CN117534463A - Temperature-stable lead zirconate titanate-based high-temperature piezoelectric ceramic and preparation method thereof - Google Patents
Temperature-stable lead zirconate titanate-based high-temperature piezoelectric ceramic and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a lead zirconate titanate-based high-temperature piezoelectric ceramic with stable temperature and a preparation method thereof, wherein the molecular formula of the lead zirconate titanate-based high-temperature piezoelectric ceramic is (1-x-y) Pb (Yb) 1/2 Nb 1/2 )O 3 ‑yPbZrO 3 ‑xPbTiO 3 Wherein, the value range of x is 0.4-0.6, and the value range of y is 0.4-0.6. The present invention achieves a combination of excellent curie temperature (TC-400 ℃), piezoelectric constant (d 33-450 pC/N), and high coercive field (EC-17.5 kV/cm), and excellent temperature stability in tetragonal phase samples.
Description
Technical Field
The invention relates to the technical field of piezoelectric ceramics, in particular to a lead zirconate titanate-based high-temperature piezoelectric ceramic with stable temperature and a preparation method thereof.
Background
Piezoelectric ceramics tend to be in a relatively high temperature state during use, and the source of high temperature has two aspects. On one hand, the piezoelectric ceramic device applied to some special fields can be in a high-temperature environment from the external environment, for example, the working temperature of the piezoelectric ceramic device applied to the military field can reach 125 ℃; the working temperature of the pressure sensor used in energy development and deep well detection can reach 200 ℃; the vibration sensor and the piezoelectric fuel injector used in the automotive field can work at 300 ℃ at most; the operating temperature of piezoelectric acceleration sensors used in the aerospace field will be higher. On the other hand dielectric and mechanical losses from the piezoelectric ceramic itself. Both of these reasons result in the piezoelectric ceramic being in a relatively high temperature state during use. And the change of the working temperature can lead to various performances of the piezoelectric ceramic, which can seriously affect the use of the piezoelectric ceramic device. In order to ensure stable operation of the piezoelectric device, it is necessary to minimize the range of each performance parameter of the piezoelectric ceramic along with the temperature change as much as possible, so it is important to study the temperature stability of the piezoelectric ceramic.
The piezoelectric ceramic material can realize high-efficiency conversion between mechanical energy and electric energy, is widely applied to high and new technical fields such as ultrasonic detection, mobile communication, artificial intelligence and the like at present, and has different requirements on the performance of the piezoelectric ceramic in different application fields, such as aerospace, energy development and the like, the piezoelectric ceramic energy is required to have high Curie temperature and good resonance frequency temperature stability at the same time, so that the performance of the piezoelectric ceramic cannot be deteriorated due to temperature change. Typical ternary lead zirconate titanate-based piezoelectric ceramics, such as lead magnesium niobate-lead zirconate titanate (PMN-PZT), lead nickel niobate-lead zirconate titanate (PNN-PZT), and the like, curie temperature T C All lower than 250 ℃ if the temperature is lower than the temperature of the piezoelectric ceramicsIs T C Is less than 130 c. T of PYN-PZT ternary system ceramic C Up to 395 c, the practical use temperature is close to 200 c, so that the PYN-PZT ceramic has potential for application in high temperature fields.
However, the resonant frequency of piezoelectric ceramics is very sensitive to temperature fluctuations during use. The change in the resonant frequency constant will directly cause the resonant frequency of the piezoelectric ceramic to drift. For piezoelectric devices such as a filter, a resonator, an ultrasonic motor and the like, the working frequency of the piezoelectric devices is the resonance frequency point of the piezoelectric devices, and if the resonance frequency drifts, an automatic frequency tracking loop is additionally arranged in a driving circuit, so that the driving circuit is more complex, has higher cost and is unfavorable for the application of the devices. The temperature stability of the resonant frequency of the piezoelectric ceramic is an urgent problem to be solved.
The ternary solid solution of lead ytterbium niobate-lead zirconate titanate (PYN-PZT) has excellent comprehensive performance, and compared with PZT piezoelectric ceramics, the ternary solid solution has high piezoelectric constant (d 33 About 450 pC/N) and high Curie temperature (T) C 400 ℃ and the resonance frequency temperature coefficient (deltaf) of the tetragonal phase component r /f r25℃ ) Is kept within 0.5 percent from room temperature to 300 ℃ and becomes an important high-temperature piezoelectric device manufacturing material.
