CN105648386A - Thermal spraying aluminum oxide-yttrium oxide composite ceramic coating and preparing method thereof - Google Patents
Thermal spraying aluminum oxide-yttrium oxide composite ceramic coating and preparing method thereof Download PDFInfo
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- CN105648386A CN105648386A CN201610091244.4A CN201610091244A CN105648386A CN 105648386 A CN105648386 A CN 105648386A CN 201610091244 A CN201610091244 A CN 201610091244A CN 105648386 A CN105648386 A CN 105648386A
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- 238000005524 ceramic coating Methods 0.000 title claims abstract description 109
- 238000000034 method Methods 0.000 title claims abstract description 42
- 238000007751 thermal spraying Methods 0.000 title claims abstract description 29
- MEWCPXSDLIWQER-UHFFFAOYSA-N aluminum oxygen(2-) yttrium(3+) Chemical compound [O-2].[Y+3].[O-2].[Al+3] MEWCPXSDLIWQER-UHFFFAOYSA-N 0.000 title claims abstract description 24
- RUDFQVOCFDJEEF-UHFFFAOYSA-N yttrium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Y+3].[Y+3] RUDFQVOCFDJEEF-UHFFFAOYSA-N 0.000 claims abstract description 97
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 55
- 229910052751 metal Inorganic materials 0.000 claims abstract description 52
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- 238000005507 spraying Methods 0.000 claims abstract description 40
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- 229910001845 yogo sapphire Inorganic materials 0.000 claims abstract description 25
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 claims abstract description 17
- 229910003158 γ-Al2O3 Inorganic materials 0.000 claims abstract description 15
- 238000011065 in-situ storage Methods 0.000 claims abstract description 10
- 229910019901 yttrium aluminum garnet Inorganic materials 0.000 claims abstract description 8
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims abstract description 6
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- 239000007789 gas Substances 0.000 claims description 36
- 239000000463 material Substances 0.000 claims description 33
- 229910052786 argon Inorganic materials 0.000 claims description 24
- 238000007750 plasma spraying Methods 0.000 claims description 21
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- 238000002360 preparation method Methods 0.000 claims description 14
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- NPXOKRUENSOPAO-UHFFFAOYSA-N Raney nickel Chemical compound [Al].[Ni] NPXOKRUENSOPAO-UHFFFAOYSA-N 0.000 claims description 12
- 239000012159 carrier gas Substances 0.000 claims description 12
- 238000000151 deposition Methods 0.000 claims description 11
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- 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
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
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Classifications
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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
Abstract
The invention relates to a thermal spraying aluminum oxide-yttrium oxide composite ceramic coating and a preparing method thereof. The aluminum oxide-yttrium oxide composite ceramic coating is formed on a metal substrate or formed on a stress transition layer located on the surface of the metal substrate; and the aluminum oxide-yttrium oxide composite ceramic coating comprises an alpha-Al2O3 phase, a gamma-Al2O3 phase, a c-Y2O3 phase, an m-Y2O3 phase and a YxAlyOz phase generated by aluminum oxide and yttrium oxide in situ, wherein YxAlyOz is Y3Al5O12, Y4Al2O9 and/or YAlO3, and the mass ratio of the alpha-Al2O3 phase to the gamma-Al2O3 phase is 1:(2-3). The aluminum oxide-yttrium oxide composite ceramic coating prepared through a thermal spraying process is compact in structure and lower in gas hole ratio. Solid solution between the Al2O3 and Y2O3 is avoided, a YxAlyOz compound can be generated in situ in the spraying process, and the effects of dispersion toughening and phase interface strengthening are achieved; and bonding of interlayer interfaces between coatings is better, the obdurability and the thermal shock resistance are improved.
Description
Technical Field
The invention relates to a thermal spraying aluminum oxide-yttrium oxide composite ceramic coating and a preparation method thereof, belonging to the technical field of wear-resistant ceramic coatings.
Background
The oxide ceramic material has the characteristics of high strength, high hardness, wear resistance, high temperature resistance, oxidation resistance, corrosion resistance and the like, shows better comprehensive performance, has better potential when being applied to harsh wear service working conditions such as high specific pressure (namely high PV value: P is contact pressure and V is friction rate), high temperature, oxygen enrichment, strong thermal shock, strong corrosion and the like as a thermal spraying coating material, can combine the advantages of a metal substrate and the oxide ceramic coating, and is expected to obtain good engineering application2And the like. The addition of the ductile metal phase can release the stress concentration at the tip of the crack, the corresponding crack in the crack tip area is not easy to form, the crack propagation resistance is increased, and the fracture toughness of the material is improved; the addition of the hard ceramic phase can dissipate the crack advancing power by refining the matrix grains and the crack shielding effect, thereby achieving the toughening purpose. The process is simple and easy to implement, the cost is low, and when the parameters such as the type, the size, the content and the like of the particles are properly selected, the toughening effect is more obvious. In order to achieve a good toughening effect,② toughening fiber (or whisker) and dispersing high-strength fiber (or whisker) as the second phase in ceramic matrix, wherein the fiber (or whisker) is used as the first phase to increase the fracture energy and the fiber (or whisker) is used as the second phase to reduce the energy consumption and prevent crack propagation3N4③ phase transformation toughening of crystal whisker, carbon fiber and B fiber, etc. by using tetragonal phase (t phase) ZrO2Martensitic transformation to monoclinic (m-phase) ZrO2④ component or structure gradient toughening, forming gradient material through component or structure change, eliminating macro interface basically, solving the problem of abrupt change of internal performance of material, and relaxing thermal stress.
