CN116082034B - Bismuth sodium titanate-based high-entropy ceramic material with high energy storage characteristic, and preparation method and application thereof - Google Patents
Bismuth sodium titanate-based high-entropy ceramic material with high energy storage characteristic, and preparation method and application thereof Download PDFInfo
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- FSAJRXGMUISOIW-UHFFFAOYSA-N bismuth sodium Chemical compound [Na].[Bi] FSAJRXGMUISOIW-UHFFFAOYSA-N 0.000 title claims abstract description 45
- 229910010293 ceramic material Inorganic materials 0.000 title claims abstract description 39
- 238000004146 energy storage Methods 0.000 title claims abstract description 36
- 238000002360 preparation method Methods 0.000 title abstract description 8
- 229910002115 bismuth titanate Inorganic materials 0.000 claims abstract description 22
- 239000011734 sodium Substances 0.000 claims abstract description 18
- 239000000203 mixture Substances 0.000 claims abstract description 5
- 239000000126 substance Substances 0.000 claims abstract description 5
- 239000000843 powder Substances 0.000 claims description 37
- 239000000919 ceramic Substances 0.000 claims description 32
- 238000000034 method Methods 0.000 claims description 14
- 238000000498 ball milling Methods 0.000 claims description 10
- 238000005245 sintering Methods 0.000 claims description 9
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 8
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical group [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 7
- 229910052760 oxygen Inorganic materials 0.000 claims description 7
- 239000001301 oxygen Substances 0.000 claims description 7
- 230000015556 catabolic process Effects 0.000 claims description 6
- 229920003023 plastic Polymers 0.000 claims description 6
- 239000004033 plastic Substances 0.000 claims description 6
- 230000032683 aging Effects 0.000 claims description 5
- 239000002994 raw material Substances 0.000 claims description 5
- 238000003756 stirring Methods 0.000 claims description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical group CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 4
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 4
- 239000007864 aqueous solution Substances 0.000 claims description 4
- 239000011230 binding agent Substances 0.000 claims description 4
- 238000001354 calcination Methods 0.000 claims description 4
- 238000000748 compression moulding Methods 0.000 claims description 4
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 4
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims description 3
- 239000003985 ceramic capacitor Substances 0.000 claims description 3
- 230000005684 electric field Effects 0.000 claims description 3
- 238000000227 grinding Methods 0.000 claims description 3
- 238000005303 weighing Methods 0.000 claims description 3
- 229910052726 zirconium Inorganic materials 0.000 claims description 3
- 229910015902 Bi 2 O 3 Inorganic materials 0.000 claims description 2
- 238000005469 granulation Methods 0.000 claims description 2
- 230000003179 granulation Effects 0.000 claims description 2
- 238000004321 preservation Methods 0.000 claims description 2
- 230000000630 rising effect Effects 0.000 claims description 2
- 238000002441 X-ray diffraction Methods 0.000 description 6
- 239000000463 material Substances 0.000 description 6
- 230000010287 polarization Effects 0.000 description 5
- 239000004677 Nylon Substances 0.000 description 4
- 229920001778 nylon Polymers 0.000 description 4
- 239000003990 capacitor Substances 0.000 description 3
- 238000007873 sieving Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- 229910010413 TiO 2 Inorganic materials 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 239000006104 solid solution Substances 0.000 description 2
- 239000012856 weighed raw material Substances 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000003111 delayed effect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 239000003989 dielectric material Substances 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000001755 magnetron sputter deposition Methods 0.000 description 1
- 239000008204 material by function Substances 0.000 description 1
- 239000011812 mixed powder Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000000643 oven drying Methods 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 238000007650 screen-printing Methods 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 238000003746 solid phase reaction Methods 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 238000004506 ultrasonic cleaning Methods 0.000 description 1
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- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
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Abstract
The invention relates to a sodium bismuth titanate-based high-entropy ceramic material with high energy storage property, and a preparation method and application thereof. The chemical composition of the bismuth sodium titanate-based high-entropy ceramic material is (1-x) (Bi 0.5 Na 0.5 )TiO 3 ‑x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 Where x=0.1 to 0.5, preferably x=0.15 to 0.45, more preferably x=0.35 to 0.45.