For commercial applications of piezoelectric ceramics, the piezoelectric device must operate stably in an operating temperature range, and when the performance of the piezoelectric device varies with temperature, the driving of the piezoelectric device is difficult to control or the operating performance is lowered, so that the temperature stability of the piezoelectric material is a primary consideration. The resonance frequency and the piezoelectric constant are sensitive to temperature fluctuation, so that the temperature stability of the piezoelectric ceramic resonance frequency and the piezoelectric constant is very urgent to study. However, there is currently little research on the temperature stability of piezoelectric ceramics of the PYN-PZT system.
Disclosure of Invention
The invention aims to provide a lead zirconate titanate-based high-temperature piezoelectric ceramic with stable temperature and a preparation method thereof, so as to solve the problems in the prior art.
In a first aspect, the present invention provides a temperature-stable lead zirconate titanate-based high temperature piezoelectric ceramic having a molecular formula of (1-x-y) Pb (Yb) 1/2 Nb 1/2 )O 3 -yPbZrO 3 -xPbTiO 3 Wherein, the value range of x is 0.4-0.6, and the value range of y is 0.4-0.6.
In certain embodiments, the molecular formula (1-x-y) Pb (Yb 1/2 Nb 1/2 )O 3 -yPbZrO 3 -xPbTiO 3 In the lead zirconate titanate-based high temperature piezoelectric ceramic, x=0.28, y=0.52, and the resonance frequency temperature coefficient (Δf r /f r 25 ℃ from room temperature to 300 ℃ below 0.5%.
In certain embodiments, the lead zirconate titanate-based high temperature piezoceramic has a large signal piezoelectric coefficient (d 33 * ) 400-750 pm/V.
In certain embodiments, the lead zirconate titanate-based high temperature piezoceramic has a small signal piezoelectric coefficient (d 33 ) 210-485 pC/N.
In certain embodiments, the lead zirconate titanate-based high temperature piezoelectric ceramic has a curie temperature of 350 ℃ to 450 DEG C
In certain embodiments, the lead zirconate titanate-based high temperature piezoceramic crystal structure is a perovskite structure.
In a second aspect, the invention provides a method for preparing a temperature-stable lead zirconate titanate-based high-temperature piezoelectric ceramic, comprising the following steps:
step S1, according to YbNbO 4 Stoichiometric ratio of raw materials including Yb 2 O 3 And Nb (Nb) 2 O 5 Mixing all the weighed raw materials uniformly, filling the mixture into a nylon pot, taking zirconia balls as grinding balls and absolute ethyl alcohol as ball milling media, fully mixing and ball milling for 18-24 hours by using a ball mill for 150-300 r/min, separating the zirconia balls, drying the raw material mixture at 80-100 ℃ for 12-24 hours, grinding by using a mortar, and sieving by a 80-mesh sieve; placing the sieved powder into an alumina crucible, capping, calcining at 1000-1100 ℃ for 5-10 hours to synthesize YbNbO 4 Precursor powder;
step S2, according to (1-x-y) Pb (Yb 1/2 Nb 1/2 )O 3 -yPbZrO 3 -xPbTiO 3 Preparing raw materials according to a stoichiometric ratio (x is 0.4-0.6, y is 0.4-0.6), uniformly mixing all the weighed raw materials, filling the mixture into a nylon tank, fully mixing and ball milling for 18-24 hours by taking zirconium balls as grinding balls and absolute ethyl alcohol as ball milling media, separating the zirconium balls, drying the raw material mixture at 80-100 ℃ for 12-24 hours, grinding the raw material mixture by using a mortar, and sieving the raw material mixture by using an 80-mesh sieve;
step S3, placing the raw material mixture after being sieved by the 80-mesh sieve in the step S2 into an alumina crucible, compacting by an agate rod to ensure that the compacted density is 1.5g/cm 3 Capping, presintering for 4-6 hours at 750-800 ℃, naturally cooling to room temperature, and grinding by using a mortar to obtain presintering powder;
s4, putting the presintered powder into a nylon pot, fully mixing and ball-milling for 12-24 hours by taking zirconium balls as grinding balls and absolute ethyl alcohol as ball-milling media, separating the zirconium balls, drying the presintered powder at 80-100 ℃ for 12-24 hours, grinding by using a mortar, and sieving by a 180-mesh sieve;
