CN116120062A - High-temperature-resistant defect type Y (Y) x Ta 1-x )O 4-x Oxygen barrier/thermal barrier ceramic integrated material and preparation method thereof - Google Patents

High-temperature-resistant defect type Y (Y) x Ta 1-x )O 4-x Oxygen barrier/thermal barrier ceramic integrated material and preparation method thereof Download PDF

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CN116120062A
CN116120062A CN202211020994.4A CN202211020994A CN116120062A CN 116120062 A CN116120062 A CN 116120062A CN 202211020994 A CN202211020994 A CN 202211020994A CN 116120062 A CN116120062 A CN 116120062A
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temperature
yttrium oxide
thermal barrier
oxygen barrier
integrated material
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CN116120062B (en
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冯晶
汪俊
种晓宇
张宇轩
苏涛
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Kunming University of Science and Technology
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Abstract

The patent application discloses a high temperature resistant defect type Y (Y x Ta 1‑x )O 4‑x Oxygen barrier/thermal barrier ceramic integrated material and preparation method thereof, wherein the raw material comprises synthetic yttrium oxide Y 2 O 3 Tantalum pentoxide Ta 2 O 5 Synthetic yttrium oxide Y 2 O 3 And tantalum pentoxide Ta 2 O 5 The molar ratio of (2) is 1:1, synthesizing YTaO by a solid phase method 4 Powder; the dopant yttrium oxide Y 2 O 3 For dopingIn YTaO 4 The powder is ball milled, dried and sieved, and then sintered by spark plasma to obtain high temperature resistant defect type Y (Y) x Ta 1‑x )O 4‑x The oxygen barrier/thermal barrier ceramic integrated material, wherein x ranges from 0.03 to 0.15. The material has low heat conductivity, excellent high-temperature fracture toughness and excellent oxygen barrier property, and can prevent oxygen ions from diffusing, avoid growth of TGO and prolong the service life of a coating.

Description

High-temperature-resistant defect type Y (Y) x Ta 1-x )O 4-x Oxygen barrier/thermal barrier ceramic integrated material and preparation method thereof
Technical Field
The invention relates to the technical field of high-temperature heat protection and oxidation resistance, in particular to a high-temperature defect-resistant Y (Y x Ta 1-x )O 4-x An oxygen barrier/thermal barrier ceramic integrated material and a preparation method thereof.
Background
Thermal barrier coating materials are widely used in aircraft engines, gas turbines, and the like due to their good thermal insulation, high Wen Que-swage resistance, corrosion resistance, thermal shock resistance, and thermal shock resistance. A typical thermal barrier coating system generally includes an alloy substrate, a bond coat, a ceramic layer, and a thermally grown oxide layer (TGO) located between the bond coat and the ceramic layer. Leckie et al found that TGO is one of the main causes of failure of the thermal barrier coating, and during the high temperature thermal cycle stage, the continuous growth of TGO causes mismatch of thermal expansion coefficients of the bond coat and the ceramic layer, and huge stress is generated inside the thermal barrier coating system, so that the TGO is displaced in the vertical direction of the ceramic layer, and when the displacement of TGO is too large, the TGO will be caused to fail and flake, and the thermal barrier coating system will fail.
In order to avoid high temperature oxidation of the metal matrix and the bond coat, the diffusion of oxygen ions in the thermal barrier coating should be reduced. Yttria Stabilized Zirconia (YSZ) is the most widely studied class of thermal barrier coating materials today, but it is actually an oxygen ion conductor, and Rajeswari et al report that the ionic conductivity of stabilized zirconia ceramic (8 YSZ) ranges from 0.09S/cm to 0.134S/cm at 800 ℃, just as YSZ is a conductor of oxygen ions and is also used as an electrode material for fuel cells, but when used in thermal barrier coatings, oxygen ions diffuse through the ceramic layer YSZ to the bond coat, leading to oxidation of the metal substrate and bond coat, accelerating the failure of the thermal barrier coating system, and therefore, there is a strong need to find a novel thermal barrier and oxygen barrier integrated coating material.
Disclosure of Invention
In order to overcome the defects in the prior art, the invention aims to provide a high-temperature-resistant defect type Y (Y x Ta 1-x )O 4-x The oxygen barrier/thermal barrier ceramic integrated material has low heat conductivity, excellent high-temperature fracture toughness and excellent oxygen barrier performance, can prevent oxygen ions from diffusing, avoid the growth of TGO and prolong the service life of a coating.
