CN114230339B - Rare earth tantalate high-entropy ceramic material and preparation method and application thereof - Google Patents

Rare earth tantalate high-entropy ceramic material and preparation method and application thereof Download PDF

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CN114230339B
CN114230339B CN202210048214.0A CN202210048214A CN114230339B CN 114230339 B CN114230339 B CN 114230339B CN 202210048214 A CN202210048214 A CN 202210048214A CN 114230339 B CN114230339 B CN 114230339B
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rare earth
ceramic material
entropy ceramic
oxide powder
tantalate
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CN114230339A (en
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刘玲
马壮
柳彦博
刘瀚文
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Beijing Institute of Technology BIT
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Abstract

The invention provides a rare earth tantalate high-entropy ceramic material and a preparation method and application thereof, belonging to the technical field of high-temperature thermal protection ceramic materials. The rare earth tantalate high-entropy ceramic material provided by the invention has a chemical formula of RELA 3 O 9 The RE is rare earth elements which comprise more than five of Y, la, ce, pr, nd, gd, tb and Tm. According to the invention, more than five rare earth elements are introduced into tantalate simultaneously, so that the lattice distortion degree of the tantalate can be adjusted, the phonon scattering of the tantalate is enhanced, the rare earth tantalate high-entropy ceramic material is ensured to have the characteristics of high phase stability and low thermal conductivity, and the rare earth tantalate high-entropy ceramic material has a wide application prospect in the field of thermal barrier coating materials.

Description

Rare earth tantalate high-entropy ceramic material and preparation method and application thereof
Technical Field
The invention relates to the technical field of high-temperature thermal protection ceramic materials, in particular to a rare earth tantalate high-entropy ceramic material and a preparation method and application thereof.
Background
The turbine engine blade is made of high-temperature nickel-based alloy, but the maximum working temperature of the turbine engine blade is only 1100 ℃, which is far lower than the turbine inlet temperature of the engine, so that a layer of thermal barrier coating material with low thermal conductivity needs to be coated on the surface of the engine blade to protect the engine blade from high-temperature erosion.
The most widely used thermal barrier coating material at present is yttria-stabilized zirconia (YSZ), which is a ceramic material, and the thermal conductivity is less than or equal to 2.4W/m.K under 1073K, but the thermal barrier coating material has the problems of unstable structure and sintering (namely, the growth of crystal grains is increased, so that pores are sealed and filled, and the porosity is reduced) under the condition of higher temperature, so that the thermal insulation capability of the thermal barrier coating material at high temperature is reduced, the thermal protection capability of the thermal barrier coating material is reduced, and the reliability of the service of an engine is influenced. In the development of other thermal barrier coating material systems, materials represented by pyrochlore rare earth zirconate ceramics, magnetoplumbite hexaaluminate ceramics and the like have attracted considerable attention from researchers, but the thermal conductivity of the ceramic materials is generally 2.0 to 3.5W/mK, and further improvement is still needed.
Disclosure of Invention
The invention aims to provide a rare earth tantalate high-entropy ceramic material and a preparation method and application thereof.
In order to achieve the above object, the present invention provides the following technical solutions:
the invention provides a rare earth tantalate high-entropy ceramic material with a chemical formula of RETa 3 O 9 And RE is a rare earth element, and the rare earth element comprises more than five of Y, la, ce, pr, nd, gd, tb and Tm.
Preferably, the rare earth elements in the rare earth tantalate high-entropy ceramic material are Y, la, ce, nd and Gd, or Y, la, nd, tb and Tm.
Preferably, the amount of each rare earth element in the rare earth tantalate high-entropy ceramic material is the same.
Preferably, the chemical formula of the rare earth tantalate high-entropy ceramic material is (Y) 1/5 La 1/5 Ce 1/5 Nd 1/5 Gd 1/5 )Ta 3 O 9 Or (Y) 1/5 La 1/5 Nd 1/5 Tb 1/5 Tm 1/5 )Ta 3 O 9
Preferably, the granularity of the rare earth tantalate high-entropy ceramic material is less than or equal to 7 mu m, and the purity of the rare earth tantalate high-entropy ceramic material is more than or equal to 99wt%.