The four typical ceramic toughening methods have the characteristics and show good toughening effect on ceramic composite blocks, but show obvious limitations when the methods are combined with the thermal spraying process, particularly represented by ①, the grain toughening effect of the ceramic composite blocks is good, and the average grain size of the ceramic composite blocks is submicron or nanometer② toughening of fiber (or whisker) can improve the mechanical properties of the coating, but the aspect ratio is large, and the fiber (or whisker) maintains moderate bonding strength with the substrate, however, during the thermal spraying process, the particles are in a molten or semi-molten state, and the original aspect ratio, surface functionalization and strength of the fiber (or whisker) are difficult to ensure2Or Y2O3Partially stabilized ZrO2(YSZ) may also be used to toughen ceramic coatings. The problems that arise in this way are: ZrO (ZrO)2④ gradient coating toughening usually needs to prepare more single layers for superposition, the thickness of each single layer is limited, and different components or structures need to be controlled, the process is complicated, actual requirements are difficult to meet, and the integral hardness and strength of the gradient coating are not ideal.
The traditional ceramic toughening means is combined with a thermal spraying process, so that the toughness of the oxide ceramic coating is difficult to effectively improve. In single component oxide wear resistant ceramic coatings, Al2O3And Cr2O3The wear resistance of the coating is better than that of ZrO2And (4) coating. Under more severe abrasion working conditions, Al2O3The wear resistance of the coating is superior to that of Cr2O3Coatings, mainly due to the higher thermal conductivity of the former. Therefore, strengthening and toughening studies are currently being directed more to thermal spraying Al2O3The coating mainly comprises ① raw material particles for nanocrystallization, spray granulation of nano Al2O3The mechanical property of the coating obtained by taking the particles as raw materials is superior to that of the traditional micron-sized coating② addition of Metal phase the addition of second phase metals (e.g., Al, Ni, Mo, etc.) increases Al2O3The fracture toughness and the heat conductivity of the coating show better wear resistance, ③ solid solution toughness, more typical Al2O3–TiO2And Al2O3–Cr2O3And (4) preparing the system. TiO 22Low melting point, formed solid solution and partial TiO2Is liable to be in Al2O3The aggregation of the coating grain boundary can improve the internal binding force of the coating sheet and inhibit the propagation of transverse cracks. Al (Al)2O3–Cr2O3The composite coating showed better than single Al2O3The coating has better mechanical, heat conduction and wear resistance. The above-mentioned improved Al2O3The research on the obdurability of the coating has made some progress, but still has some problems that ① has unstable coating nano structure due to high friction heat generated under severe abrasion working conditions, ② nano-structure ceramic coating has more crystal boundaries, has large phonon scattering effect, causes heat conductivity reduction and is not beneficial to application under severe abrasion working conditions, ③ adds metal phase to reduce the hardness and strength of the coating, is not beneficial to service under severe working conditions, and the interface bonding performance of the metal phase and the ceramic matrix is difficult to control, ④ TiO 2 has the defects that2The ⑤ solid solution can appear re-precipitation phenomenon under repeated high and low temperature service environment, which destroys the solid solution structure and performance in the sprayed coating.
Disclosure of Invention
The invention aims to solve the technical problems in the prior art and provides a thermal spraying aluminum oxide-yttrium oxide composite ceramic coating and a preparation method thereof, aiming at improving the compactness, the mechanical property, the heat conduction property, the interlayer bonding property and the wear resistance of the ceramic coating under the severe wear service working conditions of high specific pressure, high temperature, oxygen enrichment, strong thermal shock and the like and avoiding the adverse effects of the traditional nano structure, the addition of a metal second phase and the solid solution effect of a compound on the performance and service life of the ceramic coating under the severe wear conditions.
To achieve the object, the present invention provides an alumina-yttria composite ceramic coating formed on a metal substrate or on a stress transition layer on a surface of the metal substrate, and the alumina-yttria composite ceramic coating includes α -Al2O3Phase, gamma-Al2O3Phase, c-Y2O3Phase, m-Y2O3Phase and Y generated in situ from alumina and yttriaxAlyOzPhase of the YxAlyOzIs Y3Al5O12、Y4Al2O9And/or YAlO3Wherein α -Al2O3Phase with gamma-Al2O3The mass ratio of the phases is 1: (2-3).
The alumina-yttria composite ceramic coating provided by the invention comprises Y generated by alumina and yttria in situxAlyOzPhase of YxAlyOzThe phase can play the role of dispersion toughening and phase interface strengthening, the interface bonding between coating layers is better, the toughness and the thermal shock resistance are improved, the possible adverse effects of the nano coating structure, the metal second phase addition and the solid solution effect on the mechanical property, the microstructure stability and the service life of the ceramic coating under the severe abrasion working conditions of high bearing, high temperature, oxygen enrichment, strong thermal shock and the like can be avoided, and the α -Al in the composite coating of the invention2O3The content of phase is obviously increased, and α -Al2O3The thermal conductivity and the strength of the material are better than those of gamma-Al2O3Simultaneously introduced Y2O3The composite ceramic coating has good heat conductivity, so that the heat conductivity of the composite ceramic coating is improved, the thermal stress generated between the ceramic coating and the metal base material due to the difference of thermal expansion coefficients is reduced, the expansion of microcracks in the coating is relieved, the wear resistance of the ceramic coating under a severe wear service working condition is improved, and the service life of the ceramic coating is prolonged.