Description
Technical Field
The invention relates to a sodium bismuth titanate-based high-entropy ceramic material with high energy storage property, and a preparation method and application thereof, and belongs to the field of functional materials.
Background
With the rapid development of the electronic information industry, energy storage devices are becoming increasingly a research hotspot target. Ceramic dielectric materials are of great interest due to high power density, fast charge and discharge rates. At present, lead-free materials have become a necessary trend to replace lead-based materials, but lead-free dielectric ceramics have low energy storage density and poor stability, so that the requirements of miniaturization and integration of devices are difficult to achieve. The bismuth sodium titanate-based ceramic has large polarization intensity and has large application potential in the energy storage field, but the application of the bismuth sodium titanate-based ceramic in a dielectric capacitor is limited due to high remnant polarization intensity, low breakdown field intensity and poor stability. How to improve the energy storage characteristics, the temperature, the frequency, the fatigue resistance and other stability of the sodium bismuth titanate-based ceramic, so that the sodium bismuth titanate-based ceramic meets the practical application requirements is a research difficult problem to be solved urgently.
Disclosure of Invention
Aiming at the defects, the invention provides a sodium bismuth titanate-based high-entropy ceramic material with high energy storage property, and a preparation method and application thereof.
In a first aspect, the invention provides a sodium bismuth titanate-based high-entropy ceramic material, the chemical composition of the sodium bismuth titanate-based high-entropy ceramic material is (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 Where x=0.1 to 0.5, preferably x=0.15 to 0.45, more preferably x=0.35 to 0.45.
In the invention, a high-entropy component is introduced, and a bismuth sodium titanate-based high-entropy structure is constructed by a method of equimolar increasing the element quantity on the A site of perovskite and introducing Nb element on the B site. In particular, ag incorporating large ionic radii + 、K + The ion aggravates lattice distortion to further increase site disorder, reduce remnant polarization, induce generation and enhancement of relaxation characteristics, reduce crystal grains, increase breakdown field strength, and further obtain a novel relaxation ferroelectric material with excellent energy storage characteristics. In particular, the bismuth sodium titanate-based high-entropy ceramic material has a single perovskite structure.
Preferably, the breakdown electric field of the bismuth sodium titanate-based high-entropy ceramic material is 344.86-405.49 kV/cm.
Preferably, the recoverable energy storage density of the bismuth sodium titanate-based high-entropy ceramic material is 5.531-6.252J/cm 3 。
Preferably, the energy storage efficiency of the bismuth sodium titanate-based high-entropy ceramic material is 79.71-83.94%.
In a second aspect, the invention provides a preparation method of a sodium bismuth titanate-based high-entropy ceramic material, which comprises the following steps:
(1) According to the stoichiometric ratio (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 Weighing Bi 2 O 3 Powder, tiO 2 Powder, na 2 CO 3 Powder, srCO 3 Powder, caCO 3 Powder body and BaCO 3 Powder, ag 2 O powder, K 2 CO 3 Powder, nb 2 O 5 The powder is taken as raw material powder and mixed, and the ceramic powder is obtained through calcination and ball milling;
(2) Placing the ceramic powder into a stirring mill for fine grinding again, and granulating, aging and compression molding to obtain a ceramic green body;
(3) And (3) performing plastic removal and sintering on the ceramic green body to obtain the sodium bismuth titanate-based high-entropy ceramic material.
Preferably, in the step (1), the purity of the raw material powder is more than 99%; the ball milling parameters include: the ball milling medium is absolute ethyl alcohol and zirconia balls with the diameter of 6mm, the ball milling rotating speed is 300-360 revolutions per minute, and the time is 4-8 hours;
the atmosphere of the closed calcination is oxygen atmosphere, the temperature is 950-1050 ℃, and the time is 2-4 hours.
Preferably, in the step (2), the rotation speed of the stirring mill is 400-500 r/min, the diameter of the zirconium ball is 1mm, and the time is 4-6 h;
the binder used for granulation is polyvinyl alcohol aqueous solution, and the addition amount of the binder is 5-7% of the mass of the ceramic powder;
the aging time is 18-24 hours.