The invention provides a preparation method of a rare earth tantalate high-entropy ceramic material in the technical scheme, which comprises the following steps of:
according to the element composition of the rare earth tantalate high-entropy ceramic material, mixing rare earth oxide powder and tantalum oxide powder and calcining to obtain the rare earth tantalate high-entropy ceramic material.
Preferably, the method of mixing the rare earth oxide powder with the tantalum oxide powder comprises:
mixing rare earth oxide powder, tantalum oxide powder and a ball milling medium, then carrying out ball milling, carrying out solid-liquid separation on the obtained slurry, and drying the obtained solid material.
Preferably, the ball milling time is 3 to 12 hours.
Preferably, the calcination is pressureless calcination; the calcining temperature is 1400-1600 ℃ and the time is 2-4 h.
The invention provides an application of the rare earth tantalate high-entropy ceramic material or the rare earth tantalate high-entropy ceramic material prepared by the preparation method in the technical scheme in a thermal barrier coating material.
The invention provides a rare earth tantalate high-entropy ceramic material with a chemical formula of RETa 3 O 9 The RE is a rare earth element, and the rare earth element comprises more than five of Y, la, ce, pr, nd, gd, tb and Tm; the ratio of the total mass amount of the rare earth elements to the mass amount of Ta is 1:3. according to the invention, more than five rare earth elements are introduced into tantalate simultaneously, so that the lattice distortion degree of the tantalate can be adjusted, the phonon scattering of the tantalate is enhanced, the rare earth tantalate high-entropy ceramic material is ensured to have the characteristics of high phase stability and low thermal conductivity, and the rare earth tantalate high-entropy ceramic material has a wide application prospect in the field of thermal barrier coating materials. The results of the examples show that the thermal conductivity of the rare earth tantalate high-entropy ceramic material provided by the invention is not higher than 1.7W/m.K under the condition of 1073K, and the phase composition from room temperature (25 ℃) to 700 ℃ is not changed, which indicates that the rare earth tantalate high-entropy ceramic material has high phase stability.
The invention provides a preparation method of a rare earth tantalate high-entropy ceramic material, which comprises the following steps: according to the element composition of the rare earth tantalate high-entropy ceramic material, mixing rare earth oxide powder and tantalum oxide powder and calcining to obtain the rare earth tantalate high-entropy ceramic material. The preparation method provided by the invention is simple to operate, flexible and controllable, and strong in practicability; the prepared rare earth tantalate high-entropy ceramic material has high phase stability, low thermal conductivity and high purity which is more than or equal to 99wt%.
Drawings
FIG. 1 is an X-ray diffraction spectrum of the rare earth tantalate high-entropy ceramic material powder prepared in example 1;
FIG. 2 is an X-ray diffraction spectrum of the rare earth tantalate high-entropy ceramic material powder prepared in example 1 at different temperatures;
FIG. 3 is a thermal conductivity diagram of the rare earth tantalate high-entropy ceramic material powder prepared in example 1.
Detailed Description
The invention provides a rare earth tantalate high-entropy ceramic material with a chemical formula of RETa 3 O 9 And RE is a rare earth element, and the rare earth element comprises more than five of Y, la, ce, pr, nd, gd, tb and Tm.
In the present invention, for example, the formula is RELA 3 O 9 Specifically, the ratio of the total amount of rare earth elements to the amount of Ta is 1:3.
in the invention, the chemical formula of the rare earth tantalate high-entropy ceramic material can be further expressed as (Y) a La b Ce c Pr d Nd e Gd f Tb g Tm h )Ta 3 O 9 Wherein a + b + c + d + e + f + g + h =1, and at least 5 values of a, b, c, d, e, f, g and h>0。
In the invention, the rare earth elements in the rare earth tantalate high-entropy ceramic material can be Y, la, ce, nd and Gd, and can also be Y, la, nd, tb and Tm; in the invention, the amount of each rare earth element in the rare earth tantalate high-entropy ceramic material is preferably the same. In the invention, the chemical formula of the rare earth tantalate high-entropy ceramic material is preferably (Y) 1/ 5 La 1/5 Ce 1/5 Nd 1/5 Gd 1/5 )Ta 3 O 9 Or (Y) 1/5 La 1/5 Nd 1/5 Tb 1/5 Tm 1/5 )Ta 3 O 9
In the invention, the granularity of the rare earth tantalate high-entropy ceramic material is preferably less than or equal to 7 microns, and more preferably 1-5 microns; the purity of the rare earth tantalate high-entropy ceramic material is more than or equal to 99wt%. In the invention, the thermal conductivity of the rare earth tantalate high-entropy ceramic material is not higher than 1.7W/m.K under the condition of 1073K; the use temperature of the rare earth tantalate high-entropy ceramic material is 1000-1600 ℃.