Preferably, the α -Al2O3The mass fraction of the phases is 9-24%.
Preferably, said c-Y2O3The mass fraction of the phases is 9-29%, and m-Y2O3And phase with c-Y2O3The mass ratio of the phases is 1: (3-4).
Preferably, Y isxAlyOzThe phase mass fraction is 6-10%.
Preferably, the thickness of the alumina-yttria composite ceramic coating is 250-500 μm.
The invention also provides a preparation method of the alumina-yttria composite ceramic coating, which comprises the following steps:
(1) pretreating the metal base material, including roughening and purifying the surface of the metal base material to be sprayed;
(2) mechanically and uniformly mixing alumina powder and yttrium oxide powder to obtain composite powder;
(3) depositing the composite powder obtained in the step (2) on the surface of the pretreated metal base material obtained in the step (1) by adopting thermal spraying to obtain the aluminum oxide-yttrium oxide composite ceramic coating; or before depositing the composite powder, spraying a stress transition layer on the surface of the pretreated metal substrate obtained in the step (1), and depositing the composite powder obtained in the step (2) on the stress transition layer by thermal spraying to obtain the aluminum oxide-yttrium oxide composite ceramic coating.
Preferably, the metal substrate is stainless steel, alloy or metal matrix composite, the roughened surface roughness Ra of the metal substrate is 5-10 μm, and the stress transition layer is nickel-chromium (NiCr) or nickel-aluminum (NiAl) alloy and has a thickness of 40-100 μm.
Preferably, the mass fraction of the alumina powder in the step (2) is 20-40% of the composite powder, and the particle size is 15-45 μm.
Preferably, the particle size of the yttrium oxide powder in the step (2) is 15 to 45 μm.
Preferably, the thermal spraying in step (3) is plasma spraying, and the plasma spraying process parameters are as follows: plasma gas argon gas flow 40 ~ 50slpm, plasma gas hydrogen gas flow 6 ~ 10slpm, current 630 ~ 690A, power 45 ~ 50kW, powder feeding carrier gas argon gas flow 3 ~ 4slpm, powder feeding rate 30 ~ 40g/min, spraying distance 100 ~ 120 mm. Where slpm is an abbreviation for standard liters per minute.
Preferably, the powder particle size distribution range of the stress transition layer in the step (3) is 35-65 μm, the stress transition layer is sprayed by plasma, and the plasma spraying process parameters are as follows: plasma gas argon gas flow 50 ~ 70slpm, plasma gas hydrogen gas flow 8 ~ 12slpm, current 550 ~ 620A, power 40 ~ 45kW, powder feeding carrier gas argon gas flow 3 ~ 4slpm, powder feeding rate 20 ~ 30g/min, spraying distance 110 ~ 130 mm. Where slpm is an abbreviation for standard liters per minute.
The alumina-yttria composite ceramic coating prepared by the thermal spraying process has compact structure and lower porosity. Al (Al)2O3And Y2O3Does not dissolve in the water, and can generate Y in situ in the spraying processxAlyOzThe compound plays roles of dispersion toughening and phase interface strengthening, the interface bonding between coating layers is good, and the toughness and the thermal shock resistance are improved.
During the spraying process, Y2O3Is favorable for α -Al in the coating2O3Phase stabilization, therefore, α -Al in the alumina-yttria composite ceramic coating phase composition compared to a single alumina coating2O3Phase with gamma-Al2O3The content ratio of the phases is obviously increased, and α -Al2O3The thermal conductivity and the strength of the material are better than those of gamma-Al2O3While Y is2O3The self heat-conducting property is better, which can improve the heat conductivity of the composite ceramic coating and reduce the difference between the ceramic coating and the metal base material due to the thermal expansion coefficientThe generated thermal stress relieves the expansion of microcracks in the coating, improves the wear resistance and the effective service life of the ceramic coating under the harsh wear service working condition.
Drawings
FIG. 1 shows two powder scanning electron microscope morphologies: (a) alumina; (b) yttrium oxide;
FIG. 2 is an X-ray diffraction pattern of the alumina-yttria composite powders and coatings;
FIG. 3 is a scanning electron microscope morphology of polished cross sections of composite ceramic coatings of different yttria content: (a)30 percent; (b)20 percent; (c)40 percent;
FIG. 4 is a cross-sectional compositional analysis of a composite ceramic coating having a yttria content of 30%;
FIG. 5 is a comparison photograph of the alumina coating and the alumina-yttria composite ceramic coating before and after thermal shock (total 40 water quenching times after 30 minutes of heat preservation at 500 ℃): (a) an aluminum oxide coating; (b) an alumina-yttria composite ceramic coating (the mass fraction of yttria is 40%);
FIG. 6 is a graph showing the room temperature thermal conductivity and thermal diffusivity of an alumina coating, an yttria coating, and an alumina-yttria composite ceramic coating (20% by mass yttria);
FIG. 7 is a friction coefficient curve (ring-block wear mode, load 1000N, friction speed 0.84m/s, wear time 60min) with time obtained by respectively pairing the alumina coating and the alumina-yttria composite ceramic coating with graphite and carrying out a high-load wear test;
FIG. 8 is a graph of the respective wear rates of the alumina coating and the alumina-yttria composite ceramic coating (20% by mass yttria) for the coating and graphite in a paired graphite wear test;
FIG. 9 shows the wear surface topography of the alumina coating and the alumina-yttria composite ceramic coating (yttria mass fraction 30%): (a) al (Al)2O3；(b)Al2O3-30wt％Y2O3；
FIG. 10 is a graph of the coefficient of friction over time (ring-block wear mode, load 1000N, friction speed 0.84m/s, wear time 60min) obtained by pairing a composite ceramic coating with 60% yttria content with graphite and performing a high load wear test.