Preferably, in the step (3), the temperature of plastic discharge is 650-800 ℃ and the time is 1-3 hours;
the sintering atmosphere is oxygen atmosphere, the sintering temperature is 1100-1200 ℃, and the heat preservation time is 2-3 hours; preferably, the temperature rising rate of the sintering is 2-4 ℃/min.
In a third aspect, the present invention provides an energy storage ceramic element comprising: the bismuth sodium titanate-based high-entropy ceramic material and the electrode distributed on the surface of the bismuth sodium titanate-based high-entropy ceramic material.
In a fourth aspect, the present invention provides an application of a sodium bismuth titanate based high entropy ceramic material in a multilayer ceramic capacitor (MLCC).
The beneficial effects are that:
(1-x) (Bi) prepared by the method of the present invention 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 (x=0.15-0.45) the perovskite lattice distortion is further increased by introducing a high entropy component to regulate the a-site disorder of the perovskite. Not only induces the relaxation characteristic, obtains excellent energy storage performance, but also has stable preparation process, is green and environment-friendly, and is a powerful candidate material for the energy storage capacitor.
Drawings
FIG. 1 is (1-x) (Bi) 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 XRD pattern of the ceramic;
FIG. 2 is (1-x) (Bi) 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 A P-E curve of the ceramic;
FIG. 3 is (1-x) (Bi) 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 The energy storage characteristic parameter of the ceramic is changed along with x.
Detailed Description
The invention is further illustrated by the following embodiments, which are to be understood as merely illustrative of the invention and not limiting thereof.
In the present disclosure, the chemical composition of the bismuth sodium titanate-based high-entropy ceramic material is (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 X=0.15 to 0.45. The high-entropy component of the invention is designed independently and forms a single phaseA total solid solution. In particular, ag+ and k+ have large ionic radii, which may lead to an increase in lattice distortion, thereby leading to improvements in relaxation characteristics and energy storage characteristics. In the invention, besides forming local high entropy at the A position, nb element is introduced at the B position, so that the disorder degree of lattice points is further increased.
In the invention, the sodium bismuth titanate-based high-entropy ceramic material is prepared by using a solid phase reaction method under an oxygen atmosphere. The preparation method comprises the steps of proportioning, ball milling, calcining to obtain pre-synthesized powder, and carrying out fine grinding, granulating, aging, compression molding, sintering and the like to obtain the sodium bismuth titanate-based ceramic sample. The material has the advantages of excellent performance, stable process and environment friendliness, and is a powerful candidate material for the energy storage capacitor. The raw materials used comprise Bi with the purity of more than 99 percent 2 O 3 、TiO 2 、Na 2 CO 3 、SrCO 3 、CaCO 3 、BaCO 3 、Ag 2 O、K 2 CO 3 、Nb 2 O 5 And (3) powder.
In the invention, a ferroelectric analyzer is adopted to test the breakdown electric field of the sodium bismuth titanate-based high-entropy ceramic material with high energy storage property to be 344.86-405.49 kV/cm.
In the invention, a ferroelectric analyzer is adopted to test the energy storage density 5.531-6.252J/cm of the sodium bismuth titanate-based high-entropy ceramic material with high energy storage property 3 。
According to the invention, the ferroelectric analyzer is adopted to test that the energy storage efficiency of the sodium bismuth titanate-based high-entropy ceramic material with high energy storage property is 79.71-83.94%.
The present invention will be further illustrated by the following examples. It is also to be understood that the following examples are given solely for the purpose of illustration and are not to be construed as limitations upon the scope of the invention, since numerous insubstantial modifications and variations will now occur to those skilled in the art in light of the foregoing disclosure. The specific process parameters and the like described below are also merely examples of suitable ranges, i.e., one skilled in the art can make a suitable selection from the description herein and are not intended to be limited to the specific values described below. The following examples and comparative examples are not particularly limitedIt is indicated that the Bi with the purity of more than 99 percent is used 2 O 3 、TiO 2 、Na 2 CO 3 、SrCO 3 、CaCO 3 、BaCO 3 、Ag 2 O、K 2 CO 3 、Nb 2 O 5 The powder is prepared according to a chemical formula.
