CN113292329B - Bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material and preparation method and application thereof - Google Patents

Bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material and preparation method and application thereof Download PDF

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CN113292329B
CN113292329B CN202110698422.0A CN202110698422A CN113292329B CN 113292329 B CN113292329 B CN 113292329B CN 202110698422 A CN202110698422 A CN 202110698422A CN 113292329 B CN113292329 B CN 113292329B
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barium titanate
bismuth ferrite
ball milling
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陈建国
仝宾宾
程晋荣
沈昕
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University of Shanghai for Science and Technology
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Abstract

The invention provides a bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material and a preparation method and application thereof, belonging to the technical field of high-temperature piezoelectric materials. According to the method, the bismuth ferrite-barium titanate coarse powder and the bismuth ferrite-barium titanate fine powder with the particle size difference of 700 nm-1.2 mu m are used as raw materials, the bismuth ferrite-barium titanate is prepared from the mixed powder with different particle sizes, and the surface tension of large particles and small particles is larger than that of the same particles when the large particles and the small particles are in contact, so that the bismuth ferrite-barium titanate is more favorable for the growth of crystal grains, the relative density of a ceramic material is increased, the porosity is reduced, the dielectric constant and the piezoelectric coefficient of the ceramic material are further improved, the dielectric property is improved, the dielectric loss tan delta is reduced, the insulating property of the ceramic is improved, the leakage current is reduced, and the piezoelectric ceramic has excellent piezoelectric property. The results of the examples show that the piezoelectric constant of the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material prepared by the invention reaches 200 pC/N.

Description

Bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material and preparation method and application thereof
Technical Field
The invention relates to the technical field of high-temperature piezoelectric materials, in particular to a bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material and a preparation method and application thereof.
Background
The main research system in high-temperature piezoelectric materials is Pb (Zr)xTi1-x)O3Lead-based piezoelectric ceramics represented by (x ═ 0.52), niobate-based lead-free piezoelectric ceramics, and various bismuth layer structures. Among them, PZT ceramics of lead zirconate titanate are the most well studied among all piezoelectric ceramics and are widely used in practice. However, one disadvantage of PZT piezoelectric ceramics is that their curie temperature Tc is typically less than 400 ℃, which limits their use in high temperature applications. Meanwhile, lead-based materials pollute the environment in the processes of production, use and waste treatment, and bring great harm to the health of organisms and human beings, people begin to put the center of gravity in searching and developing environment-friendly lead-free piezoelectric ceramics for replacing the application of the lead-based piezoelectric ceramics in transducers and sensors.
BiFeO3-BaTiO3The (BF-BT) has been widely studied for its multiferroic properties, high curie temperature (Tc 619 ℃), good thermal stability, and the like, and has potential applications in the field of piezoelectric and dielectric energy storage devices. BF-BT ceramic and lead-based piezoelectric ceramic systemSimilarly, the compositions have excellent piezoelectric and ferroelectric properties when they are located near the Morphotropic Phase Boundary (MPB), but due to the presence of Bi in BF-BT ceramics during sintering2O3Volatile and Fe3+The valence variation and the like of the ceramic sample cause the problems of high defect ion concentration, large dielectric loss tan delta, low piezoelectric performance and the like of the ceramic sample, and the application of the ceramic sample in a piezoelectric device is greatly limited. Therefore, it is necessary to further reduce the leakage current and the dielectric loss tan δ of BF-BT ceramic, thereby realizing high temperature and high electric field polarization and improving the piezoelectric performance.
Disclosure of Invention
The invention aims to provide a bismuth ferrite-barium titanate binary high-temperature piezoelectric 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 preparation method of a bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material, which comprises the following steps:
mixing bismuth ferrite-barium titanate powder with a first ball milling medium, and performing first ball milling to obtain bismuth ferrite-barium titanate coarse powder, wherein the particle size of the bismuth ferrite-barium titanate coarse powder is 800 nm-1.5 mu m;
mixing bismuth ferrite-barium titanate powder with a second ball milling medium, and performing second ball milling to obtain bismuth ferrite-barium titanate fine powder, wherein the particle size of the bismuth ferrite-barium titanate fine powder is 100-800 nm;
mixing the bismuth ferrite-barium titanate coarse powder and the bismuth ferrite-barium titanate fine powder to obtain mixed powder; and mixing the mixed powder with a binder, and sequentially performing granulation, isostatic pressing, binder removal and sintering to obtain the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material.
