3, pr2O3, sm2O3, er2O3 and Dy2O 3.
4. A multi-element composite stable zirconia thermal barrier coating is characterized by comprising a metal bonding layer and a thermal barrier ceramic layer, wherein the thermal barrier ceramic layer comprises tetravalent B element and trivalent rare earth oxide, and the chemical formula of the thermal barrier ceramic layer is (Zr 1-x B x )O 2 -yA 2 O 3 Wherein x is the content of doped tetravalent B element, y is the mass percentage of doped trivalent rare earth oxide, x is more than or equal to 0.1 and less than or equal to 0.3, y is more than or equal to 10 and less than or equal to 25, the metal bonding layer comprises one or more of CoNiCrAlY, niCoCrAlY or NiCoCrAlTaY, the thickness of the metal bonding layer is 100-200 mu m, and the metal bonding is prepared on an alloy substrate by adopting supersonic flame spraying; and adopting atmospheric plasma spraying to prepare the surface thermal barrier ceramic layer on the surface of the metal bonding layer.
5. A preparation method of a multielement composite stable zirconia thermal barrier coating material is characterized in that,
1) Four or more rare earth oxides A 2 O 3 Two or more tetravalent metal oxides BO 2 With ZrOCl 2 ·8H 2 O is as follows (0.1-0.3): (10-25) weighing, dissolving oxide in diluted concentrated nitric acid or concentrated sulfuric acid, and adding ZrOCl 2 ·8H 2 O is dissolved in deionized water;
2) Mixing the two solutions, adding a polyethylene glycol dispersing agent, and stirring with a glass rod to obtain a clear mixed solution;
3) Under the ultrasonic vibration environment, reversely titrating the mixed solution into an ammonia water solution to form colloidal precipitate, keeping the PH value of the ammonia water solution to be more than or equal to 10 in the titration process, and standing for 24 hours after the titration is completed;
4) Centrifuging and washing the colloidal precipitate with deionized water at a centrifugal speed of 5000-8000 r/min until the pH value of the supernatant after centrifugation is neutral, washing with absolute ethyl alcohol, and drying in an oven to obtain precursor powder;
5) Sintering the precursor powder for 5-8 hours in an air environment at 1200-1400 ℃ to obtain the composite rare earth stabilized zirconia thermal barrier ceramic material;
6) Carrying out wet ball milling and crushing on the composite rare earth stabilized zirconia thermal barrier ceramic material to obtain slurry, wherein the ball milling medium is absolute ethyl alcohol, and the ball milling bead material is zirconia;
7) Placing the slurry into a drying box for drying to obtain powder, wherein the drying temperature is 80-100 ℃ and the drying time is 15-20 h;
8) Adding the dried powder into a ball mill for mixing to obtain mixed slurry;
9) Carrying out centrifugal spray granulation on the mixed slurry to obtain agglomerated powder;
10 And (3) sintering, crushing and screening the agglomerated powder to obtain the multi-component composite stable zirconia thermal barrier ceramic material spraying powder.
6. The multi-component composite stabilized zirconia thermal barrier coating material and the preparation method thereof according to claim 5, wherein the ball milling rotation speed in the step (6) is 400-600 r/min, and the ball milling time is 20-30 h.
7. The multi-component composite stabilized zirconia thermal barrier coating material and the preparation method thereof according to claim 5, wherein the rotational speed of the ball milling in the step (8) is 300-500 r/min, and the ball milling mixing time is 15-25 h.
8. The multi-component composite stabilized zirconia thermal barrier coating material according to claim 5, wherein 15 to 30wt.% deionized water and 3 to 6wt.% polyacrylic acid and 2 to 5wt.% polyvinyl alcohol are added in the mass thereof in the step (8).
9. The multiple composite stabilized zirconia thermal barrier coating material of claim 5, wherein the centrifugal rotational speed at which the centrifugal spray granulation is performed in step (9): 15000-20000 rpm, air inlet temperature: 250-320 ℃, and the air outlet temperature is: 100-150 ℃, and the feeding rate is as follows: 30-45 rpm.
10. The multi-component composite stabilized zirconia thermal barrier coating material of claim 5, wherein in step (10) the sintering temperature is 1200-1400 ℃ and the sintering holding time is 2-6 hours.
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