The technical scheme adopted by the invention is as follows:
high-temperature-resistant defect type Y (Y) x Ta 1-x )O 4-x Oxygen barrier/thermal barrier ceramic integrated material, raw materials comprise synthetic yttrium oxide Y 2 O 3 Tantalum pentoxide Ta 2 O 5 Synthetic yttrium oxide Y 2 O 3 And tantalum pentoxide Ta 2 O 5 The molar ratio of (2) is 1:1, synthesizing YTaO by a solid phase method 4 Powder;
the dopant yttrium oxide Y 2 O 3 For doping in YTaO 4 The powder is ball milled, dried and sieved, and then sintered by spark plasma to obtain high temperature resistant defect type Y (Y) x Ta 1-x )O 4-x Oxygen barrier/thermal barrier ceramic integrated material, wherein x ranges from 0.03 to 0.15.
Compared with the prior art, the invention has the beneficial effects that:
the scheme of the invention adopts the raw materials and the proportion, firstly, the oxygen barrier and thermal barrier coating integrated coating material with excellent performance can be obtained, and the rare earth tantalate is used as a novel thermal barrier coating material for high-temperature heat protection and has thermal conductivity (2.5 W.m -1 ·K -1 Has lower thermal conductivity (1.57-2.2 W.m) than 800 DEG C -1 ·K -1 800 ℃ C.), and furthermore the inventors of the present invention found that, when Y was added in a specific content range (x was in the range of 0.03 to 0.15) 2 O 3 Doping modified Y (Y) x Ta 1-x )O 4-x Also an insulator of oxygen ion, has excellent propertiesOxygen barrier performance can prevent oxygen ions from diffusing, avoid the growth of TGO and prolong the service life of the coating.
As a preferred embodiment of the invention, the synthesis feedstock Y 2 O 3 And tantalum pentoxide Ta 2 O 5 The purity of the product is more than or equal to 99.99 percent, and the grain diameter is in the range of 10-50 mu m. The particle size is controlled in the range, small particles fill pores among large particles in the sintering process, so that the density and strength of a sample can be improved, and the stability of the material performance is ensured by adopting the raw materials with the purity of more than or equal to 99.99% and the particle size range.
The embodiment of the invention also provides a high-temperature-resistant defect type Y (Y) x Ta 1-x )O 4-x The preparation method of the oxygen barrier/thermal barrier ceramic integrated material comprises the following steps:
(1) Weighing yttrium oxide Y as synthetic material in proportion 2 O 3 Tantalum pentoxide Ta 2 O 5 Taking absolute ethyl alcohol as a medium, uniformly ball-milling in a ball mill, drying and sieving;
(2) Calcining at 1500-1700 deg.c for 10-15 hr at 5-10 deg.c/min, cooling after calcining, cooling to room temperature and taking out powder to obtain YTaO 4 Powder;
(3) Weighing the doping agent yttrium oxide Y 2 O 3 YTaO is reused by the ball mill 4 Powder and dopant yttrium oxide Y 2 O 3 Ball grinding into slurry, drying and sieving the particle size;
(4) Sintering the ceramic block by using spark plasma sintering equipment, wherein the sintering temperature is 1500-1700 ℃, the heat preservation is carried out for 5-20 min, the heating rate is 50-100 ℃/min, and the sintered ceramic block is annealed at a low temperature and then annealed at a high temperature.
The preparation method provided by the invention has the following beneficial effects:
1. doped yttrium oxide Y 2 O 3 After that, Y 3+ Ion solid solution to Ta 5+ And Y 3+ The position of the oxygen vacancy concentration in the material system is increased, so that oxygen vacancies in the system form clusters, the concentration of carriers (available oxygen vacancies) is reduced,further, the oxygen ion conductivity is reduced, the oxygen insulativity of the material is improved, and the formation equation of oxygen vacancies is as follows:
Figure BDA0003813923670000021
2. the sintered ceramic block is subjected to a unique annealing process, namely low-temperature annealing and then high-temperature annealing, wherein the purpose of the low-temperature annealing is to remove internal stress in the ceramic block, prevent the ceramic block from pulverization or fragmentation caused by stress release in the high-temperature use process, and the purpose of the high-temperature annealing is to completely remove carbon permeated in the ceramic block in the sintering process.