Detailed Description
The following examples further illustrate the invention, it being understood that the following examples are illustrative only and are not limiting of the invention.
The invention uses Al2O3And Y2O3An alumina-yttria composite ceramic coating was prepared for the raw material, and the following example illustrates the preparation method of the alumina-yttria composite ceramic coating.
The pretreatment of the metal substrate may include roughening and cleaning the pre-sprayed surface of the metal substrate. Wherein, the metal substrate can be stainless steel, alloy or metal matrix composite. After the surface of the metal base material is roughened, the surface roughness Ra of the roughened metal base material is 5-10 mu m, and the roughening is beneficial to improving the bonding performance between the spray coating and the metal base material. Then the surface of the metal substrate is purified. As an example, the 2Cr13 stainless steel substrate is selected to be firstly subjected to sand blasting treatment by 20# white corundum sand, the working pressure is 0.4-0.5MPa, then ultrasonic cleaning is carried out for 5 minutes by ethanol, and then the stainless steel substrate is dried by compressed air.
The alumina powder and the yttrium oxide powder are mechanically mixed uniformly to obtain the composite powder for subsequent spraying. Wherein, the mass fraction of the yttrium oxide powder can be 20-40% of the composite powder. Y is2O3Is favorable for α -Al in the coating2O3Stabilisation of the phase, α -Al2O3The thermal conductivity and the strength of the material are better than those of gamma-Al2O3While Y is2O3The composite ceramic coating has good heat conductivity, so that the heat conductivity of the composite ceramic coating is improved, the thermal stress generated between the ceramic coating and the metal base material due to the difference of thermal expansion coefficients is reduced, the expansion of microcracks in the coating is relieved, the wear resistance of the ceramic coating under a severe wear service working condition is improved, and the service life of the ceramic coating is prolonged. When the content of the yttrium oxide is less than 20 percent (such as 0 percent), the effect of improving the performance of the coating cannot be achieved, and when the content of the yttrium oxide exceeds 40 percent (such as 60 percent), the hardness of the composite coating is greatly reduced, so that the composite coating is not beneficial to service under high-load severe wear conditions. The grain size of the yttrium oxide is 15-45 μm, and the grain size of the aluminum oxide powder is 15-45 μm. The proper particle size distribution range is beneficial to ensuring the quality of the sprayed coating. When the particle size is smaller than 15 mu m, the powder transportation fluidity begins to be poor, some fine powder can block the nozzle of a spray gun and randomly jet large agglomerated particles to remain in the coating to induce cracks and holes, the fine powder can be over-melted, a sputtering type spreading morphology can occur when the fine powder is spread and deposited on the surface of a base material, and the bonding strength is poor; when the particle size is larger than 45 mu m, the powder may have insufficient melting, so a large amount of unmelted particles are left in spraying, the bonding inside the coating sheet layer is not good, and the mechanical property and the wear-resisting property of the coating are reduced. The type of the alumina and yttria powder may be, but not limited to, one of a melt-crushing type, an agglomerated type, a spheroidized compact type, and a spray-drying type.
And depositing composite powder on the surface of the pretreated metal substrate by thermal spraying to obtain the aluminum oxide-yttrium oxide composite ceramic coating. The thermal spraying can be, but not limited to, plasma spraying, and explosive spraying or supersonic flame spraying can also be adopted. As an example, the plasma spray process parameters are: plasma gas argon gas flow 40 ~ 50slpm, plasma gas hydrogen gas flow 6 ~ 10slpm, current 630 ~ 690A, power 45 ~ 50kW, powder feeding carrier gas argon gas flow 3 ~ 4slpm, powder feeding rate 30 ~ 40g/min, spraying distance 100 ~ 120 mm. The thickness of the obtained coating can be 250-500 mu m, the selection of the thickness of the coating is beneficial to service under severe abrasion working conditions, the stress accumulation is large in the process of spraying the coating with overlarge thickness, the coating with longer spraying time can be sintered, and the mechanical property and the wear-resisting property of the coating are reduced; the service life of the coating with too small thickness is reduced in the abrasion process, and in addition, the later grinding and polishing processing uniformity is difficult due to the too small thickness.
Or before the composite powder is deposited, spraying a stress transition layer on the surface of the pretreated metal substrate, and depositing the obtained composite powder on the stress transition layer to obtain the aluminum oxide-yttrium oxide composite ceramic coating. The powder particle size distribution range of nickel-chromium (NiCr) or nickel-aluminum (NiAl) alloy in the stress transition layer is 35-65 mu m. The spraying stress transition layer can be, but not limited to, plasma spraying, vacuum plasma spraying, supersonic flame spraying, etc. As an example, the process parameters of plasma spraying are: plasma gas argon gas flow 50 ~ 70slpm, plasma gas hydrogen gas flow 8 ~ 12slpm, current 550 ~ 620A, power 40 ~ 45kW, powder feeding carrier gas argon gas flow 3 ~ 4slpm, powder feeding rate 20 ~ 30g/min, spraying distance 110 ~ 130 mm.