step S5, firstly pressing the presintered powder after 180-mesh screening into a cylindrical blank by a powder tablet press, and then carrying out cold isostatic pressing for 15-20 minutes under the pressure of 200-300 MPa;
s6, placing the cylindrical blank on a zirconia flat plate, placing the zirconia flat plate in an alumina closed sagger, heating to 1100-1200 ℃ at a heating rate of 2-5 ℃/min, sintering for 3-5 hours, and naturally cooling to room temperature along with a furnace;
step S7, firstly, selecting one of the surfaces of the ceramic sintered in the step S6, polishing with 320-mesh sand paper, then polishing with 800-mesh sand paper, finally polishing with 1500-mesh sand paper and silicon carbide to a thickness of 0.5-0.6 mm, and wiping with alcohol;
and S8, coating silver paste with the thickness of 0.01-0.03 mm on the upper and lower surfaces of the ceramic polished in the step S7, placing the ceramic in a resistance furnace, preserving heat at 600 ℃ for 30 minutes, and naturally cooling to room temperature to prepare the PYN-PZT piezoelectric ceramic material.
In certain embodiments, in step S7, the sintering temperature is 1100 ℃ to 1300 ℃ and the sintering time is 1 to 5 hours.
In certain embodiments, the PYN-PZT piezoceramic material has a thickness of 0.8-1.5mm and a diameter of 8-15mm.
Preferably, in the step S2, the material is prepared according to 0.2Pb (Yb 1/2 Nb 1/2 )O 3 -0.4PbZrO 3 -0.4PbTiO 3 Respectively weighing the purity of 99.9%PbO 66.2130g,YbNbO 4 9.7883g of ZrO with a purity of 99.9% 2 14.6218g and 99.9% pure TiO 2 9.4770g as raw material.
Compared with the prior art, the invention has the following advantages:
the piezoelectric ceramic with high temperature stability is obtained by controlling the components of the material and solving the technical problems existing in the material industrialization. Secondly, through researching components and phase structures, the problem that high-voltage electric performance, high Curie temperature and coercive field are difficult to be combined is solved, and the piezoelectric ceramic with excellent comprehensive performance is obtained, and compared with the PZT ceramic material used at present and PZT base piezoelectric ceramics of other ternary systems, the piezoelectric ceramic prepared by the invention realizes excellent Curie temperature (T) C 400 ℃ C. And piezoelectric constant (d) 33 About 450 pC/N) and high coercive field (E) C About 17.5 kV/cm). And achieves excellent temperature stability in tetragonal phase samples, its resonance frequency temperature coefficient (Δf r /f r25℃ ) Kept below 0.5% from room temperature to 300 ℃. The prepared piezoelectric ceramics can be suitable for high-temperature or high-excitation device application.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings that are needed in the description of the embodiments or the prior art will be briefly described, and it is obvious that the drawings in the description below are some embodiments of the present invention, and other drawings can be obtained according to the drawings without inventive effort for a person skilled in the art.
Fig. 1 is an X-ray diffraction (XRD) pattern of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramics prepared in example 1 and example 5.
Fig. 2 is a cross-sectional profile of a Scanning Electron Microscope (SEM) image of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramic prepared in example 1.
FIG. 3 is a graph showing the change of dielectric constant with temperature of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramics prepared in examples 1 to 5.
Fig. 4 is a graph of the temperature dependence of the large signal piezoelectric constant d33 of the lead ytterbium niobate-lead zirconate titanate high temperature piezoceramics prepared in examples 3 and 5.
Fig. 5 is a graph of the temperature dependence of the impedance of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramic prepared in example 5.
Fig. 6 is a graph of the temperature dependence of the phase angle at resonance of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramic prepared in example 5.