As a preferred embodiment of the present invention, the balls are ball-milled in step (1): raw materials: the mass ratio of the absolute ethyl alcohol is 5-9: 1 to 3: 2-6, the ball milling time is more than or equal to 20h, and the rotating speed of the ball mill is 400-600 r/min. Selecting yttrium oxide Y as a synthetic material according to the requirements 2 O 3 Tantalum pentoxide Ta 2 O 5 During ball milling, the granularity distribution of the raw materials is more uniform, and the subsequent reaction is more sufficient.
As a preferred embodiment of the invention, the slurry after ball milling in the step (3) is dried at 60-100 ℃ for 10-100 hours and then screened, and particles with the particle size of 325-1500 meshes are screened. The sintered powder of the raw materials with the particle size range has higher density.
As a preferred embodiment of the invention, the temperature is 600-900 ℃ during low-temperature annealing, the heating rate is 2-5 ℃/min, the temperature is kept for 120-600 min, the temperature of high-temperature annealing is 1500-1700 ℃, the heating rate is 5-10 ℃/min, and the temperature is kept for 120-600 min. The low-temperature annealing and the high-temperature annealing adopt the temperature, the heating rate and the heat preservation time in the control range, so that the internal stress in the ceramic block can be removed to a greater extent, and the carbon permeated in the ceramic block in the sintering process can be completely removed.
Drawings
FIG. 1 is the XRD patterns of inventive examples 1-5 and comparative example 1.
FIG. 2 is an oxygen ion conductivity spectrum of examples 1 to 5 and comparative example 1 of the present invention.
FIG. 3 is an oxygen ion conductivity spectrum of 8 YSZ.
FIG. 4 shows examples 1 to 5Y (Y) x Ta 1-x )O 4-x (x=0, 0.03, 0.06, 0.09, 0.12, 0.15), thermal conductivity maps of comparative example 1 and comparative example 2.
FIG. 5 shows the conductivity patterns of the present invention in example 6 and example 7 at different temperatures.
Detailed Description
Exemplary embodiments that embody features and advantages of the present invention will be set forth in detail in the following description. It will be understood that the invention is capable of various modifications in various embodiments, all without departing from the scope of the invention, and that the description and illustrations herein are intended to be by way of illustration only and not to be construed as limiting the invention.
Example 1:
high-temperature-resistant defect type Y (Y) x Ta 1-x )O 4-x Oxygen barrier/thermal barrier ceramic integrated material, raw materials comprise synthetic material Y 2 O 3 Tantalum pentoxide Ta 2 O 5 Weighing yttrium oxide Y as synthetic material 2 O 3 And tantalum pentoxide Ta 2 O 5 2500g in total, the molar ratio of the two being 1:1, synthesizing YTaO by a solid phase method 4 Powder, yttrium oxide Y as doping agent 2 O 3 Doped in YTaO 4 The powder is ball milled, dried and sieved, and is sintered by spark plasma to obtain Y (Y) x Ta 1-x )O 4-x The oxygen barrier/thermal barrier ceramic integrated material, x in this embodiment is 0.03.
The high temperature resistant defect type Y (Y) x Ta 1-x )O 4-x The preparation method of the oxygen barrier/thermal barrier ceramic integrated material comprises the following steps:
(1) The synthetic material Y is weighed according to the mol ratio of 1:1 2 O 3 And tantalum pentoxide Ta 2 O 5 2500g in total, the mass ratio is 8:3:5, weighing zirconia balls, raw materials and absolute ethyl alcohol according to the proportion, putting the zirconia balls, the raw materials and the absolute ethyl alcohol into a ball mill for ball milling for 20 hours, wherein the rotating speed of the ball mill is 600r/min, drying the materials at 90 ℃ for 60 hours, and sieving the materials with a 325-mesh sieve;
(2) Calcining in a high-temperature box furnace at 1500 ℃ and 6h for 5 ℃/min, cooling with the furnace after calcining, and taking out the powder after the temperature is reduced to room temperature;
(3) 3% molY 2 O 3 Doped in 97 mol% YTaO 4 Putting 500g of powder into a ball mill for ball milling until the particle size of particles in slurry is 0.01-2 mu m (zirconium oxide balls, sintered powder and absolute ethyl alcohol are weighed according to the mass ratio of 8:3:5 in secondary ball milling), drying the powder at 90 ℃ for 60 hours after ball milling for 20 hours, and screening particles with the particle size range of 325-1300 meshes;
(4) Sintering the sieved powder into ceramic blocks by using spark plasma sintering equipment (SPS), wherein the sintering temperature is 1500 ℃, the heat preservation is carried out for 10min, the heating rate is 50 ℃/min, and the ceramic blocks are taken out after furnace cooling to obtain Y (Y) 0.03 Ta 0.97 )O 3.97 The oxygen barrier/thermal barrier ceramic integrated material is prepared by annealing a sintered ceramic block at a low temperature of 800 ℃ for 600min at a heating rate of 2 ℃/min, and annealing the ceramic block at a high temperature of 1600 ℃ for 300min after furnace cooling at a heating rate of 10 ℃/min.
