CN116639988A - Thermal barrier coating material with perovskite structure and preparation method thereof - Google Patents

Thermal barrier coating material with perovskite structure and preparation method thereof Download PDF

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Publication number
CN116639988A
CN116639988A CN202310539216.4A CN202310539216A CN116639988A CN 116639988 A CN116639988 A CN 116639988A CN 202310539216 A CN202310539216 A CN 202310539216A CN 116639988 A CN116639988 A CN 116639988A
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coating material
barrier coating
thermal barrier
valence
perovskite structure
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CN202310539216.4A
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娄晓杰
乔文婧
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Xian Jiaotong University
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Xian Jiaotong University
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Priority to CN202310539216.4A priority Critical patent/CN116639988A/en
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Abstract

The application discloses a thermal barrier coating material with perovskite structure and a preparation method thereof, wherein the chemical composition of the thermal barrier coating material is (A) 1‑x M x )(B 1‑y N y )O 3 Belongs to ABO 3 A perovskite structure; x is more than or equal to 0 and less than or equal to 1; y is more than or equal to 0 and less than or equal to 1; m and N are additive elements, M is in A bit, N is in B bit; the valence state of the element at the A position is +1 valence, +2 valence or +3 valence, and the valence state of the element at the B position is +2 valence, +3 valence, +4 valence, +5 valence or +6 valence. The thermal barrier coating material has low thermal expansion coefficient, low thermal conductivity, extremely high Vickers hardness and elastic modulusAn amount of; can be applied to the surfaces of equipment working in high-temperature environments such as aero turbine engines, gas turbine blades and the like.