Preferably, the preparation method of the bismuth ferrite-barium titanate powder comprises the following steps:
adding Bi2O3、Fe2O3、TiO2、BaCO3、MnO2Mixing with water, and sequentially and alternately performing ball milling and calcination on the obtained mixed material to obtain the bismuth ferrite-barium titanate powder.
Preferably, the chemical composition of the bismuth ferrite-barium titanate powder is (1-x) BiFeO3-xBaTiO3Wherein, 0<x<1。
Preferably, the rotation speed of each ball milling is 250-400 r/min independently, and the time of each ball milling is 6-8 h independently.
Preferably, the temperature of each time of calcination is 700-800 ℃ independently, and the heat preservation time is 3-6 hours independently; the rate of temperature rise to the temperature for each calcination was 5 ℃/min.
Preferably, the mass ratio of the bismuth ferrite-barium titanate coarse powder to the bismuth ferrite-barium titanate fine powder is (0-10): 1 and not 0.
Preferably, the first ball milling medium is zirconia balls with the diameter of 2-5 mm, the rotating speed of the first ball milling is 250-400 r/min, and the time of the first ball milling is 4-8 h; the second ball milling medium is zirconia balls with the diameter of 0.5-1.5 mm; the rotation speed of the second ball milling is 250-400 r/min, and the time of the second ball milling is 48-100 h.
Preferably, the temperature of the rubber discharge is 600-800 ℃, and the heat preservation time is 3-6 h; the heating rate of heating to the glue discharging temperature is 5 ℃/min; the sintering temperature is 950-1040 ℃, and the heat preservation time is 2-4 h.
The invention provides the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material prepared by the preparation method in the technical scheme, and the chemical composition of the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material is (1-x) BiFeO3-xBaTiO3Wherein, 0<x<1。
The invention provides the application of the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material in piezoelectric and dielectric energy storage devices.
The invention provides a preparation method of a bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material, which comprises the following steps: mixing bismuth ferrite-barium titanate powder with a first ball milling medium, and performing first ball milling to obtain bismuth ferrite-barium titanate coarse powder, wherein the particle size of the bismuth ferrite-barium titanate coarse powder is 800 nm-1.5 mu m; mixing bismuth ferrite-barium titanate powder with a second ball milling medium, and performing second ball milling to obtain bismuth ferrite-barium titanate fine powder, wherein the particle size of the bismuth ferrite-barium titanate fine powder is 100-800 nm; mixing the bismuth ferrite-barium titanate coarse powder and the bismuth ferrite-barium titanate fine powder to obtain mixed powder; and mixing the mixed powder with a binder, and sequentially performing granulation, isostatic pressing, binder removal and sintering to obtain the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material. According to the method, the bismuth ferrite-barium titanate coarse powder and the bismuth ferrite-barium titanate fine powder with the particle size difference of 700 nm-1.2 mu m are used as raw materials, the bismuth ferrite-barium titanate is prepared from the mixed powder with different particle sizes, and the surface tension is larger than that of the same particles when large particles and small particles are contacted, so that the growth of crystal grains is facilitated, the relative density of a ceramic material is increased, the porosity is reduced, the dielectric constant and the piezoelectric coefficient of the ceramic material are improved, the dielectric loss tan delta is reduced, the dielectric property is improved, the insulating property of the ceramic is improved, the leakage current is reduced, and the piezoelectric ceramic has excellent piezoelectric property. The results of the examples show that the piezoelectric constant of the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material prepared by the invention reaches 200 pC/N.
Drawings
FIG. 1 is an SEM photograph of coarse bismuth ferrite-barium titanate powder and fine bismuth ferrite-barium titanate powder prepared in example 1.