Y (Y) 0.03 Ta 0.97 )O 3.97 XRD component analysis of the ceramic mass, as shown in FIG. 1 (a), was carried out, and by comparing the ceramic mass with a standard card, the synthetic Y (Y) of the present invention was found in FIG. 1 (b) which is a partial enlarged view (26 DEG to 35 DEG) of FIG. 1 (a) 0.03 Ta 0.97 )O 3.97 With YTaO 4 The peak positions are relatively close. The impedance value at 600 to 900 c was measured using ac impedance and the electrical conductivity was calculated as shown in fig. 2 (a).
Example 2:
the difference from example 1 is the dopant yttrium oxide Y 2 O 3 The ratio of the total mole is 6%, and the conductivity at 600-900 ℃ is shown in FIG. 2 (b).
Example 3:
the difference from example 1 is the dopant yttrium oxide Y 2 O 3 The ratio of the total mole is 9%, and the conductivity at 600-900 ℃ is shown in FIG. 2 (b).
Example 4:
the difference from example 1 is the dopant yttrium oxide Y 2 O 3 The ratio of the total mole is 12%, and the conductivity at 600-900 ℃ is shown in fig. 2 (b).
Example 5:
the difference from example 1 is the dopant yttrium oxide Y 2 O 3 The proportion of the total mole is 15%, and the conductivity at 600-900 ℃ is shown in figure 2 (b).
Comparative example 1:
the difference from example 1 is the dopant yttrium oxide Y 2 O 3 The ratio of the total mole is 0%, and the conductivity at 600-900 ℃ is shown in figure 2 (a).
Analysis of examples 1-5 and comparative example 1 in combination, it was found that yttria Y was added with the dopant 2 O 3 The conductivity of the rare earth tantalate tends to increase and then decrease when the mole percentage is increased, and the conductivity is the lowest when the mole percentage is 9%. This is because of the 3-valent Y 3+ Ion solid solution to Ta 5+ And RE (RE) 3+ The position, the disorder degree of atoms increases, the oxygen vacancy concentration increases, the oxygen ion conductivity and the oxygen diffusion rate increase, and the oxidation resistance decreases, but the oxygen vacancy conductivity does not increase with the increase of the doping concentration, but decreases after having a peak because: (1) After the concentration of oxygen vacancies is increased to a certain concentration, defect association occurs, and the association between vacancies is performed, so that part of oxygen vacancies cannot be used as oxygen ion transmission paths; (2) In order to maintain electrostatic balance, the electrons adsorb oxygen vacancies such that the oxygen vacancies cannot act as oxygen ion transport paths; in summary, after the oxygen vacancy concentration increases to a certain peak value, the conductivity tends to increase and then decrease, thereby reducing the conductivity of the rare earth tantalate.
Example 6
The difference from example 1 is the dopant Y 2 O 3 The ratio of the spark plasma sintering to the total mass is 9%, the temperature of spark plasma sintering is 1600 ℃, and the conductivity of the spark plasma sintering is 600-900 ℃ as shown in figure 5.
Example 7
The difference from example 6 is that the spark plasma sintering temperature is 1700℃and the electrical conductivity is shown in FIG. 5 at 600 to 900 ℃.
Comparative examples 6 and 7 show that the sintering temperature has a certain effect on the conductivity of oxygen ions, mainly the higher the sintering temperature, the higher the density and the higher the conductivity.
Comparative example 2
The existing commonly used thermal barrier coating material 8YSZ is a control group, the electrical conductivity at 600-900 ℃ is shown in figure 3, the electrical conductivity is shown in figure 3, and the thermal conductivity is shown in figure 4.