Description

Thermal barrier coating material with perovskite structure and preparation method thereof
Technical Field
The application belongs to the technical field of high-temperature protective coatings, and relates to a ceramic thermal barrier coating material and a preparation method thereof.
Background
The thermal barrier coating material has very important application in the fields of industrial manufacture, military national defense, aerospace, aviation and the like. For example, for an aeroengine, its high pressure turbine needs to withstand thermal shock from ultra-high temperature and high velocity gas, which places extremely high demands on its thermal barrier coating material. The traditional engine thermal barrier coating mostly adopts yttrium-doped zirconia-based ceramic materials (such as 8% yttrium-doped zirconia, which is abbreviated as 8 YSZ). However, as the temperature increases, the performance of zirconia-based ceramic materials rapidly decreases. And is embodied by oxidation of the material, an increase in thermal conductivity, and thus failure of the thermal barrier coating. In addition, the temperature before the turbine of the four-generation aero-engine reaches 1600 ℃ at present, and the future temperature possibly exceeds 2000 ℃, which is the temperature which is not bearable by the existing thermal barrier coating materials at present. Therefore, the search for thermal barrier coating materials with better performance, lower cost and higher working temperature has become the key to developing the next generation of high-performance aeroengines.
Disclosure of Invention
Aiming at the defects existing in the prior art, the application aims to provide a thermal barrier coating material with a perovskite structure and a preparation method thereof, and the thermal barrier coating material has the following characteristics of Al 2 O 3f /Al 2 O 3 The ceramic matrix composite material has matched thermal expansion coefficient, very compact structure, low heat conductivity, extremely high Vickers hardness and elastic modulus.
In order to solve the technical problems, the application adopts the following technical scheme:
a thermal barrier coating material with perovskite structure has a chemical composition formula (A) 1-x M x )(B 1-y N y )O 3 X is more than or equal to 0 and less than or equal to 1; y is more than or equal to 0 and less than or equal to 1; belongs to ABO 3 A perovskite structure;
m and N are additive elements, M is in A bit, N is in B bit; the valence state of the A-site element is +1 valence, +2 valence or +3 valence, and the valence state of the B-site element is +2 valence, +3 valence, +4 valence, +5 valence or +6 valence;
a and M are selected from one or more of the following elements: ba. Sr, K, na, bi, ca, li, la, pb;
b and N are selected from one or more of the following elements: zr, ti, sn, hf, mg, nb, ta, Y, sm, sc, ce, al, fe, mn, pr, co, nd, eu, V, mo, W, si.
The application also comprises the following technical characteristics:
specifically, the raw materials of the thermal barrier coating material are oxides of all constituent elements, and the purity of all the raw materials is higher than 99%.
Specifically, the thermal barrier coating material is Ba (Zr 0.2 Ti 0.2 Sn 0.2 Hf 0.2 Nb 0.2 )O 3 。
Specifically, the raw materials of the thermal barrier coating material comprise BaCO 3 Powder, zrO 2 Powder, tiO 2 Powder, snO 2 Powder, hfO 2 Powder and Nb 2 O 5 And (5) powder.
The preparation method of the thermal barrier coating material with the perovskite structure comprises the following steps:
weighing the raw materials according to the proportion in the chemical composition formula; sequentially performing ball milling, presintering, granulating, tabletting, forming and sintering to obtain the thermal barrier coating material with the perovskite structure.
Specifically, the ball milling speed was 400 rpm, and the ball milling time was 24 hours.
Specifically, the burn-in temperature was 1350 ℃ in an air atmosphere, and the burn-in time was 3 hours.
Specifically, the sintering temperature was 1650 ℃ in an air atmosphere, and the sintering time was 2 hours.
The thermal barrier coating material prepared by the preparation method of the thermal barrier coating material with the perovskite structure is applied to surface coating materials of high-temperature environment working equipment of aviation turbine engines and gas turbines.
Compared with the prior art, the application has the following technical effects:
(1) The material of the application has a perovskite structure and is used for the first time in the aspect of thermal barrier coating.
(2) The thermal barrier coating material of the application has the following characteristics of Al 2 O 3f /Al 2 O 3 The ceramic matrix composite material has matched thermal expansion coefficient, very compact structure, low heat conductivity, extremely high Vickers hardness and elastic modulus.
(3) The average thermal expansion coefficient of the thermal barrier coating of the application at 25-1400 ℃ is 9.00 multiplied by 10 -6 Heat conductivity at 1.974 W.m -1 ·K -1 (1200 ℃ C.); the vickers hardness was 11.82GPa.
(4) The preparation method of the application is to sinter the ceramics by a simple sintering process; the prepared perovskite ceramic has the advantage of simple structure.
(5) The application has stable thermal performance, and the thermal expansion coefficient of the sample is equal to that of Al along with the increase of temperature 2 O 3f /Al 2 O 3 The ceramic matrix composites are almost equal, the thermal conductivity is kept at a lower level, and the ceramic matrix composite has the potential to replace the most mainstream thermal barrier coating material 8YSZ at present.
(6) The preparation method is simple, has high preparation efficiency and product qualification rate, and has good application popularization; the reagents and materials of the application are commercially available; the thermal barrier coating material has stable performance and is environment-friendly.
(7) The principle of the application for reducing the thermal conductivity of ceramic materials has the possibility of being expanded to other materials. Based on the principle, the ceramic material of the optimal thermal barrier coating which is applied to the technical field of high-temperature protective coatings and has all the performances satisfied is found.
Drawings
FIG. 1 is a schematic diagram of a thermal barrier coating material system of the present application.
Fig. 2 is a theta-2 theta scan of a material prepared in accordance with an embodiment of the present application.
FIG. 3 shows a schematic view of the present application (A) 1-x M x )(B 1-y N y )O 3 Schematic of the coefficient of thermal expansion of the ceramic.
FIG. 4 shows a schematic diagram of the present application (A) 1-x M x )(B 1-y N y )O 3 The thermal diffusivity and thermal conductivity of the ceramic are schematically shown.
FIG. 5 shows a schematic view of the present application (A) 1-x M x )(B 1-y N y )O 3 Vickers hardness of the ceramic is schematically shown.
Detailed Description