Detailed Description
The invention provides a preparation method of a bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material, which comprises the following steps:
mixing bismuth ferrite-barium titanate powder with a first ball milling medium, and performing first ball milling to obtain bismuth ferrite-barium titanate coarse powder, wherein the particle size of the bismuth ferrite-barium titanate coarse powder is 800 nm-1.5 mu m;
mixing bismuth ferrite-barium titanate powder with a second ball milling medium, and performing second ball milling to obtain bismuth ferrite-barium titanate fine powder, wherein the particle size of the bismuth ferrite-barium titanate fine powder is 100-800 nm;
mixing the bismuth ferrite-barium titanate coarse powder and the bismuth ferrite-barium titanate fine powder to obtain mixed powder; and mixing the mixed powder with a binder, and sequentially performing granulation, isostatic pressing, binder removal and sintering to obtain the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material.
In the present invention, unless otherwise specified, all the starting materials required for the preparation are commercially available products well known to those skilled in the art. The ball milling process is preferably carried out in a ball milling tank, and the ball milling tank is not particularly limited in the invention and can be a ball milling tank well known in the art.
The bismuth ferrite-barium titanate powder is mixed with a first ball milling medium for first ball milling to obtain bismuth ferrite-barium titanate coarse powder, and the particle size of the bismuth ferrite-barium titanate coarse powder is 800 nm-1.5 mu m.
In the invention, the preparation method of the bismuth ferrite-barium titanate powder comprises the following steps: adding Bi2O3、Fe2O3、TiO2、BaCO3、MnO2Mixing with water, and sequentially and alternately performing ball milling and calcination on the obtained mixed material to obtain the bismuth ferrite-barium titanate powder. In the present invention, the Bi2O3、Fe2O3、 TiO2、BaCO3And MnO2Independently is preferably of analytically pure grade. In the invention, the chemical composition of the bismuth ferrite-barium titanate powder is preferably (1-x) BiFeO3-xBaTiO3Wherein, 0<x<1. In the present invention, x is preferably 0.25, 0.30 or 0.36, and Bi2O3、Fe2O3、TiO2、BaCO3And MnO2The molar ratio of (b) is preferably adjusted according to the chemical composition.
The invention is directed to the Bi2O3、Fe2O3、TiO2、BaCO3、MnO2The process of mixing with water is not particularly limited, and the feed may be carried out according to a process well known in the art. In the present invention, the Bi2O3、 Fe2O3、TiO2、BaCO3And MnO2The ratio of the total mass of (A) to the amount of water is preferably (30-50) g, (30-50) mL, and more preferably 30: 30.
In the present invention, the process of performing ball milling and calcining alternately in sequence is preferably performing ball milling, calcining, ball milling, calcining and ball milling in sequence, that is, performing ball milling three times and calcining two times.
In the invention, the medium used in each ball milling is preferably zirconia balls, and the diameters of the zirconia balls are independently preferably 5-10 mm; the Bi2O3、Fe2O3、TiO2、BaCO3And MnO2The mass ratio of the total mass of the zirconia balls to the zirconia balls is (30-50): 90-150), and the mass ratio of the zirconia balls to the total mass of the zirconia balls is more preferably 30: 90.
In the invention, the rotation speed of each ball milling is preferably 250-400 r/min independently, more preferably 300-350 r/min independently, and the time of each ball milling is preferably 6-8 h independently, more preferably 6.5-7.5 h independently.
After each ball milling is finished, the obtained ball milling material is preferably dried and sieved in sequence, and the drying process is not particularly limited and can be carried out according to the process well known in the art; the screening is preferably performed by adopting a screen of 100-120 meshes.
After sieving, the material obtained is preferably calcined according to the invention. In the invention, the temperature of each time of calcination is preferably 700-800 ℃ independently, more preferably 750 ℃, and the heat preservation time is preferably 3-6 h independently, more preferably 4-5 h; the rate of temperature rise to the temperature for each calcination is preferably 5 ℃/min.
According to the invention, the reaction is more complete by adopting two times of calcination, and the powder can be uniformly mixed again by ball milling after each calcination for calcination, so that the bismuth ferrite-barium titanate powder with uniform particle size is obtained.