Example 1: (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 ,x=0.35
(1) Weighing the weighed raw materials, putting the weighed raw materials into a nylon pot, taking zirconia balls and absolute ethyl alcohol as media, and putting the nylon pot on a planetary ball mill for mixing for 4 hours; sieving with 40 mesh nylon sieve after oven drying, and pressing the sieved mixed powder into cylinder with diameter of 10cm x height of 6cm on a press; synthesizing for 2 hours at 1000 ℃ under the condition of oxygen introduction, and then crushing and sieving with a 40-mesh sieve to obtain ceramic pre-synthesized powder;
(2) Putting the obtained powder into a nylon pot, performing secondary ball milling for 6 hours by taking the zirconia balls and the absolute ethyl alcohol as media in the step (1), and drying in a baking oven to obtain ceramic powder; the obtained powder was placed in a stirring mill, and finely ground using zirconium balls having a diameter of 1 mm.
(3) Adding a polyvinyl alcohol aqueous solution with the concentration of 6wt% into the ground ceramic powder, wherein the addition amount of the polyvinyl alcohol aqueous solution is 5% of the mass of the ceramic powder, uniformly granulating, sieving with a 40-mesh sieve, performing compression molding to obtain a small cylinder with the size of 13mm multiplied by 1mm, and performing plastic discharge;
(4) Placing the blank after plastic discharge in a muffle furnace cavity in oxygen atmosphere, heating to 1160 ℃ at a heating rate of 2 ℃/min, preserving heat for 2 hours, and naturally cooling along with the furnace.
(5) After processing and ultrasonic cleaning, silver electrodes were plated by screen printing and fired at 650 ℃ for 30 minutes. And plating a gold electrode by adopting a magnetron sputtering method.
Figure 1 shows the X-ray diffraction pattern of example 1. The ceramic was ground, polished, electrode plated on both sides, and tested for electrical properties, and the P-E curves and energy storage parameters of example 1 are shown in fig. 2 and 3.
Example 2: (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 ,x=0.40
The procedure was the same as in example 1, except that x was 0.40.
Figure 1 shows the X-ray diffraction pattern of example 2. The ceramic was ground, polished, electrode plated on both sides, and tested for electrical properties, and the P-E curves and energy storage parameters of example 2 are shown in fig. 2 and 3.
Example 3: (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 ,x=0.45
The procedure was the same as in example 1, except that x was 0.45.
Figure 1 shows the X-ray diffraction pattern of example 3. The ceramic was ground, polished, electrode plated on both sides, and tested for electrical properties, and the P-E curves and energy storage parameters of example 3 are shown in fig. 2 and 3.
Example 4: (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 ,x=0.15。
The procedure was the same as in example 1, except that x was 0.15.
Figure 1 shows the X-ray diffraction pattern of example 4. The ceramic was ground, polished, electrode plated on both sides, and tested for electrical properties, and the P-E curves and energy storage parameters of example 4 are shown in fig. 2 and 3.
Example 5: (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 ,x=0.25。
The procedure was the same as in example 4, except that x was 0.25.
Figure 1 shows the X-ray diffraction pattern of example 5. The ceramic was ground, polished, electrode plated on both sides, and tested for electrical properties, and the P-E curves and energy storage parameters of example 5 are shown in fig. 2 and 3.
FIG. 1 is an XRD plot of the sodium bismuth titanate based high entropy ceramic materials prepared in examples 1-5. It can be seen that (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 The single-phase perovskite structure shows that all elements enter lattice sites, and the A-site local high entropy is formed.
FIG. 2 is a P-E curve of the sodium bismuth titanate based high entropy ceramic material prepared in examples 1-5. With a high entropy component (Sr) 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 The P-E curve of the ceramic shows regular change, the electric hysteresis loop is thinned, the residual polarization intensity is reduced, the polarization response is obviously delayed, and the relaxation characteristic is obviously generated and enhanced.
FIG. 3 is a graph showing the energy storage characteristics of the sodium bismuth titanate based high entropy ceramic materials prepared in examples 1-5 as a function of the composition. It can be seen that the energy storage density W can be recovered rec Breakdown field strength E b The sum efficiency η increases with the increase of the solid solution amount of the high-entropy component and reaches an optimum value, W, at example 2 (x=0.40) rec 、E b And eta are respectively 6.252J/cm 3 405.49kV/cm, 80.95%. The key energy storage parameters of each sample are shown in table 1, and the key energy storage parameters have great application potential in the field of multilayer ceramic capacitors.