The stress transition layer can be nickel-chromium (NiCr) or nickel-aluminum (NiAl) alloy, and researches show that under the high-load (namely high PV value) composite severe abrasion service condition (which is usually accompanied by high temperature, strong oxidation and large thermal shock), the heat generated by friction increases suddenly, the higher the thermal conductivity of the coating is, the easier the heat is to be transferred to the metal base material, and the heat is radiated to the surrounding environment. The temperature gradient between the friction surface and the metal base material can be further effectively controlled by adding the stress transition layer, so that the thermal stress generated by the difference of the thermal expansion coefficients between the coating and the base material is smaller, and the coating is not easy to crack or peel; on the contrary, if the stress transition layer is not provided, the thermal stress concentration is easy to cause the rapid propagation of micro-cracks in the coating, and the coating is easy to crack or peel off in the fatigue wear process, so that the wear resistance of the coating is greatly reduced. The thickness of the stress transition layer is 40-100 mu m, and the excessive stress accumulation of the thickness is large, so that the abrasion service of the ceramic layer is not facilitated; insufficient thickness causes uneven spraying, the performance of the stress transition layer is reduced, and the stress adjusting effect cannot be fully displayed.
The alumina-yttria composite ceramic coating prepared by the invention is analyzed by X diffraction and comprises α -Al2O3Phase, gamma-Al2O3Phase, c-Y2O3Phase sum m-Y2O3Phase, in addition to Y, formed in situ during thermal spraying from mutually undissolved aluminum oxide and yttrium oxidexAlyOzPhases, e.g. Y3Al5O12(YAG)、Y4Al2O9(YAM) or YAlO3(YAP) equal to α -Al2O3The content of the phases is obviously increased compared with that of a single alumina coating, because Y is sprayed during the spraying process2O3Is favorable for α -Al in the coating2O3And (4) stabilizing the phase. c-Y2O3Phase sum m-Y2O3The total content of phases may be determined by the addition of Y2O3The amount of the raw material powder. In situ generated YxAlyOzThe compound can play a role in dispersion toughening and phase interface strengthening, the interface bonding between coating layers is good, and the toughness and the thermal shock resistance are improved. The adverse effects of the structure of the nano coating, the addition of a metal second phase and the solid solution effect on the mechanical property, the microstructure stability and the service life of the ceramic coating under the harsh abrasion working conditions of high bearing, high temperature, oxygen enrichment, strong thermal shock and the like can be avoided.
The present invention will be described in detail by way of examples. It is also to be understood that the following examples are illustrative of the present invention and are not to be construed as limiting the scope of the invention, and that certain insubstantial modifications and adaptations of the invention by those skilled in the art may be made in light of the above teachings. The specific process parameters and the like of the following examples are also only one example of suitable ranges, i.e., those skilled in the art can select the appropriate ranges through the description herein, and are not limited to the specific values exemplified below.
Example 1
The thermal spraying alumina-yttria composite ceramic coating and the preparation method thereof, the method comprises the following steps:
(1) pretreating a metal substrate comprising: and carrying out roughening and purification treatment on the pre-sprayed surface of the metal substrate. Two 2Cr13 stainless steel substrates: square slices (30mm × 15mm × 1.25 mm); secondly, the circular ring (phi outer diameter is 40mm multiplied by phi inner diameter is 16mm multiplied by 10mm) is subjected to sand blasting treatment by 20# white corundum sand under the working pressure of 0.4-0.5MPa, then is subjected to ethanol ultrasonic cleaning for 5 minutes, and is dried by compressed air. The average value of the surface roughness Ra of the stainless steel base material after pretreatment is 7.32 mu m;
(2) and depositing an aluminum oxide-yttrium oxide composite ceramic coating on the surface of the treated metal substrate by adopting a thermal spraying process. Firstly, alumina powder with the grain diameter of 15-45 mu m and yttrium oxide powder with the grain diameter of 15-45 mu m are mechanically mixed for 48 hours in a roller type manner to obtain uniformly dispersed composite powder, wherein the mass fraction of the yttrium oxide powder is 30%. The alumina powder is of a melt-crushing type, and the yttrium oxide powder is of an agglomerated sintering type (see fig. 1). The phases of the two powders are alpha-Al 2O3 and c-Y2O3 (see FIG. 2). Spraying a nickel-chromium alloy stress transition layer on the surface of a treated 2Cr13 stainless steel base material, wherein the particle size distribution range of alloy powder is 35-65 mu m, and a plasma spraying process is adopted, and the specific parameters are as follows: the plasma gas argon flow is 60slpm, the plasma gas hydrogen flow is 8slpm, the current is 580A, the power is 42kW, the powder feeding carrier gas argon flow is 3slpm, the powder feeding speed is 20g/min, and the spraying distance is 120 mm. In addition to the above atmospheric plasma spraying, vacuum plasma spraying, supersonic flame spraying, or the like may be employed. The thickness of the nickel-chromium alloy layer is 60-80 μm. And then plasma spraying an aluminum oxide-yttrium oxide composite ceramic coating on the surface of the nickel-chromium alloy bonding layer, wherein the spraying process parameters are as follows: the plasma gas argon flow rate is 45slpm, the plasma gas hydrogen flow rate is 9slpm, the current is 650A, the power is 46kW, the powder feeding carrier gas argon flow rate is 4slpm, the powder feeding speed is 35g/min, and the spraying distance is 110 mm. In addition to the above atmospheric plasma spraying, explosion spraying or supersonic flame spraying may be employed. The thickness of the composite ceramic coating is 440-460 mu m. The obtained composite ceramic coating contains alpha-Al 2O3, gamma-Al 2O3, c-Y2O3 and m-Y2O3 phases (see figure 2). Wherein the mass ratio of alpha-Al 2O3 to gamma-Al 2O3 is 1:2, and the mass ratio of alpha-Al 2O3 to gamma-Al 2O3 in the single alumina coating is 1: 9. Therefore, the phase stability of the alpha-Al 2O3 in the alumina-yttria composite ceramic coating prepared by spraying is better, which is beneficial to improving the mechanical property and the heat-conducting property of the coating.
