CN116063071A - High-temperature piezoelectric ceramic material and phase boundary regulating and controlling method thereof - Google Patents

High-temperature piezoelectric ceramic material and phase boundary regulating and controlling method thereof Download PDF

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CN116063071A
CN116063071A CN202310065885.2A CN202310065885A CN116063071A CN 116063071 A CN116063071 A CN 116063071A CN 202310065885 A CN202310065885 A CN 202310065885A CN 116063071 A CN116063071 A CN 116063071A
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piezoelectric ceramic
ceramic material
phase
temperature
phase boundary
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赵天龙
石柯飞
费春龙
董广志
王满之
孙韬
孙昕郝
张娟
刘�文
全熠
戴显英
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Xidian University
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Abstract

The invention discloses a high-temperature piezoelectric ceramic material and a phase boundary regulating and controlling method thereof, which comprises the following steps: preparing an R-phase piezoelectric ceramic material; preparing a T-phase piezoelectric ceramic material; mixing an R-phase piezoelectric ceramic material and a T-phase piezoelectric ceramic material according to a specific proportion to find a phase boundary MPB, and pressing and forming the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material corresponding to the phase boundary MPB to form a ceramic blank; and firing the ceramic blank by adopting a specific plastic-arranging sintering process to form the final high-temperature piezoelectric ceramic material. The invention can quickly find the phase boundary MPB, thereby shortening the preparation period of the high-temperature piezoelectric ceramic material.

Description

High-temperature piezoelectric ceramic material and phase boundary regulating and controlling method thereof
Technical Field
The invention belongs to the technical field of piezoelectric ceramic materials, and particularly relates to a high-temperature piezoelectric ceramic material and a phase boundary regulating and controlling method thereof.
Background
The high-temperature piezoelectric material is widely applied to a plurality of high-tech fields requiring to work under special environments, such as aerospace, geological exploration, petrochemical industry, automobile engines and the like, and the high-temperature piezoelectric material is needed to be used for a micro-displacement driver on a satellite, an automobile electronic injection, a vibration sensor, an acceleration sensor and the like in the geological exploration process.
The most widely used piezoelectric materials at present are mainly lead zirconate titanate (PZT) based piezoelectric materials of perovskite structure. The quasi-homotypic phase boundary (Morphotropic Phase Boundary, MPB for short) was originally proposed in the study of perovskite-structured PZT solid solutions, and generally refers to the region separating critical components of two ferroelectric phases with different structures when the two phases form solid solutions in different proportions. Novel perovskite structure ferroelectric BiScO 3 -PbTiO 3 With its electrical properties comparable to those of PZT, curie temperatures as high as 450 ℃ have attracted considerable attention. However, due to the high price of Sc element, the material system is not put into large-scale industrial production, and In recent years, people replace Sc element by introducing Co, in, fe and other elements, so that the piezoelectric performance is greatly reduced although the higher Curie temperature can be ensured; researchers have also introduced LiNbO 3 、LiTaO 3 Equal ABO 3 Third ternary systemSolid solutions, while guaranteeing excellent piezoelectric properties, have a greatly reduced curie temperature. One of the most effective methods at present is to introduce a ferroelectric with a relaxation structure to form a ternary solid solution with BS-PT, so that not only can excellent piezoelectric ferroelectric properties be ensured, but also the curie temperature of more than 400 ℃ can be maintained.
However, the piezoelectric ceramic material system with the relaxor structure ferroelectric is complex in phase structure, difficult to accurately regulate and control, and difficult to find the phase boundary MPB, and most of the currently adopted phase boundary regulating and controlling methods are to perform multiple experiments, so that the phase boundary MPB is found by a cooking method, time and labor are consumed, and the preparation period of the high-temperature piezoelectric ceramic material is prolonged.
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides a high-temperature piezoelectric ceramic material and a phase boundary regulating method thereof. The technical problems to be solved by the invention are realized by the following technical scheme:
in a first aspect, an embodiment of the present invention provides a method for phase boundary regulation of a high-temperature piezoelectric ceramic material, including:
preparing an R-phase piezoelectric ceramic material;
preparing a T-phase piezoelectric ceramic material;
mixing the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material according to a specific proportion to find a phase boundary MPB, and pressing the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material corresponding to the phase boundary MPB to form a ceramic blank;
and firing the ceramic blank by adopting a specific plastic-arranging sintering process to form the final high-temperature piezoelectric ceramic material.