After each calcination is finished, the obtained material is cooled along with a furnace, and is filtered by a 100-120-mesh screen, and then the obtained material is subjected to ball milling, calcination and ball milling in sequence according to the conditions to obtain bismuth ferrite-barium titanate powder ((1-x) BiFeO3-xBaTiO3)。
After the bismuth ferrite-barium titanate powder is obtained, the bismuth ferrite-barium titanate powder is mixed with a first ball milling medium for first ball milling. In the invention, the reagent used for the first ball milling mixing is preferably absolute ethyl alcohol, and the dosage ratio of the absolute ethyl alcohol, the bismuth ferrite-barium titanate powder and the first ball milling medium is preferably (10-15) mL:15g (30-45) g, and more preferably 15mL:15g:30 g.
In the invention, the first ball milling medium is preferably zirconia balls with the diameter of 2-5 mm, the rotating speed of the first ball milling is preferably 250-400 r/min, more preferably 300-350 r/min, and the time of the first ball milling is preferably 4-8 h, more preferably 5-6 h.
After the first ball milling is finished, the obtained ball milling material is preferably placed in a ceramic bowl to be dried, the dried material is sieved by a 100-120-mesh sieve to obtain bismuth ferrite-barium titanate coarse powder, and the particle size of the bismuth ferrite-barium titanate coarse powder is 800 nm-1.5 mu m.
After the bismuth ferrite-barium titanate powder is obtained, the bismuth ferrite-barium titanate powder is mixed with a second ball milling medium for second ball milling. In the invention, the reagent used for the second ball milling mixing is preferably absolute ethyl alcohol, and the dosage ratio of the absolute ethyl alcohol, the bismuth ferrite-barium titanate powder and the second ball milling medium is preferably (10-15) mL:15g (30-45) g, and more preferably 15mL:15g:30 g.
In the invention, the second ball milling medium is preferably zirconia balls with the diameter of 0.5-1.5 mm; the rotation speed of the second ball milling is preferably 250-400 r/min, and more preferably 300-350 r/min; the second ball milling time is preferably 48-100 h, and more preferably 60-80 h.
After the second ball milling is finished, the obtained ball milling material is preferably placed in a ceramic bowl to be dried, the dried material is sieved (100-120 meshes), and bismuth ferrite-barium titanate fine powder is obtained, wherein the particle size of the bismuth ferrite-barium titanate fine powder is 100-800 nm. The invention utilizes sieving to disperse powder.
After the bismuth ferrite-barium titanate coarse powder and the bismuth ferrite-barium titanate fine powder are obtained, the bismuth ferrite-barium titanate coarse powder and the bismuth ferrite-barium titanate fine powder are mixed to obtain mixed powder. In the present invention, the mass ratio of the bismuth ferrite-barium titanate coarse powder to the bismuth ferrite-barium titanate fine powder is preferably (0 to 10):1 and not 0, and more preferably 0.5:1, 1:1 or 10: 1. In the invention, the bismuth ferrite-barium titanate coarse powder and the bismuth ferrite-barium titanate fine powder are preferably mixed by ball milling, the ball milling mixing time is preferably 1h, the rotating speed is preferably 200-300 r/min, and the ball milling medium used for ball milling mixing is preferably zirconia balls with the diameter of 2-4 mm.
After the mixing is finished, the obtained materials are preferably dried and sieved in sequence to obtain mixed powder. The drying and sieving processes are not particularly limited in the present invention and may be performed according to processes well known in the art. The particle size of the mixed powder is not particularly limited, and the mixed powder can be obtained by sieving and dispersing the powder according to a well-known process.
After mixed powder is obtained, the mixed powder is mixed with a binder, and granulation, isostatic pressing, binder removal and sintering are sequentially carried out to obtain the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material.