The polished section appearance of the prepared alumina-yttria composite ceramic coating shows that: the porosity of the coating is low, the compactness is high, and the interface among the ceramic coating, the nickel-chromium alloy layer and the stainless steel base material is well combined (see figure 3). The composition analysis showed that Al2O3And Y2O3Y is formed in situ during the spraying process3Al5O12And Y4Al2O9Compound (see FIG. 4) wherein, α -Al2O3The phase mass fraction is 18 percent, and the gamma-Al2O3The phase mass fraction is 45 percent, c-Y2O3The mass fraction of the phase is 22 percent, m-Y2O3The phase mass fraction is 6%, Y3Al5O12Phase mass fraction of 4%, Y4Al2O9The phase mass fraction is 5%. The combination of the coating section morphology and the energy spectrum analysis result proves that: al (Al)2O3And Y2O3The coating layer is not solid-dissolved, and a compound can be generated in situ in the spraying process, so that the effects of dispersion toughening and phase interface strengthening are achieved, the interface bonding between the coating layers is good, and the improvement of the toughness and the thermal shock resistance of the coating layer is facilitated.
Further, the wear resistance of the alumina-yttria composite ceramic coating under the high-load condition is investigated. The abrasion material was graphite block (30mm x 7mm x 6mm) and compared to a single alumina coating using a ring-block abrasion mode (coating deposited on the circumferential outer edge surface of the ring), dry abrasion conditions, load 1000N, abrasion speed 0.84m/s (400 rpm), abrasion time 60 min. The test result shows that: the friction coefficient of the alumina-yttria composite ceramic coating/graphite friction pair is very low, the numerical stability is good, the average value is 0.045, and the average value is obviously superior to that of a single alumina coating (see figure 7). The wear surface topography showed: after abrasion, the surface of the aluminum oxide-yttrium oxide composite ceramic coating hardly sees abrasion marks except graphite phase residues. However, the single alumina coating worn surface developed a visibly white striped wear scar (see fig. 9). In conclusion, the aluminum oxide-yttrium oxide composite ceramic coating has better wear resistance.
Example 2
The thermal spraying alumina-yttria composite ceramic coating and the preparation method thereof, the method comprises the following steps:
(1) pretreating a metal substrate comprising: roughening and purifying the surface of the metal substrate to be sprayed
The metal substrate selection and pretreatment method was the same as in example 1. The surface roughness Ra of the stainless steel substrate after pretreatment was 6.56 μm on average. The square piece sample is used for observing the section appearance and performing a thermal shock test, and the circular ring sample is used for performing a frictional wear test;
(2) depositing an aluminum oxide-yttrium oxide composite ceramic coating on the surface of a treated metal substrate by adopting a thermal spraying process
The preparation method of the selected composite powder is the same as that of the embodiment 1, wherein the difference is that: the mass fraction of the yttrium oxide powder is 40%. Spraying a nickel-chromium alloy stress transition layer on the surface of a treated 2Cr13 stainless steel base material, wherein the particle size distribution range of alloy powder is 35-65 mu m, and a plasma spraying process is adopted, and the specific parameters are as follows: the plasma gas argon flow is 55slpm, the plasma gas hydrogen flow is 9slpm, the current is 600A, the power is 43kW, the powder feeding carrier gas argon flow is 3.5slpm, the powder feeding speed is 22g/min, and the spraying distance is 120 mm. In addition to the above atmospheric plasma spraying, vacuum plasma spraying, supersonic flame spraying, or the like may be employed. The thickness of the nickel-chromium alloy layer is 60-80 μm. And then plasma spraying an aluminum oxide-yttrium oxide composite ceramic coating on the surface of the nickel-chromium alloy bonding layer, wherein the spraying process parameters are as follows: the plasma gas argon flow rate is 47slpm, the plasma gas hydrogen flow rate is 8slpm, the current is 670A, the power is 47kW, the powder feeding carrier gas argon flow rate is 4slpm, the powder feeding speed is 40g/min, and the spraying distance is 115 mm. In addition to the above atmospheric plasma spraying, explosion spraying or supersonic flame spraying may be employed. The thickness of the composite ceramic coating is 420-440 μm. And (3) displaying the polished section morphology of the corresponding coating: the porosity of the coating is low, the compactness is high, and the interface among the ceramic coating, the nickel-chromium alloy layer and the stainless steel base material is well combined (see figure 3).