The invention provides a preparation method of a rare earth tantalate high-entropy ceramic material in the technical scheme, which comprises the following steps:
according to the element composition of the rare earth tantalate high-entropy ceramic material, mixing the rare earth oxide powder and the tantalum oxide powder for calcining to obtain the rare earth tantalate high-entropy ceramic material.
In the present invention, the particle size of the rare earth oxide powder and the tantalum oxide powder is preferably not more than 2 μm independently; the purity of the tantalum oxide powder and the rare earth oxide powder is preferably more than or equal to 99.9wt% independently. In the present invention, the rare earth oxide powder is specifically Y 2 O 3 Powder, la 2 O 3 Powder of CeO 2 Powder, nd 2 O 3 Powder of Gd 2 O 3 Powder, tb 2 O 3 Powder and Tm 2 O 3 Five or more kinds of the powder; the tantalum oxide powder is specifically Ta 2 O 5 And (3) powder.
In the present invention, the method of mixing the rare earth oxide powder with the tantalum oxide powder preferably includes:
mixing rare earth oxide powder, tantalum oxide powder and a ball milling medium, then performing ball milling, performing solid-liquid separation on the obtained slurry, and drying the obtained solid material.
In the invention, the ball milling medium is preferably a volatile medium, more preferably absolute ethyl alcohol, and the amount of the ball milling medium is based on immersing the rare earth oxide powder and the tantalum oxide powder. In the present invention, the time for the ball milling is preferably 3 to 12 hours, more preferably 4 to 6 hours. The solid-liquid separation method is not particularly limited, and the solid-liquid separation can be realized. The present invention is not particularly limited to the above drying, and sufficient drying can be achieved. The invention preferably adopts the mixing method to be beneficial to realizing the full mixing of the rare earth oxide powder and the tantalum oxide powder, wherein, the anhydrous ethanol is adopted as the ball milling medium to ensure the better dispersion of the powder, and the ball milling can ensure the better distribution and the even mixing of the powder.
Mixing the rare earth oxide powder and tantalum oxide powderThe obtained mixed material is calcined to obtain the rare earth tantalate high-entropy ceramic material. In the present invention, the calcination is preferably pressureless calcination; the calcining temperature is preferably 1400-1600 ℃, and the time is preferably 2-4 h. In the present invention, the reaction formula of the system during the calcination process is shown as follows, wherein, the RE is 2 O 3 Represents a rare earth oxide:
RE 2 O 3 +3Ta 2 O 5 =2RETa 3 O 9
the invention preferably carries out calcination under the conditions, which is beneficial to obtaining the rare earth tantalate high-entropy ceramic material with high purity and proper grain size; the product purity is insufficient due to the fact that the calcination temperature is too low and the calcination time is too short, and the product particle size is too large due to the fact that the calcination temperature is too high and the calcination time is too long, so that the thermal conductivity of the product is affected.
After the calcination, the invention preferably cools the calcined material to room temperature along with the furnace, and then carries out crushing treatment to obtain the rare earth tantalate high-entropy ceramic material powder. In the present invention, the specific method of the pulverization treatment is not particularly limited, and a method known to those skilled in the art may be used. In the invention, the grinding treatment is preferably carried out after the crushing treatment, so that the particle size of the rare earth tantalate high-entropy ceramic material powder can be further refined. The method of the present invention for polishing is not particularly limited, and a method known to those skilled in the art may be used.