Table 1 shows the energy storage characteristic parameters of the sodium bismuth titanate based high entropy ceramic material:
x | W rec (J/cm 3 ) | E b (kV/cm) | η(%) | |
example 1 | 0.35 | 5.621 | 344.86 | 79.70 |
Example 2 | 0.40 | 6.252 | 405.49 | 80.95 |
Example 3 | 0.45 | 5.531 | 397.06 | 83.94 |
Example 4 | 0.15 | 2.175 | 142.5 | 55.51 |
Example 5 | 0.25 | 3.65 | 214.73 | 74.39 |
。
Claims (9)
1. A bismuth sodium titanate-based high-entropy ceramic material is characterized in that the chemical composition of the bismuth sodium titanate-based high-entropy ceramic material is (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 Wherein x=0.35 to 0.45.
2. The bismuth sodium titanate based high entropy ceramic material according to claim 1, wherein the bismuth sodium titanate based high entropy ceramic material has a single perovskite structure.
3. The bismuth sodium titanate based high entropy ceramic material according to claim 1 or 2, wherein the breakdown electric field of the bismuth sodium titanate based high entropy ceramic material is 344.86-405.49 kV/cm;
the recoverable energy storage density of the bismuth sodium titanate-based high-entropy ceramic material is 5.531-6.252J/cm 3 ;
The energy storage efficiency of the bismuth sodium titanate-based high-entropy ceramic material is 79.71-83.94%.
4. A method for preparing the sodium bismuth titanate-based high-entropy ceramic material as claimed in any one of claims 1 to 3, comprising:
(1) According to the stoichiometric ratio (1-x) (Bi 0.5 Na 0.5 )TiO 3 -x(Sr 0.2 Ca 0.2 Ba 0.2 Ag 0.2 K 0.2 )(Ti 0.6 Nb 0.4 )O 3 Weighing Bi 2 O 3 Powder, tiO 2 Powder, na 2 CO 3 Powder, srCO 3 Powder, caCO 3 Powder body and BaCO 3 Powder, ag 2 O powder, K 2 CO 3 Powder, nb 2 O 5 The powder is taken as raw material powder and mixed, and calcinedFiring and ball milling to obtain ceramic powder;
(2) Placing the ceramic powder into a stirring mill for fine grinding again, and granulating, aging and compression molding to obtain a ceramic green body;
(3) And (3) performing plastic removal and sintering on the ceramic green body to obtain the sodium bismuth titanate-based high-entropy ceramic material.
5. The method according to claim 4, wherein in the step (1), the purity of the raw material powder is > 99%; the ball milling parameters include: the ball milling medium is absolute ethyl alcohol and zirconia balls with the diameter of 6mm, the ball milling rotating speed is 300-360 revolutions per minute, and the time is 4-8 hours;
the calcining atmosphere is oxygen atmosphere, the temperature is 950-1050 ℃, and the time is 2-4 hours.
6. The method according to claim 4, wherein in the step (2), the rotation speed of the stirring mill is 400-500 rpm, the diameter of the zirconium balls is 1mm, and the time is 4-6 hours;
the binder used for granulation is polyvinyl alcohol aqueous solution, and the addition amount of the binder is 5-7% of the mass of the ceramic powder;
the aging time is 18-24 hours.
7. The method according to any one of claims 4 to 6, wherein in the step (3), the temperature of the plastic discharge is 650 to 800 ℃ for 1 to 3 hours;
the sintering atmosphere is oxygen atmosphere, the sintering temperature is 1100-1200 ℃, and the heat preservation time is 2-3 hours; the temperature rising rate of the sintering is 2-4 ℃/min.
8. An energy storage ceramic element comprising: a bismuth sodium titanate based high entropy ceramic material as claimed in any one of claims 1 to 3, an electrode distributed on the surface of the bismuth sodium titanate based high entropy ceramic material.
9. Use of the sodium bismuth titanate based high entropy ceramic material as defined in any one of claims 1-3 in a multilayer ceramic capacitor.
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