The prepared alumina-yttria composite ceramic coating is subjected to component analysis, and the analysis shows that α -Al2O3The phase mass fraction is 15 percent, and the gamma-Al2O3The mass fraction of the phase is 37 percent, c-Y2O3The mass fraction of the phase is 29 percent, m-Y2O39% of phase mass fraction, Y3Al5O12Phase mass fraction of 4%, Y4Al2O94% of phase mass fraction, YAlO3The phase mass fraction is 2%. Carrying out a thermal shock test on the alumina coating and the alumina-yttria composite ceramic coating square sample, wherein the specific conditions are as follows: keeping the temperature at 500 ℃ for 30 minutes, and then quenching the mixture with water for 40 times in total. After repeated thermal shock for 40 times, the alumina-yttria composite ceramic coating does not crack or peel. However, the single alumina coating spalled only 6 times of thermal shock, and the spalled area increased significantly after 40 times of thermal shock (see fig. 5). Therefore, the alumina-yttria composite ceramic coating has better thermal shock resistance, which shows that the alumina-yttria composite ceramic coating has higher fracture toughness and bonding strength.
Further, the wear resistance of the alumina-yttria composite ceramic coating under the high-load condition is investigated. The frictional wear test conditions were the same as in example 1. The test result shows that: the friction coefficient of the alumina-yttria composite ceramic coating/graphite friction pair is low, the numerical stability is good, the average value is 0.066, and the average value is obviously superior to that of a single alumina coating (see figure 7).
Example 3
The thermal spraying alumina-yttria composite ceramic coating and the preparation method thereof, the method comprises the following steps:
(1) pretreating a metal substrate comprising: and carrying out roughening and purification treatment on the pre-sprayed surface of the metal substrate. The metal substrate selection and pretreatment method was the same as in example 1. The average value of the surface roughness Ra of the stainless steel base material after pretreatment is 8.19 mu m;
(2) depositing an aluminum oxide-yttrium oxide composite ceramic coating on the surface of a treated metal substrate by adopting a thermal spraying process
The preparation method of the selected composite powder is the same as that of the embodiment 1, wherein the difference is that: the mass fraction of the yttrium oxide powder is 20%. Firstly spraying a nickel-aluminum alloy stress transition layer on the surface of a treated 2Cr13 stainless steel base material, wherein the size distribution range of alloy powder particle is 35-55 mu m, and a plasma spraying process is adopted, and the specific parameters are as follows: the plasma gas argon flow is 65slpm, the plasma gas hydrogen flow is 12slpm, the current is 560A, the power is 45kW, the powder feeding carrier gas argon flow is 3.5slpm, the powder feeding speed is 25g/min, and the spraying distance is 125 mm. In addition to the above atmospheric plasma spraying, vacuum plasma spraying, supersonic flame spraying, or the like may be employed. The thickness of the nickel-aluminum alloy layer is 60 to 80 μm. And then plasma spraying an alumina-yttria composite ceramic coating on the surface of the nickel-aluminum alloy bonding layer, wherein the spraying process parameters are as follows: the plasma gas argon flow rate is 49slpm, the plasma gas hydrogen flow rate is 7slpm, the current is 680A, the power is 48kW, the powder feeding carrier gas argon flow rate is 3.5slpm, the powder feeding speed is 37g/min, and the spraying distance is 105 mm. In addition to the above atmospheric plasma spraying, explosion spraying or supersonic flame spraying may be employed. The thickness of the composite ceramic coating is 440-460 mu m. And (3) displaying the polished section morphology of the corresponding coating: the porosity of the coating is low, the compactness is high, and the interface among the ceramic coating, the nickel-aluminum alloy layer and the stainless steel base material is well combined (see figure 3).
The prepared alumina-yttria composite ceramic coating is subjected to component analysis, and the analysis shows that α -Al2O3The phase mass fraction is 24 percent, and the gamma-Al2O3Phase mass fraction of 53%, c-Y2O3The phase mass fraction is 13 percent, m-Y2O3Phase mass fraction of 4%, Y3Al5O12Phase mass fraction of 2%, Y4Al2O9The phase mass fraction is 4%. The laser scintillation method is used for measuring the room temperature thermal diffusion coefficient and the thermal conductivity of the aluminum oxide coating and the aluminum oxide-yttrium oxide composite ceramic coating, and the data show that: the composite ceramic coating has better thermal conductivity than the single alumina coating (see fig. 6). This will facilitate the service of the coating under harsh conditions.
Further, the wear resistance of the alumina-yttria composite ceramic coating under the high-load condition is investigated. The frictional wear test conditions were the same as in example 1. The test result shows that: the friction coefficient of the alumina-yttria composite ceramic coating/graphite friction pair is low, the numerical stability is good, the average value is 0.078, and the average value is obviously superior to that of a single alumina coating (see figure 7). Meanwhile, the alumina-yttria composite ceramic coating/graphite friction pair showed lower wear rate compared to the alumina coating/graphite friction pair, whether the coating or graphite (see fig. 8).
Comparative example 1
In order to fully illustrate the performance superiority of the thermal spraying alumina-yttria composite ceramic coating of the invention, single Al is also prepared2O3The coating was prepared as a comparative example, the same as example 1, except that: only pure alumina powder is used as the spraying raw material. Al (Al)2O3The thickness of the coating is 440-450 μm, and the thickness of the nickel-chromium alloy stress transition layer is 65-75 μm. The coated grinding rings prepared in example 1, example 2, example 3 and comparative example 1 were respectively matched with graphite blocks of the same material, and the tribological behavior of the coated friction pair under high-load conditions was examined. The frictional wear test method was the same as described in example 1. The results show that: compared with a single alumina coating, the alumina-yttria composite ceramic coating has lower friction coefficient, better friction coefficient stability,The wear rate of the coating and graphite was lower (see fig. 7 and 8). This is due to the fact that the composite ceramic coating has better thermal shock resistance and thermal conductivity (see fig. 5 and 6), which indicates that the toughness of the composite ceramic coating is higher.