In one embodiment of the present invention, the process for preparing the R-phase piezoceramic material includes:
according to chemical composition of (1-x) 1 )BiScO 3 -x 1 PbTiO 3 Is to weigh the Sc of the raw material 2 O 3 、Bi 2 O 3 、PbO、TiO 2 The method comprises the steps of carrying out a first treatment on the surface of the Wherein, (1-x 1 ) And x 1 Respectively represent BiScO 3 、PbTiO 3 Is of the mole of (2)Molar ratio, x 1 The value is less than 0.63;
sequentially performing ball milling mixing, presintering, secondary ball milling mixing, drying and grinding processes on the weighed raw materials to prepare mixed powder;
adding the adhesive polyvinyl alcohol into the prepared mixed powder, and granulating to form the R-phase piezoelectric ceramic material.
In one embodiment of the present invention, the process of preparing the T-phase piezoelectric ceramic material includes:
according to chemical composition of (1-x) 2 )BiScO 3 -x 2 PbTiO 3 Is to weigh the Sc of the raw material 2 O 3 、Bi 2 O 3 、PbO、TiO 2 The method comprises the steps of carrying out a first treatment on the surface of the Wherein, (1-x 2 ) And x 2 Respectively represent BiScO 3 、PbTiO 3 Molar ratio, x 2 The value is more than 0.64;
sequentially performing ball milling mixing, presintering, secondary ball milling mixing, drying and grinding processes on the weighed raw materials to prepare mixed powder;
adding adhesive polyvinyl alcohol into the prepared mixed powder, and granulating to form the T-phase piezoelectric ceramic material.
In one embodiment of the present invention, mixing the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material in a specific ratio includes:
the R phase piezoelectric ceramic material and the T phase piezoelectric ceramic material are mixed according to the proportion of 1 to 5:5 to 1.
In one embodiment of the present invention, before firing the ceramic green body to form the high temperature piezoelectric ceramic material by using a specific plastic-lined sintering process, the method further comprises:
and respectively discharging the adhesive polyvinyl alcohol in the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material at 600-600 ℃.
In one embodiment of the invention, firing the ceramic green body to form a final high temperature piezoelectric ceramic material using a specific plastic displacement sintering process comprises:
and firing the ceramic blank under the technological conditions of 600-600 ℃ of plastic discharging temperature, 1050-1150 ℃ of sintering temperature and 2-4 h of sintering heat preservation time to form the final high-temperature piezoelectric ceramic material.
In one embodiment of the present invention, further comprising:
ag electrodes are grown on the upper and lower surfaces of the high-temperature piezoelectric ceramic material, and the related performance of the high-temperature piezoelectric ceramic material is tested.
In one embodiment of the invention, ag electrodes are grown on the upper and lower surfaces of the high-temperature piezoelectric ceramic material under the process conditions that the silver burning temperature is 500-600 ℃ and the silver burning heat preservation time is 1-2 h;
and (3) carrying out direct-current high-voltage polarization under the polarization conditions that the polarization voltage is 4 kV/mm-6 kV/mm and the polarization time is 20 min-40 min in silicone oil with the temperature of 120-200 ℃, and carrying out the related performance on the high-temperature piezoelectric ceramic material after the polarization.
In one embodiment of the present invention, before growing Ag electrodes on the upper and lower surfaces of the high temperature piezoelectric ceramic material, it comprises:
polishing the upper and lower surfaces of the high-temperature piezoelectric ceramic material.
In a second aspect, an embodiment of the present invention provides a high temperature piezoelectric ceramic material, which is characterized in that the high temperature piezoelectric ceramic material is obtained according to any one of the steps of the phase boundary regulation method for a high temperature piezoelectric ceramic material described above.
The invention has the beneficial effects that:
according to the phase boundary regulating and controlling method of the high-temperature piezoelectric ceramic material, the advantages of a BS-PT material system are utilized, a single R-phase piezoelectric ceramic material and a single T-phase piezoelectric ceramic material are prepared, only two phase structure materials of the prepared R-phase piezoelectric ceramic material and the prepared T-phase piezoelectric ceramic material are needed, and the phase boundary MPB can be quickly found through accurately regulating and controlling the proportion of the two phase structure materials, so that the high-temperature piezoelectric ceramic material with comprehensive piezoelectric property and Curie temperature advantages is formed by pressing and firing the corresponding R-phase piezoelectric ceramic material and the corresponding T-phase piezoelectric ceramic material according to the phase boundary MPB.