Fig. 7 is a graph showing the temperature dependence of the resonance frequency temperature coefficient of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramics prepared in examples 1 to 5.
Fig. 8 is an overall flow process diagram of the present invention.
Detailed Description
The following detailed description of the present invention clearly and fully describes the technical solutions of the embodiments of the present invention, and it is apparent that the described embodiments are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
The invention provides a lead zirconate titanate-based high-temperature piezoelectric ceramic with stable temperature and a preparation method thereof by improving the temperature, and the technical scheme of the invention is as follows:
as shown in fig. 8, in one embodiment, a method for preparing a temperature-stable lead zirconate titanate-based high temperature piezoelectric ceramic is provided, comprising the steps of:
step S1, according to YbNbO 4 Stoichiometric ratio of raw materials including Yb 2 O 3 And Nb (Nb) 2 O 5 Mixing all the materials, and packagingPutting the mixture into a nylon tank, taking zirconia balls as grinding balls and absolute ethyl alcohol as a ball milling medium, fully mixing and ball milling for 18-24 hours by using a ball mill for 150-300 r/min, separating the zirconia balls, drying the raw material mixture at 80-100 ℃ for 12-24 hours, grinding by using a mortar, and sieving by using a 80-mesh sieve; placing the sieved powder into an alumina crucible, capping, calcining at 1000-1100 ℃ for 5-10 hours to synthesize YbNbO 4 Precursor powder;
step S2, according to (1-x-y) Pb (Yb 1/2 Nb 1/2 )O 3 -yPbZrO 3 -xPbTiO 3 Preparing raw materials according to a stoichiometric ratio (x is 0.4-0.6, y is 0.4-0.6), uniformly mixing all the weighed raw materials, filling the mixture into a nylon tank, fully mixing and ball milling for 18-24 hours by taking zirconium balls as grinding balls and absolute ethyl alcohol as ball milling media, separating the zirconium balls, drying the raw material mixture at 80-100 ℃ for 12-24 hours, grinding the raw material mixture by using a mortar, and sieving the raw material mixture by using an 80-mesh sieve; specifically, in step S2, according to 0.2Pb (Yb 1/2Nb 1/2) O3-0.4PbZrO3-0.4PbTiO3, zrO214.6218g with purity of 99.9%PbO 66.2130g,YbNbO4 9.7883g and 99.9% and TiO2 9.4770g with purity of 99.9% are weighed as raw materials, respectively.
Step S3, placing the raw material mixture after being sieved by the 80-mesh sieve in the step S2 into an alumina crucible, compacting by an agate rod to ensure that the compacted density is 1.5g/cm 3 Capping, presintering for 4-6 hours at 750-800 ℃, naturally cooling to room temperature, and grinding by using a mortar to obtain presintering powder;
s4, putting the presintered powder into a nylon pot, fully mixing and ball-milling for 12-24 hours by taking zirconium balls as grinding balls and absolute ethyl alcohol as ball-milling media, separating the zirconium balls, drying the presintered powder at 80-100 ℃ for 12-24 hours, grinding by using a mortar, and sieving by a 180-mesh sieve;
step S5, firstly pressing the presintered powder after 180-mesh screening into a cylindrical blank by a powder tablet press, and then carrying out cold isostatic pressing for 15-20 minutes under the pressure of 200-300 MPa;
s6, placing the cylindrical blank on a zirconia flat plate, placing the zirconia flat plate in an alumina closed sagger, heating to 1100-1200 ℃ at a heating rate of 2-5 ℃/min, sintering for 3-5 hours, and naturally cooling to room temperature along with a furnace;
step S7, firstly, selecting one of the surfaces of the ceramic sintered in the step S6, polishing with 320-mesh sand paper, then polishing with 800-mesh sand paper, finally polishing with 1500-mesh sand paper and silicon carbide to a thickness of 0.5-0.6 mm, and wiping with alcohol; in one embodiment, in step S7, the sintering temperature is 1100-1300 ℃ and the sintering time is 1-5 hours.