The invention provides an application of the rare earth tantalate high-entropy ceramic material or the rare earth tantalate high-entropy ceramic material prepared by the preparation method in the technical scheme in a thermal barrier coating material. The specific mode of applying the rare earth tantalate high-entropy ceramic material to a thermal barrier coating material is not particularly limited, and the method known by the technical personnel in the field can be adopted.
The technical solution of the present invention will be clearly and completely described below with reference to the embodiments of the present invention. It is to be understood that the described embodiments are merely exemplary of the invention, and not restrictive of the full scope of the invention. All other embodiments, which can be obtained by a person skilled in the art without making any creative effort based on the embodiments in the present invention, belong to the protection scope of the present invention.
Examples below starting material Y 2 O 3 、La 2 O 3 、CeO 2 、Nd 2 O 3 、Gd 2 O 3 、Tb 2 O 3 、Tm 2 O 3 And Ta 2 O 5 Are purchased from chemical engineering Limited of Waverrucke of Beijing, the purities are all 99.9wt percent, and the particle sizes are all less than or equal to 2 mu m; the high temperature furnace is purchased from Tianjin Zhonghuan electric furnace Co., ltd, and is of the model sx-G01163.
Example 1
Preparation of the chemical formula (Y) 1/5 La 1/5 Ce 1/5 Nd 1/5 Gd 1/5 )Ta 3 O 9 The high-entropy ceramic material comprises the following steps:
will Y 2 O 3 、La 2 O 3 、CeO 2 、Nd 2 O 3 、Gd 2 O 3 And Ta 2 O 5 According to Y 2 O 3 :La 2 O 3 :CeO 2 :Nd 2 O 3 :Gd 2 O 3 :Ta 2 O 5 =1:1:2:1:1:15, adding the raw material powder and absolute ethyl alcohol into a ball milling tank for ball milling, wherein the addition amount of the absolute ethyl alcohol is proper for immersing the raw material powder, and the ball milling time is 6 hours to obtain slurry; filtering the slurry, drying the obtained solid material to obtain a mixed powder material, putting the mixed powder material into a high-temperature furnace, carrying out non-pressure calcination for 3 hours at 1550 ℃, cooling to room temperature (25 ℃) along with the furnace, and crushing the obtained material to obtain the material with the chemical formula of (Y) 1/5 La 1/5 Ce 1/5 Nd 1/5 Gd 1/5 )Ta 3 O 9 The high-entropy ceramic material powder has the granularity of less than or equal to 7 mu m and the purity of 100wt%.
Fig. 1 is an X-ray diffraction spectrum of the high-entropy ceramic material powder prepared in example 1 at room temperature, and it can be known from fig. 1 that the high-entropy ceramic material powder prepared in example 1 has a pure-phase tetragonal structure.
FIG. 2 is an X-ray diffraction spectrum of the high-entropy ceramic material powder prepared in example 1 under different temperature conditions, and it can be seen from FIG. 2 that the phase composition of the high-entropy ceramic material powder prepared in example 1 from room temperature (25 ℃) to 700 ℃ is not changed, which indicates that the high-entropy ceramic material powder has high phase stability. Further tests show that the high-entropy ceramic material powder prepared in example 1 has no phase change at 1100 ℃.
Fig. 3 is a thermal conductivity graph of the high-entropy ceramic material powder prepared in example 1, and as can be seen from fig. 3, the thermal conductivity of the high-entropy ceramic material powder prepared in example 1 under the condition of 1073K is only 1.69W/m · K, and has a relatively low thermal conductivity.
From example 1, it can be known that when the high-temperature reaction temperature is 1550 ℃, the rare earth tantalate high-entropy ceramic material with high phase stability and low thermal conductivity, the purity of which is not less than 99wt%, can be prepared.