In the invention, the binder is preferably polyvinyl alcohol (PVA), the concentration of the PVA is preferably 3-5 wt%, and the mass ratio of the mixed powder to the binder is preferably (0.5-1): 1, and more preferably (0.6-0.8): 1. In the present invention, the process of mixing the mixed powder with the binder is preferably to drop the binder into the mixed powder, and the dropping rate is not particularly limited in the present invention, and the dropping may be performed according to a process well known in the art; in the present invention, the dropping amount in the dropping process is not particularly limited, and the dropping may be performed by using an apparatus well known in the art, and in the embodiment of the present invention, a rubber head dropper is specifically used.
The granulation process is not particularly limited in the present invention, and may be performed according to a process known in the art. After the granulation is finished, the obtained materials are preferably pre-pressed and sieved in sequence (a 120-mesh screen), and then the obtained materials are uniaxially pressed into a disc-shaped blank with the diameter of 12mm and the thickness of 1mm, and are subjected to isostatic pressing. In the present invention, the pressure of the pre-pressing is preferably 50Mpa, and the time is preferably 10 min.
In the present invention, the pressure of the isostatic pressing is preferably 100 to 200MPa, more preferably 150MPa, and the time is preferably 10 to 30min, more preferably 15 to 25 min.
After the isostatic pressing is finished, the formed part is subjected to rubber removal, the rubber removal temperature is preferably 600-800 ℃, more preferably 650-750 ℃, and the heat preservation time is preferably 3-6 hours, more preferably 4-5 hours; the heating rate of the temperature rise to the glue discharging temperature is preferably 5 ℃/min.
After the binder removal is finished, preferably cooling along with a furnace, and sintering the obtained biscuit; the sintering temperature is preferably 950-1040 ℃, more preferably 1000 ℃, and the heat preservation time is preferably 2-4 h, more preferably 2.5-3.5 h. In the present invention, the sintering is preferably performed under sealed conditions.
The invention provides a bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material prepared by the preparation method in the technical scheme.
The invention provides the application of the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material in piezoelectric and dielectric energy storage devices. The method of the present invention is not particularly limited, and the method may be applied according to a method known in the art.
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 derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example 1
According to the chemical composition (1-x) BiFeO3-xBaTiO3X is 0.25, pure Bi will be analyzed2O3、Fe2O3、 TiO2、BaCO3And MnO2Weighing 30g of the raw materials in a required stoichiometric ratio, putting the weighed raw materials into a ball milling tank, and mixingAdding 30mL of deionized water and 90g of zirconia balls with the diameter of 5mm for ball milling for 6h under the condition that the ball milling rotating speed is 250r/min, pouring the ball milled slurry into a ceramic bowl for drying, putting the ceramic bowl into a crucible after passing through a 120-mesh screen, heating to 750 ℃ at the heating rate of 5 ℃/min, calcining for 4h, passing the obtained material through a 120-mesh screen, and carrying out ball milling, calcining and ball milling on the obtained material in sequence to obtain 0.75BiFeO3-0.25BaTiO3Synthesizing powder;
adding 15mL of absolute ethyl alcohol and 15g of 0.75BiFeO into a ball milling tank3-0.25BaTiO3Synthesizing powder and 45g of zirconia balls with the diameter of 5mm, performing ball milling for 6 hours under the condition that the ball milling rotating speed is 250r/min, pouring the obtained slurry into a ceramic bowl for drying, and then sieving by a 120-mesh sieve to obtain coarse powder with the particle size of 900 nm-1000 nm;
adding 15mL of absolute ethyl alcohol and 15g of 0.75BiFeO into a ball milling tank3-0.25BaTiO3Synthesizing powder and 45g of zirconia balls with the diameter of 1mm, performing ball milling for 48 hours under the condition that the ball milling rotating speed is 250r/min, pouring the obtained slurry into a ceramic bowl, drying, and then sieving by a 120-mesh sieve to obtain fine powder with the particle size of 300-350 nm;
performing ball milling and mixing on 1.67g of the coarse powder and 3.33g of the fine powder for 1 hour by using zirconia balls with the diameter of 4mm according to the mass ratio of 0.5:1 at the rotating speed of 250r/min, drying and sieving to obtain mixed powder;
taking 5g of the mixed powder, dropwise adding 8 drops (9g) of polyvinyl alcohol with the concentration of 5 wt% by using a rubber head dropper, granulating the obtained mixed material, pre-pressing the obtained granules at 50MPa for 10min, sieving the obtained material by using a 120-mesh sieve, pressing the obtained material by using a single shaft to obtain a disc-shaped blank with the diameter of 12mm and the thickness of 1mm, carrying out isostatic pressing on the obtained blank at 200MPa for 10min, carrying out glue discharge on the obtained formed piece, heating to 600 ℃ from room temperature at the speed of 5 ℃/min, preserving heat for 4h, cooling along with a furnace, sealing the obtained blank in a crucible, and sintering at 1000 ℃ for 2h to obtain the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material, which is recorded as 0.75BF-0.25 BT.