The present invention will be described in further detail with reference to the accompanying drawings and examples.
Drawings
FIG. 1 is a schematic flow chart of a method for regulating and controlling phase boundaries of a high-temperature piezoelectric ceramic material according to an embodiment of the invention;
FIG. 2 is a schematic flow chart of another method for phase boundary regulation of high-temperature piezoelectric ceramic materials according to an embodiment of the present invention;
FIG. 3 is a schematic diagram showing a phase boundary adjusting method according to the embodiment of the present invention;
fig. 4 is a schematic diagram of changes in piezoelectric performance and electromechanical coupling coefficient corresponding to a phase boundary adjusting method according to an embodiment of the present invention.
Detailed Description
The present invention will be described in further detail with reference to specific examples, but embodiments of the present invention are not limited thereto.
The inventor experiment researches show that when the PZT solid solution increases to the vicinity of critical component x-0.48 (namely, the position of the quasi-homotype phase boundary MPB), the structural transformation of the trigonal phase and the tetragonal phase occurs. Experimental results also show that the phase boundary MPB with two phases coexisting is not a single component, but a component region, which shows a certain width in the phase diagram, in which the sample electrical properties are superior. The origin and mechanism of piezoelectric ceramic materials excellent in piezoelectricity at the phase boundary MPB are attracting attention. It is considered that the total amount of ferroelectric polarization oriented in the spontaneous polarization direction is greater at the phase boundary MPB where two phases coexist than a single phase, and thus the electrical properties are optimal. It is also thought that it is related to polarization rotation between different phases in the phase boundary MPB component, where the electric polarization is from the three phases (111) R The state rotates to tetragonal phase (001) T The gibbs free energy barrier of the state is minimal, resulting in excellent piezoelectric performance at the phase boundary MPB. It is particularly critical how to find the phase boundary MPB, and when the phase boundary MPB is found by the conventional method, a wide-range search is required in a wider component area, and then the range is gradually reduced. In (1-x) BiScO 3 -xPbTiO 3 For example, when the traditional method searches for the phase boundary MPB, firstly, a section with better piezoelectric performance is searched for in the ratio of x= 0.60,0.61,0.62,0.63,0.64,0.65,0.66,0.66, and then the section is further refined until the phase boundary MPB is found. Therefore, the traditional method needs to consume a large amount of raw materials, at least 9 parts of raw materials are needed to be prepared according to the proportion, and the time for searching the phase boundary MPB is long, so that the preparation period of the high-temperature piezoelectric ceramic material is prolonged.
The traditional method can find MPB, but how to quickly find MPB to shorten the preparation period of the high-temperature piezoelectric ceramic material becomes a new focus of attention again. Based on such requirements, the embodiment of the invention provides a phase boundary regulating method of a high-temperature piezoelectric ceramic material, referring to fig. 1, aiming at the phase structure composition of a BS-PT-based high-temperature piezoelectric ceramic material, comprising the following steps:
s10, preparing an R-phase piezoelectric ceramic material.
The embodiment of the invention provides an alternative scheme, and a process for preparing an R-phase piezoelectric ceramic material comprises the following steps:
according to chemical composition of (1-x) 1 )BiScO 3 -x 1 PbTiO 3 Is to weigh the Sc of the raw material 2 O 3 、Bi 2 O 3 、PbO、TiO 2 The method comprises the steps of carrying out a first treatment on the surface of the Wherein, (1-x 1 ) And x 1 Respectively represent BiScO 3 、PbTiO 3 Molar ratio, x 1 The value is less than 0.63;
sequentially performing ball milling mixing, presintering, secondary ball milling mixing, drying and grinding processes on the weighed raw materials to prepare mixed powder; wherein, the ball milling time of the ball milling tank is 18 hours, the ball milling medium is absolute ethyl alcohol, the presintering temperature is 600-900 ℃, the presintering heat preservation time is 2-4 hours, and the grinding time is 15-30 minutes.