Example 2
Preparation of the chemical formula (Y) 1/5 La 1/5 Nd 1/5 Tb 1/5 Tm 1/5 )Ta 3 O 9 The high-entropy ceramic material comprises the following steps:
will Y 2 O 3 、La 2 O 3 、Nd 2 O 3 、Tb 2 O 3 、Tm 2 O 3 And Ta 2 O 5 According to Y 2 O 3 :La 2 O 3 :Nd 2 O 3 :Tb 2 O 3 :Tm 2 O 3 :Ta 2 O 5 =1:1:1:1:1:15, adding each raw material powder and absolute ethyl alcohol into a ball milling tank for ball milling, wherein the addition amount of the absolute ethyl alcohol is suitable for immersing each raw material powder, and the ball milling time is 6 hours to obtain slurry; filtering the slurry, drying the obtained solid material to obtain a mixed powder material, putting the mixed powder material into a high-temperature furnace, carrying out pressureless calcination for 3h at 1550 ℃, cooling to room temperature along with the furnace, and sequentially crushing and grinding the obtained material to obtain the material with the chemical formula of (Y) 1/5 La 1/5 Nd 1/5 Tb 1/5 Tm 1/5 )Ta 3 O 9 The high-entropy ceramic material powder has the granularity of 1-5 mu m and the purity of 100wt%.
The phase composition of the high-entropy ceramic material powder prepared in this embodiment is unchanged from room temperature to 700 ℃, and further tests show that the phase composition of the high-entropy ceramic material powder prepared in this embodiment is unchanged at 1100 ℃, which indicates that the high-entropy ceramic material powder has high phase stability; and the thermal conductivity of the high-entropy ceramic material powder prepared by the embodiment is only 1.67W/m.K under the condition of 1073K, and the high-entropy ceramic material powder has lower thermal conductivity.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.

Claims (7)

1. A high-entropy rare-earth tantalate ceramic material with chemical formula of RETa 3 O 9 The RE is a rare earth element which is Y, la, ce, nd and Gd, or Y, la, nd, tb and Tm;
the preparation method of the rare earth tantalate high-entropy ceramic material comprises the following steps:
according to the element composition of the rare earth tantalate high-entropy ceramic material, mixing rare earth oxide powder and tantalum oxide powder for calcining to obtain the rare earth tantalate high-entropy ceramic material; the calcination is pressureless calcination, the calcination temperature is 1400-1550 ℃, and the calcination time is 2-4 h;
the method for mixing the rare earth oxide powder and the tantalum oxide powder comprises the following steps:
mixing rare earth oxide powder, tantalum oxide powder and a ball milling medium, then performing ball milling, performing solid-liquid separation on the obtained slurry, and drying the obtained solid material; the ball milling medium is absolute ethyl alcohol.
2. The rare earth tantalate high-entropy ceramic material as claimed in claim 1, wherein the amount of each rare earth element in the rare earth tantalate high-entropy ceramic material is the same.
3. The rare earth tantalate high-entropy ceramic material as claimed in any one of claims 1 to 2, wherein the chemical formula of the rare earth tantalate high-entropy ceramic material is (Y) 1/5 La 1/5 Ce 1/5 Nd 1/5 Gd 1/5 )Ta 3 O 9 Or (Y) 1/5 La 1/5 Nd 1/5 Tb 1/5 Tm 1/5 )Ta 3 O 9
4. The rare earth tantalate high-entropy ceramic material as claimed in claim 1, wherein the particle size of the rare earth tantalate high-entropy ceramic material is not more than 7 μm, and the purity is not less than 99wt%.
5. The method for preparing the rare earth tantalate high-entropy ceramic material according to any one of claims 1 to 4, which comprises the following steps:
according to the element composition of the rare earth tantalate high-entropy ceramic material, mixing rare earth oxide powder and tantalum oxide powder for calcination to obtain the rare earth tantalate high-entropy ceramic material; the calcination is pressureless calcination, the calcination temperature is 1400-1550 ℃, and the calcination time is 2-4 h;
the method for mixing the rare earth oxide powder and the tantalum oxide powder comprises the following steps:
mixing rare earth oxide powder, tantalum oxide powder and a ball milling medium, then performing ball milling, performing solid-liquid separation on the obtained slurry, and drying the obtained solid material; the ball milling medium is absolute ethyl alcohol.
6. The preparation method according to claim 5, wherein the ball milling time is 3 to 12 hours.
7. Use of the rare earth tantalate high-entropy ceramic material according to any one of claims 1 to 4 or the rare earth tantalate high-entropy ceramic material prepared by the preparation method according to any one of claims 5 to 6 in thermal barrier coating materials.
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