The application provides a thermal barrier coating material with a perovskite structure and a preparation method thereof, wherein the chemical composition of the thermal barrier coating material is (A) 1-x M x )(B 1-y N y )O 3 Belongs to ABO 3 A perovskite structure; x is more than or equal to 0 and less than or equal to 1; y is more than or equal to 0 and less than or equal to 1;
m and N are additive elements, M is in A bit, N is in B bit; the valence state of the element at the A position is +1 valence, +2 valence or +3 valence, and the valence state of the element at the B position is +2 valence, +3 valence, +4 valence, +5 valence or +6 valence;
a and M are selected from one or more of the following elements: ba. Sr, K, na, bi, ca, li, la, pb;
b and N are selected from one or more of the following elements: zr, ti, sn, hf, mg, nb, ta, Y, sm, sc, ce, al, fe, mn, pr, co, nd, eu, V, mo, W, si;
the additive elements M, N may be additive elements of the same valence or may be composed of combinations of elements of different valence (e.g. may be used(average valence is 2+) substitution A 2+ A site; can also use +.>(average valence 4+) substitution B 4+ A site). The following table lists the a, B bit elements and related parameters:
table 1A, B bit elements and related parameters
The material of the application is A, B, M, N oxide (99 percent);
the preparation method of the application comprises the following steps: standard solid phase sintering process; the thermal barrier coating material with the perovskite structure is synthesized and sintered for 3 hours in an air environment at 1350 ℃ and sintered for 2 hours in an air environment at 1650 ℃ to obtain the thermal barrier coating material with the perovskite structure.
The shape and size of the resulting thermal barrier coating material sample was a disk of 12.7mm diameter and 2mm thickness.
The following specific embodiments of the present application are provided, and it should be noted that the present application is not limited to the following specific embodiments, and all equivalent changes made on the basis of the technical scheme of the present application fall within the protection scope of the present application.
Example 1:
the embodiment provides a thermal barrier coating material with a perovskite structure and a preparation method thereof, wherein the chemical composition of the thermal barrier coating material is Ba (Zr) 0.2 Ti 0.2 Sn 0.2 Hf 0.2 Nb 0.2 )O 3 ；
The preparation raw materials of this example are: baCO 3 Powder, zrO 2 Powder, tiO 2 Powder, snO 2 Powder, hfO 2 Powder and Nb 2 O 5 And (5) powder.
The preparation steps of this example include:
BaCO is carried out 3 Powder, zrO 2 Powder, tiO 2 Powder, snO 2 Powder, hfO 2 Powder and Nb 2 O 5 Ball milling is carried out at the speed of 400 rpm for 24 hours, presintering is carried out for 3 hours in an air environment at 1350 ℃, pelleting is carried out, tabletting molding is carried out, sintering is carried out for 2 hours in an air environment at 1650 ℃, and the thermal barrier coating material with the perovskite structure is obtained.
Characterization of the properties:
after obtaining the sample of the material according to the examples of the application, it was subjected to structural and performance tests. During testing, the surface of the sample is polished, and graphite is sprayed on the sample to test the thermal conductivity.
The thermal performance test method comprises the following steps: the thermal expansion coefficient was measured by a TMA 402F3 thermal expansion instrument. Thermal conductivity was measured using a TPS 2200 laser thermal conductivity meter.
The mechanical property test method comprises the following steps: the vickers hardness and modulus of elasticity were measured using LECOAMH43 nanoindentation test system from the american lacca company.
FIG. 1 is a schematic diagram of a thermal barrier coating structure system, 1- (A) 1-x M x )(B 1-y N y )O 3 A thermal barrier coating; a 2-TGO layer; 3-Al 2 O 3f /Al 2 O 3 A ceramic base layer; 4-matrix.
Fig. 2 is a theta-2 theta scan of the present example, and it can be seen that the prepared ceramics all have a perovskite single-phase structure, and no second phase occurs.
As shown in fig. 3, the deformation according to the embodiment of the present application varies with temperature (fig. 3 (a)), and the thermal expansion coefficient varies with temperature (fig. 3 (b)). It can be seen that in the range of 25℃to 1400℃the average thermal expansion coefficient is 9.70X10 -6 Per DEG C, illustrating the presence of Al for turbine blades in accordance with embodiments of the present application 2 O 3f /Al 2 O 3 Ceramic matrix composites have similar coefficients of thermal expansion.
FIG. 4 shows the variation of thermal diffusivity and thermal conductivity with temperature according to an embodiment of the present application, wherein FIG. 4 (a) shows the variation of thermal diffusivity with temperature, FIG. 4 (b) shows the variation of reciprocal of thermal diffusivity with temperature, and FIG. 4 (c) shows the variation of thermal conductivity with temperature; it can be seen that the thermal diffusivity decreases with increasing temperature. Taking the reciprocal of the thermal diffusivity, according to the formulaA slope and an intercept of the reciprocal thereof are obtained according to non-patent document 1: tian, z.; lin, C.; zheng, l.; sun, l.; li, J; wang, J., defect-mediated multiple-enhancement of phonon scattering and decrement of thermal conductivity in (Y) x Yb 1-x ) 2 SiO 5 The larger the intercept, the larger the concentration of point defects, which are phonon scattering centers, and the more centers, the more energy losses, and thus the mean free path of phonons and the thermal conductivity of the material, are known. In addition, as the temperature increases, the heat radiation effect of the material becomes obvious, and the thermal conductivity of the material is also reduced. The ceramic prepared by the application has the thermal conductivity of 2.77-W m within the temperature range of 25-1200 DEG C -1 K -1 The ceramic of the present application is illustrated to have extremely low thermal conductivity.
FIG. 5 shows the measured Vickers hardness and elastic modulus at room temperature for the examples of the present application. It can be seen that the ceramic prepared by the application has extremely high Vickers hardness (13.13 GPa) and elastic modulus of 210.89GPa, which indicates that the embodiment of the application has extremely good mechanical properties.
According to the application (A) 1-x M x )(B 1-y N y )O 3 Ceramics, which have unique combination properties of low thermal expansion coefficient, low thermal conductivity, high vickers hardness, and the like, have potential to be widely used as surface coating materials on equipment surfaces operating in high temperature environments such as aeroturbine engines and gas turbine blades, for example, modern aeroturbine engines, gas turbines for power generation, marine gas turbines, high temperature furnace liners, high-end automobile engines, integrated circuits, and precision instruments.