And S8, coating silver paste with the thickness of 0.01-0.03 mm on the upper and lower surfaces of the ceramic polished in the step S7, placing the ceramic in a resistance furnace, preserving heat at 600 ℃ for 30 minutes, and naturally cooling to room temperature to prepare the PYN-PZT piezoelectric ceramic material. In one embodiment, the PYN-PZT piezoelectric ceramic material has a thickness of 0.8-1.5mm and a diameter of 8-15mm.
Example 2
The difference from example 1 is that Pb having a purity of 99.9% was weighed out separately 3 O 4 67.4225g，YbNbO 4 9.7345g of ZrO with a purity of 99.9% 2 11.6227g and 99.9% pure TiO 2 11.3099g of the mixture was mixed uniformly to prepare 0.2Pb (Yb) 1/2 Nb 1/2 )O 3 -0.32PbZrO 3 -0.48PbTiO 3 A piezoelectric ceramic material.
Example 3
The difference from example 1 is that Pb having a purity of 99.9% was weighed out separately 3 O 4 67.5088g，YbNbO 4 9.7470g of ZrO with a purity of 99.9% 2 11.2739g and 99.9% pure TiO 2 11.5603g of the mixture was mixed uniformly to prepare 0.2Pb (Yb) 1/2 Nb 1/2 )O 3 -0.31PbZrO 3 -0.49PbTiO 3 A piezoelectric ceramic material.
Example 4
The difference from example 1 is that Pb having a purity of 99.9% was weighed out separately 3 O 4 67.5952g，YbNbO 4 9.7595g of ZrO with a purity of 99.9% 2 10.9242g and 99.9% pure TiO 2 11.8113g of the mixture was mixed uniformly to prepare 0.2Pb (Yb) 1/2 Nb 1/2 )O 3 -0.30PbZrO 3 -0.50PbTiO 3 A piezoelectric ceramic material.
Example 5
The difference from example 1 is that Pb having a purity of 99.9% was weighed out separately 3 O 4 67.7698g，YbNbO 4 9.7846g of ZrO with a purity of 99.9% 2 10.2221g and 99.9% pure TiO 2 12.3153g of the mixture was mixed uniformly to prepare 0.2Pb (Yb) 1/2 Nb 1/2 )O 3 -0.28PbZrO 3 -0.52PbTiO 3 A piezoelectric ceramic material.
Example 6
A temperature-stable lead zirconate titanate-based high temperature piezoelectric ceramic having a molecular formula of (1-x-y) Pb (Yb) is provided 1/2 Nb 1/2 )O 3 -yPbZrO 3 -xPbTiO 3 Wherein, the value range of x is 0.4-0.6, and the value range of y is 0.4-0.6.
In one embodiment, the molecular formula is (1-x-y) Pb (Yb 1/2 Nb 1/2 )O 3 -yPbZrO 3 -xPbTiO 3 X=0.28, y=0.52, and the temperature coefficient of resonance frequency (Δf) r /f r 25 ℃ from room temperature to 300 ℃ below 0.5%.
In one embodiment, the large signal piezoelectric coefficient (d 33 * ) 400-750 pm/V.
In one embodiment, the small-signal piezoelectric coefficient (d 33 ) 210-485 pC/N.
In one embodiment, the lead zirconate titanate-based high temperature piezoelectric ceramic has a Curie temperature of 350 ℃ to 450 DEG C
In one embodiment, the lead zirconate titanate-based high temperature piezoceramic crystal structure is a perovskite structure.
Fig. 1 is an X-ray diffraction (XRD) pattern of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramics prepared in example 1 and example 5. The prepared piezoelectric ceramics are all of pure perovskite structures and have no second phase.
Fig. 2 is a cross-sectional profile of a Scanning Electron Microscope (SEM) image of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramic prepared in example 1. The prepared piezoelectric ceramic has uniform grain size and compact structure. FIG. 3 is a graph showing the change of dielectric constant with temperature of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramics prepared in examples 1 to 5. The prepared piezoelectric ceramics have high Curie temperature.
FIG. 4 is a large-signal piezoelectric constant d of the lead ytterbium niobate-lead zirconate titanate high-temperature piezoelectric ceramics prepared in examples 3 and 5 of FIG. 1 33 * A graph of the temperature dependence of (c). The piezoelectric constants of the piezoelectric ceramics of examples 3 and 5 remained substantially unchanged with an increase in temperature.