Adding adhesive polyvinyl alcohol into the prepared mixed powder, and granulating to form the R-phase piezoelectric ceramic material. For example, the R-phase piezoelectric ceramic material can be 0.39BS-0.61PT, 0.40BS-0.60PT bismuth scandium acid-lead titanate piezoelectric ceramic material BS-PT.
S20, preparing a T-phase piezoelectric ceramic material.
The embodiment of the invention provides an alternative scheme, and a process for preparing a T-phase piezoelectric ceramic material comprises the following steps:
according to chemical composition of (1-x) 2 )BiScO 3 -x 2 PbTiO 3 Is to weigh the Sc of the raw material 2 O 3 、Bi 2 O 3 、PbO、TiO 2 The method comprises the steps of carrying out a first treatment on the surface of the Wherein, (1-x 2 ) And x 2 Respectively represent BiScO 3 、PbTiO 3 Molar ratio, x 2 The value is more than 0.64;
sequentially performing ball milling mixing, presintering, secondary ball milling mixing, drying and grinding processes on the weighed raw materials to prepare mixed powder; wherein, the ball milling time of the ball milling tank is 18 hours, the ball milling medium is absolute ethyl alcohol, the presintering temperature is 600-900 ℃, the presintering heat preservation time is 2-4 hours, and the grinding time is 15-30 minutes.
The mixed powder obtained by the preparation method is added with adhesive polyvinyl alcohol, for example, 8 weight percent of polyvinyl alcohol PVA is added, and then the mixture is granulated to form the T-phase piezoelectric ceramic material. For example, the T-phase piezoelectric ceramic material can be 0.33BS-0.66PT, 0.32BS-0.68PT bismuth scandium acid-lead titanate piezoelectric ceramic material BS-PT.
S30, mixing the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material according to a specific proportion to find a phase boundary MPB, and pressing and forming the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material corresponding to the phase boundary MPB to form a ceramic blank.
The single three-phase piezoelectric ceramic material (R-phase piezoelectric ceramic material) and the single tetragonal piezoelectric ceramic material (T-phase piezoelectric ceramic material) are respectively prepared through S10 and S20, how to mix the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material becomes key, different proportions show different phase boundary regulating and controlling effects, the aim of quickly finding out a phase boundary MPB can be achieved by accurately regulating and controlling the proportions of the two phase structure materials of the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material, the process of mixing the two phase structure materials in different proportions is simpler than the process of preparing a plurality of phase structures, the process steps are simplified, the process implementation cost is reduced, and therefore the time-consuming problem of traditional preparation of the plurality of phase structure piezoelectric ceramic materials and finding out the phase boundary MPB by adopting the plurality of phase structure materials is avoided.
According to the research of the inventor, the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material are prepared according to the following proportion of 1-5: 5-1, and the R phase piezoelectric ceramic material and the T phase piezoelectric ceramic material corresponding to the phase boundary MPB are pressed and formed to form a ceramic blank. Through the research of the inventor, more preferably, R-phase piezoelectric ceramic material and T-phase piezoelectric ceramic material are mixed according to the proportion of 5:1, 4:1, 3:1, 2:1, 1:1, 1:2, 1:3, 1:4 and 1:5, so that phase boundary MPB can be found, and R-phase piezoelectric ceramic material and T-phase piezoelectric ceramic material corresponding to the phase boundary MPB are pressed and molded to form a ceramic blank. In the pressing process, the mixed R-phase piezoelectric ceramic material and T-phase piezoelectric ceramic material are placed into a die with a certain size, for example, the diameter is 10 mm-12 mm, and a tablet press is used for pressing under the pressure of 300MPa for 20 s-30 s.
And S40, firing the ceramic blank by adopting a specific plastic-arranging sintering process to form the final high-temperature piezoelectric ceramic material.