Analysis of the above examples and comparative example 2 by comprehensive comparison revealed that Y (Y x Ta 1-x )O 4-x The oxygen barrier/thermal barrier ceramic integrated material has significantly lower oxygen ion electrical conductivity and thermal conductivity than the existing commonly used thermal barrier coating material 8YSZ, which shows that the oxygen barrier/thermal barrier ceramic integrated material has excellent thermal barrier and oxygen barrier properties.
The foregoing is merely an example of the present invention and common knowledge of the characteristics and the like of a scheme is not described in detail herein. It should be noted that modifications and improvements can be made by those skilled in the art without departing from the spirit of the invention, which should also be considered as the scope of the invention, which does not affect the effect of the implementation of the invention and the utility of the patent. The protection scope of the present application shall be subject to the content of the claims, and the description of the specific embodiments and the like in the specification can be used for explaining the content of the claims.

Claims (6)

1. High-temperature-resistant defect type Y (Y) x Ta 1-x )O 4-x The oxygen barrier/thermal barrier ceramic integrated material is characterized in that:
the raw materials comprise synthetic yttrium oxide Y 2 O 3 Tantalum pentoxide Ta 2 O 5 Synthetic yttrium oxide Y 2 O 3 And tantalum pentoxide Ta 2 O 5 The molar ratio of (2) is 1:1, synthesizing YTaO by a solid phase method 4 Powder;
the dopant yttrium oxide Y 2 O 3 For doping in YTaO 4 Ball milling, stoving and sieving the powder,high temperature resistant defect type Y (Y) is obtained by spark plasma sintering x Ta 1-x )O 4-x Oxygen barrier/thermal barrier ceramic integrated material, wherein x ranges from 0.03 to 0.15.
2. The high temperature resistant defective Y (Y x Ta 1-x )O 4-x The oxygen barrier/thermal barrier ceramic integrated material is characterized in that: the synthetic yttrium oxide Y 2 O 3 And tantalum pentoxide Ta 2 O 5 The purity of the product is more than or equal to 99.99 percent, and the grain diameter is in the range of 10-50 mu m.
3. High temperature resistant defective Y (Y) according to any one of claims 1-2 x Ta 1-x )O 4-x The preparation method of the oxygen barrier/thermal barrier ceramic integrated material is characterized by comprising the following steps of: the method comprises the following steps:
(1) Weighing yttrium oxide Y as synthetic material in proportion 2 O 3 Tantalum pentoxide Ta 2 O 5 Taking absolute ethyl alcohol as a medium, uniformly ball-milling in a ball mill, drying and sieving;
(2) Calcining at 1500-1700 deg.c for 10-15 hr at 5-10 deg.c/min, cooling after calcining, cooling to room temperature and taking out powder to obtain YTaO 4 Powder;
(3) Weighing the doping agent yttrium oxide Y 2 O 3 YTaO is reused by the ball mill 4 Powder and dopant yttrium oxide Y 2 O 3 Ball grinding into slurry, drying and sieving the particle size;
(4) Sintering the ceramic block by using spark plasma sintering equipment, wherein the sintering temperature is 1500-1700 ℃, the heat preservation is carried out for 5-20 min, the heating rate is 50-100 ℃/min, and the sintered ceramic block is annealed at a low temperature and then annealed at a high temperature.
4. The high temperature resistant defective Y (Y x Ta 1-x )O 4-x The preparation method of the oxygen barrier/thermal barrier ceramic integrated material is characterized by comprising the following steps of: and (3) ball milling, wherein the ball is formed by ball milling in the step (1): raw materials: the mass ratio of the absolute ethyl alcohol is(5-9): (1-3): (2-6), the ball milling time is more than or equal to 20h, and the rotating speed of the ball mill is 400-600 r/min.
5. The high temperature resistant defective Y (Y x Ta 1-x )O 4-x The preparation method of the oxygen barrier/thermal barrier ceramic integrated material is characterized by comprising the following steps of: drying the slurry subjected to ball milling in the step (3) at 60-100 ℃ for 10-100 hours, sieving, and screening particles with the particle size of 325-1500 meshes.
6. The high temperature resistant defective Y (Y x Ta 1-x )O 4-x The preparation method of the oxygen barrier/thermal barrier ceramic integrated material is characterized by comprising the following steps of: the temperature is 600-900 ℃ during low-temperature annealing, the heating rate is 2-5 ℃/min, the temperature is kept for 120-600 min, the temperature of high-temperature annealing is 1500-1700 ℃, the heating rate is 5-10 ℃/min, and the temperature is kept for 120-600 min.
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