Example 2
The only difference from example 1 is: the same as example 1 except that x is 0.30, and it is noted as 0.70BF-0.30 BT.
Example 3
The only difference from example 1 is: the same as example 1 except that x is 0.36, and it is noted as 0.64BF-0.36 BT.
Example 4
The only difference from example 1 is: the mass ratio of the coarse powder to the fine powder was 1:1, and the same as in example 1 was repeated.
Example 5
The only difference from example 1 is: the mass ratio of the coarse powder to the fine powder was 10:1, and the same as in example 1 was repeated.
Example 6
The only difference from example 2 is: the mass ratio of the coarse powder to the fine powder was 1:1, and the same as in example 2 was repeated.
Example 7
The only difference from example 2 is: the mass ratio of the coarse powder to the fine powder was 10:1, and the same as in example 2 was repeated.
Example 8
The only difference from example 3 is that: the mass ratio of the coarse powder to the fine powder was 1:1, and the same as in example 2 was repeated.
Example 9
The only difference from example 3 is that: the mass ratio of the coarse powder to the fine powder was 10:1, and the same as in example 3.
Comparative example 1
The only difference from example 1 is: the mass ratio of the coarse powder to the fine powder was 1:0, and the same as in example 1 was repeated.
Comparative example 2
The only difference from example 2 is: the mass ratio of the coarse powder to the fine powder was 1:0, and the same as in example 2 was repeated.
Comparative example 3
The only difference from example 3 is that: the mass ratio of the coarse powder to the fine powder was 1:0, and the same as in example 3.
Performance testing
1) SEM tests were performed on the coarse powder and the fine powder prepared in example 1, respectively, and the results are shown in fig. 1; as can be seen from FIG. 1, the particle size of the coarse powder is 900 to 1000nm, and the particle size of the fine powder is 300 to 350nm, and the invention can prepare powder with the particle size difference of 700nm to 1.2 μm.
2) The ceramic samples prepared in examples 1 to 9 and comparative example 1 were subjected to performance testing, wherein the relative density of the ceramic samples was tested by the archimedes method, the dielectric properties were tested by an Agilent impedance analyzer (Agilent 4294A), after silver plating and polarization were sequentially performed on different ceramic samples, the piezoelectric constant was measured by a quasi-static piezoelectric meter, and the results are shown in tables 1 to 3:
TABLE 10.75 BF-0.25BT ceramic sample Performance Table
Figure BDA0003129459840000091
TABLE 20.70 BF-0.30BT ceramic sample Performance Table
Figure BDA0003129459840000092
Figure BDA0003129459840000101
TABLE 30.64 BF-0.36BT ceramic sample Performance Table
Figure BDA0003129459840000102
Figure BDA0003129459840000111
As can be seen from tables 1 to 3, the relative density of the ceramic sample prepared by mixing the coarse powder and the fine powder according to the present invention is increased, as compared to the ceramic material prepared by using only the coarse powder in comparative examples 1 to 3; furthermore, the dielectric constant values of the ceramic samples of different compositions gradually decrease with increasing frequency, while the dielectric loss values show the opposite trend. The dielectric constant of the ceramic sample prepared by the invention is increased, and the dielectric loss tan delta is reduced, which shows that the insulating property of the ceramic sample is improved, and the leakage current is reduced.