The embodiment of the invention further comprises the following steps before the ceramic blank is fired by adopting a specific plastic-arranging sintering process to form the final high-temperature piezoelectric ceramic material:
and discharging the adhesive polyvinyl alcohol in the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material at 600-600 ℃ respectively. Next, an alternative solution is provided in the embodiments of the present invention, in which a specific plastic-displacement sintering process is used to fire the ceramic green body to form a final high-temperature piezoelectric ceramic material, including:
and firing the ceramic blank under the technological conditions of 600-600 ℃ of plastic discharging temperature, 1050-1150 ℃ of sintering temperature and 2-4 h of sintering heat preservation time to form the final high-temperature piezoelectric ceramic material. In the experimental process, when the plastic-discharging sintering process conditions for realizing the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material are not properly selected, the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material cannot be successfully sintered, and after multiple experiments, the high-temperature piezoelectric ceramic material prepared from the bismuth scandium acid-lead titanate piezoelectric ceramic materials with two different phase structures provided by the embodiment of the invention can be successfully sintered by adopting the process conditions that the plastic-discharging temperature is 600-600 ℃, the sintering temperature is 1050-1150 ℃ and the sintering heat preservation time is 2-4 hours.
Further, referring to fig. 2, the method for phase boundary regulation and control of a high-temperature piezoelectric ceramic material according to the embodiment of the present invention further includes:
and S50, growing Ag electrodes on the upper surface and the lower surface of the high-temperature piezoelectric ceramic material, and testing the related performance of the high-temperature piezoelectric ceramic material.
The embodiment of the invention comprises the following steps before Ag electrodes grow on the upper and lower surfaces of a high-temperature piezoelectric ceramic material: polishing the upper and lower surfaces of the high-temperature piezoelectric ceramic material. The polishing treatment may be performed by removing the upper and lower surfaces of the high ceramic green body having a predetermined thickness, for example, a thickness of 0.4mm, to remove the influence of surface defects.
Next, the embodiment of the invention provides an alternative scheme, wherein Ag electrodes are grown on the upper and lower surfaces of the high-temperature piezoelectric ceramic material under the technological conditions that the silver burning temperature is 500-600 ℃ and the silver burning heat preservation time is 1-2 h;
and (3) carrying out direct-current high-voltage polarization under the polarization conditions that the polarization voltage is 4 kV/mm-6 kV/mm and the polarization time is 20 min-40 min in silicone oil with the temperature of 120-200 ℃, and carrying out the related performance on the high-temperature piezoelectric ceramic material after the polarization. Through tests, the high-temperature piezoelectric ceramic material prepared by the phase boundary regulating method can realize rapid searching of MPB, thereby shortening the preparation period of the high-temperature piezoelectric ceramic material.
In order to verify the effectiveness of the phase boundary regulation method of the high-temperature piezoelectric ceramic material provided by the embodiment of the invention, the following experiment is carried out for verification.
The experimental process of the embodiment of the invention comprises the following steps: preparing 0.39BS-0.61PT of R-phase piezoelectric ceramic material and 0.33BS-0.66PT of T-phase piezoelectric ceramic material; adding a polyvinyl alcohol PVA adhesive into the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material, grinding and granulating; mixing R-phase piezoelectric ceramic materials and T-phase piezoelectric ceramic materials according to the proportion of 3:1,1:1 and 1:3 respectively; placing the mixed powder into a mould with a certain size, and pressing into ceramic blanks by a tablet press under the pressure of 300 MPa; discharging adhesive polyvinyl alcohol PVA in the ceramic blank body at 650 ℃; firing at 650 ℃ of plastic discharging temperature, 1100 ℃ of sintering temperature and 3 hours of sintering heat preservation time to form a high-temperature piezoelectric ceramic material; the upper and lower surfaces of the fired high temperature piezoelectric ceramic material are covered with Ag electrodes, polarized for 20min under the voltage of 6kV/mm, and tested for performance after aging for 24h, and the test results are shown in figures 3 and 4.
The inventor prepares piezoelectric ceramic materials with x= 0.60,0.61,0.62,0.63,0.64,0.65,0.66,0.66 phase structures by adopting a traditional method, and simultaneously the inventor mixes the prepared R-phase piezoelectric ceramic materials 0.40BS-0.60PT and T-phase piezoelectric ceramic materials 0.33BS-0.66PT in different proportions to obtain piezoelectric ceramic materials with x= 0.60,0.61,0.62,0.63,0.64,0.65,0.66,0.66 phase structures, and the method reaches the conclusion as shown in figure 3 which is the same as the traditional method. As can be seen from fig. 3: when x=0.60, a diffraction peak (200) near the diffraction angle of 45 ° is observed as a single diffraction peak, the material structure is typically a three-phase (R-phase), and as the lead titanate (PT) content increases, the (200) diffraction peak starts to broaden; when the vicinity of x=0.64 gradually splits into two peaks of (002) and (200), a transition from the three-phase to the tetragonal phase (T-phase) occurs; when x=0.66, (200) splits into two peaks, (002) and (200), the material is tetragonal. Experimental results surface: near x=0.64, the material is in the intermediate state of three-way to four-way phase transition, here the MPB site of the system. Wherein, the numerals in brackets in fig. 3 indicate the crystal orientation structure of the sample currently irradiated with X-rays, and the abscissa θ indicates the incident angle at the time of X-ray irradiation.