Fig. 5 is a graph of the temperature dependence of the impedance of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramic prepared in example 5. The prepared piezoelectric ceramic keeps stable resonance peak from room temperature to 350 ℃.
Fig. 6 is a graph of the temperature dependence of the phase angle at resonance of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramic prepared in example 5.
Fig. 7 is a graph showing the temperature dependence of the resonance frequency temperature coefficient of the lead ytterbium niobate-lead zirconate titanate high temperature piezoelectric ceramics prepared in examples 1 to 5. The piezoelectric ceramic of example 5 maintains a stable resonance frequency up to 300 ℃.
The piezoelectric ceramic with high temperature stability is obtained by controlling the components of the material and solving the technical problems existing in the material industrialization. Secondly, through researching components and phase structures, the problem that high-voltage electric performance, high Curie temperature and coercive field are difficult to be combined is solved, and the piezoelectric ceramic with excellent comprehensive performance is obtained, and compared with the PZT ceramic material used at present and PZT base piezoelectric ceramics of other ternary systems, the piezoelectric ceramic prepared by the invention realizes excellent Curie temperature (T) C 400 ℃ C. And piezoelectric constant (d) 33 About 450 pC/N) and high coercive field (E) C About 17.5 kV/cm). And achieves excellent temperature stability in tetragonal phase samples, its resonance frequency temperature coefficient (Δf r /f r 25℃ ) Kept below 0.5% from room temperature to 300 ℃. The prepared piezoelectric ceramics can be applied to high-temperature or high-excitation devices。
The previous description is provided to enable any person skilled in the art to make or use the present invention. Various modifications to these embodiments will be readily apparent to those skilled in the art, and the generic principles defined herein may be applied to other embodiments without departing from the spirit or scope of the invention. Thus, the present invention is not intended to be limited to the embodiments shown herein but is to be accorded the widest scope consistent with the principles and novel features disclosed herein.
Claims (10)
1. A lead zirconate titanate-based high-temperature piezoelectric ceramic with stable temperature is characterized in that: the molecular formula of the lead zirconate titanate-based high-temperature piezoelectric ceramic is (1-x-y) Pb (Yb) 1/2 Nb 1/2 )O 3 -yPbZrO 3 -xPbTiO 3 Wherein, the value range of x is 0.4-0.6, and the value range of y is 0.4-0.6.
2. A temperature-stable lead zirconate titanate-based high temperature piezoelectric ceramic according to claim 1, wherein: the molecular formula is (1-x-y) Pb (Yb) 1/2 Nb 1/2 )O 3 -yPbZrO 3 -xPbTiO 3 In the lead zirconate titanate-based high temperature piezoelectric ceramic, x=0.28, y=0.52, and the resonance frequency temperature coefficient (Δf r /f r 25 ℃ from room temperature to 300 ℃ below 0.5%.
3. A temperature-stable lead zirconate titanate-based high temperature piezoelectric ceramic according to claim 1, wherein: the lead zirconate titanate-based high-temperature piezoelectric ceramic has a large signal piezoelectric coefficient (d 33 * ) 400-750 pm/V.
4. A temperature-stable lead zirconate titanate-based high temperature piezoelectric ceramic according to claim 1, wherein: the small-signal piezoelectric coefficient (d) of the lead zirconate titanate-based high-temperature piezoelectric ceramic 33 ) 210-485 pC/N.
5. A temperature-stable lead zirconate titanate-based high temperature piezoelectric ceramic according to claim 1, wherein: the Curie temperature of the lead zirconate titanate-based high-temperature piezoelectric ceramic is 350-450 ℃.
6. A temperature-stable lead zirconate titanate-based high temperature piezoelectric ceramic according to claim 1, wherein: the lead zirconate titanate-based high-temperature piezoelectric ceramic crystal structure is a perovskite structure.