Claims (9)

1. A thermal barrier coating material with a perovskite structure is characterized in that the chemical composition formula of the thermal barrier coating material is (A 1-x M x )(B 1-y N y )O 3 X is more than or equal to 0 and less than or equal to 1; y is more than or equal to 0 and less than or equal to 1; belongs to ABO 3 A perovskite structure;
m and N are additive elements, M is in A bit, N is in B bit; the valence state of the A-site element is +1 valence, +2 valence or +3 valence, and the valence state of the B-site element is +2 valence, +3 valence, +4 valence, +5 valence or +6 valence;
a and M are selected from one or more of the following elements: ba. Sr, K, na, bi, ca, li, la, pb;
b and N are selected from one or more of the following elements: zr, ti, sn, hf, mg, nb, ta, Y, sm, sc, ce, al, fe, mn, pr, co, nd, eu, V, mo, W, si.
2. The thermal barrier coating material with a perovskite structure of claim 1, wherein the raw material of the thermal barrier coating material is an oxide of each constituent element, and the purity of each raw material is higher than 99%.
3. The thermal barrier coating material with perovskite structure of claim 1, wherein the thermal barrier coating material is Ba (Zr 0.2 Ti 0.2 Sn 0.2 Hf 0.2 Nb 0.2 )O 3 。
4. As claimed inA thermal barrier coating material with a perovskite structure as claimed in claim 3, wherein the raw material of the thermal barrier coating material comprises BaCO 3 Powder, zrO 2 Powder, tiO 2 Powder, snO 2 Powder, hfO 2 Powder and Nb 2 O 5 And (5) powder.
5. A method of producing a thermal barrier coating material having a perovskite structure as claimed in claim 2 or 4, comprising the steps of:
weighing the raw materials according to the proportion in the chemical composition formula; sequentially performing ball milling, presintering, granulating, tabletting, forming and sintering to obtain the thermal barrier coating material with the perovskite structure.
6. The method for preparing a thermal barrier coating material with a perovskite structure according to claim 5, wherein the ball milling speed is 400 rpm and the ball milling time is 24 hours.
7. The method for preparing a thermal barrier coating material having a perovskite structure according to claim 5, wherein the pre-firing time is 3 hours in an air environment at 1350 ℃.
8. The method for preparing a thermal barrier coating material having a perovskite structure as claimed in claim 5, wherein the sintering temperature is 1650 ℃ in an air atmosphere, and the sintering time is 2 hours.
9. The use of a thermal barrier coating material prepared by the method for preparing a thermal barrier coating material having a perovskite structure as claimed in claim 5 as a surface coating material for high temperature environmental working equipment of aviation turbine engines and gas turbines.
CN202310539216.4A 2023-05-12 2023-05-12 Thermal barrier coating material with perovskite structure and preparation method thereof Pending CN116639988A (en)

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Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
ZHOU SHIYU: ""Microstructure and dielectric properties of high entropy Ba (Zr0.2Ti0.2Sn0.2Hf0.2Me0.2)O3 perovskite oxides"", 《CERAMICS INTERNATIONAL》, vol. 46, no. 6, pages 7430 - 7437, XP086054663, DOI: 10.1016/j.ceramint.2019.11.239 *
赵娟利: ""热障涂层材料研究进展"", 《现代技术陶瓷》, vol. 41, no. 3, pages 148 - 170 *

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