Comparative example 2
60% of yttrium oxide powder in the composite powder is selected, and the aluminum oxide-yttrium oxide composite ceramic coating is prepared by thermal spraying, wherein the preparation method refers to example 1. the thickness of the composite ceramic coating is 450-460 mu m, and the thickness of the nickel-chromium alloy stress transition layer is 60-70 mu m. the prepared aluminum oxide-yttrium oxide composite ceramic coating is subjected to component analysis, and analysis shows that α -Al2O3Phase mass fraction of 10%, gamma-Al2O3The phase mass fraction is 27%, c-Y2O3The mass fraction of the phases is 40 percent, m-Y2O3Phase mass fraction of 12%, Y3Al5O12Phase mass fraction of 4%, Y4Al2O94% of phase mass fraction, YAlO3The phase mass fraction was 3% and the coefficient of friction obtained by pairing the composite ceramic coating with graphite was significantly greater under the same wear test conditions, with an average value of 0.235 and less stable values (see figure 10), mainly because the excessive amount of yttria significantly reduced the hardness of the composite ceramic coating. In addition, the coefficient of thermal expansion of yttria is greatly changed along with the increase of temperature, and when the content of yttria is too high, the large coefficient of thermal expansion change can cause the initiation and the propagation of cracks of the phase interface of the coating, which is not beneficial to the improvement of the wear resistance of the coating.
Although the present invention has been described with reference to the preferred embodiments, it is not intended to limit the present invention, and those skilled in the art can make variations and modifications of the present invention without departing from the spirit and scope of the present invention by using the methods and technical contents disclosed above, and therefore, any simple modification, equivalent change and modification made to the above embodiments according to the technical essence of the present invention shall fall within the protection scope of the present invention.
Claims (10)
1. An alumina-yttria composite ceramic coating, wherein the alumina-yttria composite ceramic coating is formed on a metal substrate or on a stress transition layer positioned on the surface of the metal substrate, and the alumina-yttria composite ceramic coating comprises α -Al2O3Phase, gamma-Al2O3Phase, c-Y2O3Phase, m-Y2O3Phase and Y generated in situ from alumina and yttriaxAlyOzPhase of the YxAlyOzIs Y3Al5O12、Y4Al2O9And/or YAlO3Wherein α -Al2O3Phase with gamma-Al2O3The mass ratio of the phases is 1: (2-3).
2. The alumina-yttria composite ceramic coating of claim 1, wherein the α -Al is2O3The mass fraction of the phases is 9-24%.
3. The alumina-yttria composite ceramic coating of claim 1 or 2, wherein c-Y is2O3The mass fraction of the phases is 9-29%, and m-Y2O3And phase with c-Y2O3The mass ratio of the phases is 1: (3-4).
4. The alumina-yttria composite ceramic coating of any one of claims 1-3, wherein Y isxAlyOzThe phase mass fraction is 6-10%.
5. The alumina-yttria composite ceramic coating according to any one of claims 1 to 4, wherein the alumina-yttria composite ceramic coating thickness is 250 to 500 μm.
6. A method for preparing the alumina-yttria composite ceramic coating according to any one of claims 1 to 5, comprising:
(1) pretreating the metal base material, including roughening and purifying the surface of the metal base material to be sprayed;
(2) mechanically and uniformly mixing alumina powder and yttrium oxide powder to obtain composite powder;
(3) depositing the composite powder obtained in the step (2) on the surface of the pretreated metal base material obtained in the step (1) by adopting thermal spraying to obtain the aluminum oxide-yttrium oxide composite ceramic coating; or before depositing the composite powder, spraying a stress transition layer on the surface of the pretreated metal substrate obtained in the step (1), and depositing the composite powder obtained in the step (2) on the stress transition layer by thermal spraying to obtain the aluminum oxide-yttrium oxide composite ceramic coating.
7. The preparation method of claim 6, wherein the metal substrate is stainless steel, alloy or metal matrix composite, the roughened surface roughness Ra of the metal substrate is 5-10 μm, and the stress transition layer is nickel-chromium (NiCr) or nickel-aluminum (NiAl) alloy and has a thickness of 40-100 μm.
8. The preparation method according to claim 6 or 7, wherein the mass fraction of the yttrium oxide powder in the step (2) is 20-40% of the composite powder, the particle size is 15-45 μm, and the particle size of the aluminum oxide powder is 15-45 μm.
9. The production method according to any one of claims 6 to 8, wherein the thermal spraying in the step (3) is plasma spraying, and the plasma spraying process parameters are: plasma gas argon gas flow 40 ~ 50slpm, plasma gas hydrogen gas flow 6 ~ 10slpm, current 630 ~ 690A, power 45 ~ 50kW, powder feeding carrier gas argon gas flow 3 ~ 4slpm, powder feeding rate 30 ~ 40g/min, spraying distance 100 ~ 120 mm.
10. The preparation method according to any one of claims 6 to 9, wherein the stress transition layer in the step (3) has a powder particle size distribution range of 35 to 65 μm, the stress transition layer is sprayed by plasma, and the plasma spraying process parameters are as follows: plasma gas argon gas flow 50 ~ 70slpm, plasma gas hydrogen gas flow 8 ~ 12slpm, current 550 ~ 620A, power 40 ~ 45kW, powder feeding carrier gas argon gas flow 3 ~ 4slpm, powder feeding rate 20 ~ 30g/min, spraying distance 110 ~ 130 mm.
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