7. A method for preparing a temperature-stable lead zirconate titanate-based high temperature piezoelectric ceramic according to claim 1, comprising the steps of:
step S1, according to YbNbO 4 Stoichiometric ratio of raw materials including Yb 2 O 3 And Nb (Nb) 2 O 5 Mixing all the weighed raw materials uniformly, filling the mixture into a nylon pot, taking zirconia balls as grinding balls and absolute ethyl alcohol as ball milling media, fully mixing and ball milling for 18-24 hours by using a ball mill for 150-300 r/min, separating the zirconia balls, drying the raw material mixture at 80-100 ℃ for 12-24 hours, grinding by using a mortar, and sieving by a 80-mesh sieve; placing the sieved powder into an alumina crucible, capping, calcining at 1000-1100 ℃ for 5-10 hours to synthesize YbNbO 4 Precursor powder;
step S2, according to (1-x-y) Pb (Yb 1/2 Nb 1/2 )O 3 -yPbZrO 3 -xPbTiO 3 Preparing raw materials according to a stoichiometric ratio (x is 0.4-0.6, y is 0.4-0.6), uniformly mixing all the weighed raw materials, filling the mixture into a nylon tank, fully mixing and ball milling for 18-24 hours by taking zirconium balls as grinding balls and absolute ethyl alcohol as ball milling media, separating the zirconium balls, drying the raw material mixture at 80-100 ℃ for 12-24 hours, grinding the raw material mixture by using a mortar, and sieving the raw material mixture by using an 80-mesh sieve;
step S3, placing the raw material mixture after being sieved by the 80-mesh sieve in the step S2 into an alumina crucible, compacting by an agate rod to ensure that the compacted density is 1.5g/cm 3 Capping, presintering for 4-6 hours at 750-800 ℃, naturally cooling to room temperature, and grinding by using a mortar to obtain presintering powder;
s4, putting the presintered powder into a nylon pot, fully mixing and ball-milling for 12-24 hours by taking zirconium balls as grinding balls and absolute ethyl alcohol as ball-milling media, separating the zirconium balls, drying the presintered powder at 80-100 ℃ for 12-24 hours, grinding by using a mortar, and sieving by a 180-mesh sieve;
step S5, firstly pressing the presintered powder after 180-mesh screening into a cylindrical blank by a powder tablet press, and then carrying out cold isostatic pressing for 15-20 minutes under the pressure of 200-300 MPa;
s6, placing the cylindrical blank on a zirconia flat plate, placing the zirconia flat plate in an alumina closed sagger, heating to 1100-1200 ℃ at a heating rate of 2-5 ℃/min, sintering for 3-5 hours, and naturally cooling to room temperature along with a furnace;
step S7, firstly, selecting one of the surfaces of the ceramic sintered in the step S6, polishing with 320-mesh sand paper, then polishing with 800-mesh sand paper, finally polishing with 1500-mesh sand paper and silicon carbide to a thickness of 0.5-0.6 mm, and wiping with alcohol;
and S8, coating silver paste with the thickness of 0.01-0.03 mm on the upper and lower surfaces of the ceramic polished in the step S7, placing the ceramic in a resistance furnace, preserving heat at 600 ℃ for 30 minutes, and naturally cooling to room temperature to prepare the PYN-PZT piezoelectric ceramic material.
8. The method for preparing the lead zirconate titanate-based high-temperature piezoelectric ceramic with stable temperature according to claim 7, wherein the method comprises the following steps: in the step S7, the sintering temperature is 1100-1300 ℃ and the sintering time is 1-5 hours.
9. The method for preparing the lead zirconate titanate-based high-temperature piezoelectric ceramic with stable temperature according to claim 7, wherein the method comprises the following steps: the thickness of the PYN-PZT piezoelectric ceramic material is 0.8-1.5mm, and the diameter is 8-15mm.
10. The method for preparing the lead zirconate titanate-based high-temperature piezoelectric ceramic with stable temperature according to claim 7, wherein the method comprises the following steps: in the step S2, the material is prepared according to 0.2Pb (Yb 1/2 Nb 1/2 )O 3 -0.4PbZrO 3 -0.4PbTiO 3 Respectively weighing the pure componentsPbO 66.2130g with 99.9% and YbNbO 4 9.7883g of ZrO with a purity of 99.9% 2 14.6218g and 99.9% pure TiO 2 9.4770g as raw material.
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