Meanwhile, it can be seen from 4 that: the R-phase piezoelectric ceramic material 0.40BS-0.60PT and the T-phase piezoelectric ceramic material 0.33BS-0.66PT are mixed according to different proportions to obtain different phases of x= 0.60,0.61,0.62,0.63,0.64,0.65,0.66,0.66Piezoelectric ceramic material of structure, piezoelectric property d 33 All reach more than 360pC/N and electromechanical coupling coefficient k p /k t All reach more than 0.50, and when x=0.64, the piezoelectric property d corresponds to 33 Coefficient of electromechanical coupling k p /k t The best is achieved, and the high-temperature piezoelectric ceramic material prepared by the phase boundary regulating and controlling method provided by the embodiment of the invention has good piezoelectric performance at the MPB and keeps the Curie temperature advantage of the BS-PT material.
In summary, the phase boundary regulating method for the high-temperature piezoelectric ceramic material provided by the embodiment of the invention utilizes the advantages of the BS-PT material system to prepare a single R-phase piezoelectric ceramic material and a single T-phase piezoelectric ceramic material, and only needs to accurately regulate and control the proportion of the two phase structural materials according to the prepared R-phase piezoelectric ceramic material and the prepared T-phase piezoelectric ceramic material, so that the phase boundary MPB can be quickly found, and the high-temperature piezoelectric ceramic material with comprehensive piezoelectric property and Curie temperature advantages is formed by pressing and firing the corresponding R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material according to the phase boundary MPB.
It should be noted that the embodiment of the invention is not only suitable for BS-PT system materials, but also suitable for fast searching of phase boundary MPB of all multiphase mixed piezoelectric ceramics.
In a second aspect, an embodiment of the present invention provides a high temperature piezoelectric ceramic material, which is prepared by using the phase boundary regulation method of any one of the high temperature piezoelectric ceramic materials according to the first aspect. For the material embodiments of the second aspect, since they are substantially similar to the phase boundary control method embodiments of the first aspect, the description is relatively simple, and the relevant points are referred to in the description of the phase boundary control method embodiments of the first aspect.
In the description of the present invention, it should be understood that the terms "first," "second," and the like are used for descriptive purposes only and are not to be construed as indicating or implying a relative importance or number of technical features indicated. Thus, a feature defining "a first" or "a second" may explicitly or implicitly include one or more such feature. In the description of the present invention, the meaning of "a plurality" is two or more, unless explicitly defined otherwise.
Although the invention is described herein in connection with various embodiments, other variations to the disclosed embodiments can be understood and effected by those skilled in the art in practicing the claimed invention, from a study of the specification and the drawings. In the description, the word "comprising" does not exclude other elements or steps, and the "a" or "an" does not exclude a plurality. Some measures are described in mutually different embodiments, but this does not mean that these measures cannot be combined to produce a good effect.
The foregoing is a further detailed description of the invention in connection with the preferred embodiments, and it is not intended that the invention be limited to the specific embodiments described. It will be apparent to those skilled in the art that several simple deductions or substitutions may be made without departing from the spirit of the invention, and these should be considered to be within the scope of the invention.

Claims (10)

1. The phase boundary regulation and control method for the high-temperature piezoelectric ceramic material is characterized by comprising the following steps of:
preparing an R-phase piezoelectric ceramic material;
preparing a T-phase piezoelectric ceramic material;
mixing the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material according to a specific proportion to find a phase boundary MPB, and pressing the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material corresponding to the phase boundary MPB to form a ceramic blank;
and firing the ceramic blank by adopting a specific plastic-arranging sintering process to form the final high-temperature piezoelectric ceramic material.