Furthermore, (1-x) BiFeO as compared with comparative examples 1 to 33-xBaTiO3The piezoelectric constant of the ceramic material prepared by using the mixed powder in embodiments 1 to 9 of the present invention gradually increases, and when x is 0.25, 0.30, or 0.36, the maximum value of the piezoelectric constant of the ceramic material prepared by using the mixed powder is increased by 20 to 40pC/N, which indicates that the piezoelectric performance of the ceramic material is improved by mixing powders with different grain sizes.
From the above embodiments, the invention provides a preparation method of a bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material, and the piezoelectric property of the bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material prepared by adopting mixed powder is compared with that of (1-x) BiFeO prepared only by adopting coarse powder in comparative examples 1-33-xBaTiO3The material is relatively improved, and when x is 0.25, 0.30 and 0.36, the maximum values of the piezoelectric constants of the ceramic material prepared by the mixed powder respectively reach 130pC/N, 200pC/N and 120 pC/N; and the dielectric property is obviously improved, tan delta is reduced, the insulating property of the ceramic is improved, and the leakage current is reduced.
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 (8)

1. A preparation method of a bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material is characterized by comprising the following steps:
mixing bismuth ferrite-barium titanate powder with a first ball milling medium, and performing first ball milling to obtain bismuth ferrite-barium titanate coarse powder, wherein the particle size of the bismuth ferrite-barium titanate coarse powder is 800 nm-1.5 mu m;
mixing bismuth ferrite-barium titanate powder with a second ball milling medium, and performing second ball milling to obtain bismuth ferrite-barium titanate fine powder, wherein the particle size of the bismuth ferrite-barium titanate fine powder is 100-800 nm;
mixing the bismuth ferrite-barium titanate coarse powder and the bismuth ferrite-barium titanate fine powder to obtain mixed powder; mixing the mixed powder with a binder, and sequentially performing granulation, isostatic pressing, binder removal and sintering to obtain a bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material;
the preparation method of the bismuth ferrite-barium titanate powder comprises the following steps:
adding Bi2O3、Fe2O3、TiO2、BaCO3、MnO2Mixing with water, and sequentially and alternately performing ball milling and calcination on the obtained mixed material to obtain bismuth ferrite-barium titanate powder;
the mass ratio of the bismuth ferrite-barium titanate coarse powder to the bismuth ferrite-barium titanate fine powder is (0-10): 1 and not 0.
2. The production method according to claim 1, wherein the bismuth ferrite-barium titanate powder has a chemical composition of (1-x) BiFeO3-xBaTiO3Wherein, 0<x<1。
3. The preparation method of the ball milling product according to claim 1, wherein in the process of sequentially and alternately performing the ball milling, the rotation speed of each ball milling is 250-400 r/min independently, and the time of each ball milling is 6-8 h independently.
4. The preparation method of claim 1, wherein the temperature of each calcination is 700-800 ℃ independently, and the holding time is 3-6 h independently; the rate of temperature rise to the temperature for each calcination was 5 ℃/min.
5. The preparation method of claim 1, wherein the first ball milling medium is zirconia balls with the diameter of 2-5 mm, the rotation speed of the first ball milling is 250-400 r/min, and the time of the first ball milling is 4-8 h; the second ball milling medium is zirconia balls with the diameter of 0.5-1.5 mm; the rotation speed of the second ball milling is 250-400 r/min, and the time of the second ball milling is 48-100 h.
6. The preparation method according to claim 1, wherein the temperature of the binder removal is 600-800 ℃, and the holding time is 3-6 h; the heating rate of heating to the glue discharging temperature is 5 ℃/min; the sintering temperature is 950-1040 ℃, and the heat preservation time is 2-4 h.
7. The bismuth ferrite-barium titanate binary high-temperature piezoelectric ceramic material prepared by the preparation method of any one of claims 1 to 6, which has the chemical composition of (1-x) BiFeO3-xBaTiO3Wherein, 0<x<1。
8. The use of the bismuth ferrite-barium titanate binary high temperature piezoelectric ceramic material of claim 7 in piezoelectric and dielectric energy storage devices.
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