2. The method for phase boundary control of a high temperature piezoelectric ceramic material according to claim 1, wherein the process for preparing the R-phase piezoelectric ceramic material comprises:
according to chemical composition of (1-x) 1 )BiScO 3 -x 1 PbTiO 3 Is to weigh the Sc of the raw material 2 O 3 、Bi 2 O 3 、PbO、TiO 2 The method comprises the steps of carrying out a first treatment on the surface of the Wherein, (1-x 1 ) And x 1 Respectively represent BiScO 3 、PbTiO 3 Molar ratio, x 1 The value is less than 0.63;
sequentially performing ball milling mixing, presintering, secondary ball milling mixing, drying and grinding processes on the weighed raw materials to prepare mixed powder;
adding the adhesive polyvinyl alcohol into the prepared mixed powder, and granulating to form the R-phase piezoelectric ceramic material.
3. The method for phase boundary control of a high temperature piezoelectric ceramic material according to claim 1, wherein the process for preparing the T-phase piezoelectric ceramic material comprises:
according to chemical composition of (1-x) 2 )BiScO 3 -x 2 PbTiO 3 Is to weigh the Sc of the raw material 2 O 3 、Bi 2 O 3 、PbO、TiO 2 The method comprises the steps of carrying out a first treatment on the surface of the Wherein, (1-x 2 ) And x 2 Respectively represent BiScO 3 、PbTiO 3 Molar ratio, x 2 The value is more than 0.64;
sequentially performing ball milling mixing, presintering, secondary ball milling mixing, drying and grinding processes on the weighed raw materials to prepare mixed powder;
adding adhesive polyvinyl alcohol into the prepared mixed powder, and granulating to form the T-phase piezoelectric ceramic material.
4. The phase boundary control method of a high-temperature piezoelectric ceramic material according to claim 1, wherein mixing the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material in a specific ratio comprises:
the R phase piezoelectric ceramic material and the T phase piezoelectric ceramic material are mixed according to the proportion of 1 to 5:5 to 1.
5. The method of phase boundary control of a high temperature piezoelectric ceramic material according to claim 1, further comprising, prior to firing the ceramic green body to form the high temperature piezoelectric ceramic material using a specific plastic-displacement sintering process:
and respectively discharging the adhesive polyvinyl alcohol in the R-phase piezoelectric ceramic material and the T-phase piezoelectric ceramic material at 600-600 ℃.
6. The method of claim 1, wherein firing the ceramic green body to form a final high temperature piezoelectric ceramic material using a specific plastic displacement sintering process comprises:
and firing the ceramic blank under the technological conditions of 600-600 ℃ of plastic discharging temperature, 1050-1150 ℃ of sintering temperature and 2-4 h of sintering heat preservation time to form the final high-temperature piezoelectric ceramic material.
7. The method for phase boundary control of a high temperature piezoelectric ceramic material according to claim 1, further comprising:
ag electrodes are grown on the upper and lower surfaces of the high-temperature piezoelectric ceramic material, and the related performance of the high-temperature piezoelectric ceramic material is tested.
8. The method for phase boundary control of high-temperature piezoelectric ceramic material according to claim 6, wherein,
growing Ag electrodes on the upper and lower surfaces of the high-temperature piezoelectric ceramic material under the technological conditions that the silver burning temperature is 500-600 ℃ and the silver burning heat preservation time is 1-2 h;
and (3) carrying out direct-current high-voltage polarization under the polarization conditions that the polarization voltage is 4 kV/mm-6 kV/mm and the polarization time is 20 min-40 min in silicone oil with the temperature of 120-200 ℃, and carrying out the related performance on the high-temperature piezoelectric ceramic material after the polarization.
9. The phase boundary control method of high temperature piezoelectric ceramic material according to claim 6, comprising, before growing Ag electrodes on the upper and lower surfaces of the high temperature piezoelectric ceramic material:
polishing the upper and lower surfaces of the high-temperature piezoelectric ceramic material.
10. A high temperature piezoelectric ceramic material, characterized in that the high temperature piezoelectric ceramic material is obtained according to the steps of the high temperature piezoelectric ceramic material phase boundary regulating method according to any one of claims 1 to 9.
CN202310065885.2A 2023-01-16 2023-01-16 High-temperature piezoelectric ceramic material and phase boundary regulating and controlling method thereof Pending CN116063071A (en)

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