High-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature energy storage temperature stability and near-zero hysteresis, and preparation method and application thereof

Abstract

The present invention relates to a high entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis, and its preparation method and application. The chemical composition of the high entropy perovskite relaxor ferroelectric ceramic is (Ba 0.8‑x Na x Bi 0.2 )(Ti 0.8‑ x Ta x Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3, wherein 0≤x≤0.05. The high entropy perovskite relaxor ferroelectric ceramic is at 500kV cm ‑1 Under an electric field, within the temperature range of -85°C to 220°C, the discharge energy density varies within ±(3-8%), and the energy storage efficiency varies within ±(8-15)%. Compared to existing technologies, the high-entropy ceramics of this invention not only possess high energy storage density, but also have near-100% energy storage efficiency and excellent energy storage temperature stability across both low and high temperature ranges. This makes them highly adaptable and potentially applicable in emerging high-tech fields and extreme environmental scenarios, such as electric vehicles, aerospace vehicles, and space exploration.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of dielectric energy storage ferroelectric ceramics, in particular to a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature energy storage temperature stability and near-zero hysteresis, and a preparation method and application thereof. BACKGROUND

[0002] Dielectric ceramic capacitors are known for their ultra-high power density and fast charge and discharge capability, and are considered as key components in advanced electronic devices and power systems. The lowest recoverable energy density is the biggest problem faced by ceramic capacitors. According to the dielectric energy storage theory, large polarization difference and high breakdown strength can improve the energy storage performance, and the specific implementation methods include grain refinement, control of grain orientation, domain structure regulation, improvement of electrical uniformity, defect engineering, etc. In the past decade, the discharge energy density W rec Indeed, gradual improvement has been achieved. However, with the booming development of emerging high-tech fields such as electric vehicles, aerospace vehicles and space exploration, low energy loss and wide temperature range stability and reliability are also important performance indicators that cannot be ignored. Therefore, achieving excellent comprehensive energy storage performance will be the focus of urgent attention at this stage. SUMMARY

[0003] The purpose of the present application is to provide a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature energy storage temperature stability and near-zero hysteresis, and a preparation method and application thereof. The prepared relaxor ferroelectric ceramic has excellent discharge energy density, energy storage efficiency and energy storage temperature stability.

[0004] The purpose of the present application can be achieved by the following technical solutions:

[0005] In one aspect, the present application provides a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature energy storage temperature stability and near-zero hysteresis, the chemical composition of the high-entropy perovskite relaxor ferroelectric ceramic is (Ba 0.8-x Na x Bi 0.2 )(Ti 0.8-x Ta x Mg 0.0 4Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3, wherein 0≤x≤0.05.

[0006] Preferably, the chemical composition of the high-entropy perovskite relaxor ferroelectric ceramic is (Ba 0.76 Na 0.04 Bi 0.2 )(Ti 0.76 Ta 0.04 Mg0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3, x = 0.04.

[0007] Preferably, the high-entropy perovskite relaxor ferroelectric ceramic has a discharge energy density variation of ±(3-8)% and a storage efficiency variation of ±(8-15)% in the temperature range of -85℃ to 220℃ under an electric field of 500kV cm -1

[0008] In a second aspect, the present application provides a preparation method of the high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage energy temperature stability and near-zero hysteresis, comprising the following steps:

[0009] S1, weighing raw material powders according to the stoichiometric ratio of each element in (Ba 0.8-x Na x Bi 0.2 )(Ti 0.8-x Ta x Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3;

[0010] S2, performing primary ball milling, mixing, drying and pre-sintering on the raw material powders to obtain a primary mixed powder;

[0011] S3, grinding the primary mixed powder obtained in step S2 and then performing secondary ball milling and drying to obtain a secondary mixed powder;

[0012] S4, uniformly mixing the secondary mixed powder prepared in step S3 with a solvent, a binder, a dispersant and a plasticizer to obtain a casting slurry;

[0013] S5, performing bubble removal and casting on the casting slurry prepared in step S4 to obtain a single-layer ceramic thick film;

[0014] S6, performing shearing, lamination and hot pressing on the single-layer ceramic thick film prepared in step S5 to obtain a ceramic green body;

[0015] S7, performing degreasing and sintering on the ceramic green body prepared in step S6 to obtain the high-entropy perovskite relaxor ferroelectric ceramic.

[0016] Preferably, in step S1, the raw material powders containing elements Ba and Na are carbonates corresponding to each other, and the raw material powders containing elements Zn, Mg, Al, Sn, Zr, Ti, Ta and Bi are oxides corresponding to each other. ​

[0017] Preferably, in step S2, the rotation speed of the primary ball milling is 200-600 rpm, and the time is 4-48 h.

[0018] Preferably, in step S2, the medium of the primary ball milling comprises ball stones.

[0019] Further preferably, in step S2, the mass ratio of the ball stones is 3-5:1.5-3:1 according to the diameters of 6 mm:3 mm:1 mm.

[0020] Preferably, in step S2, the solvent of the primary ball milling comprises anhydrous ethanol.

[0021] Preferably, in step S2, the mass ratio of the primary ball milling is 1:1.5-6:1-2.

[0022] Preferably, in step S2, the drying is performed at 60-150 °C for 12-48 h.

[0023] Preferably, in step S2, the pre-sintering is performed at 800-1100 °C for 1-10 h.

[0024] Preferably, in step S2, the particle size of the primary mixed powder is 1-1.6 μm.

[0025] Preferably, in step S3, the rotation speed of the secondary ball milling is 200-600 rpm, and the time is 4-48 h.

[0026] Preferably, in step S3, the medium of the secondary ball milling comprises ball stones.

[0027] Further preferably, in step S3, the mass ratio of the ball stones is 3-5:1.5-3:1 according to the diameters of 6 mm:3 mm:1 mm.

[0028] Preferably, in step S3, the solvent of the secondary ball milling comprises anhydrous ethanol.

[0029] Preferably, in step S3, the mass ratio of the secondary ball milling is 1:1.5-6:1-2.

[0030] Preferably, in step S3, the drying is performed at 60-150 °C for 12-48 h.

[0031] Preferably, in step S3, the particle size of the secondary mixed powder is 0.3-0.8 μm.

[0032] Preferably, in steps S2 and S3, the ball stones are zirconium ball stones.

[0033] Preferably, in step S4, the solvent is selected from one or more of butanone, ethanol or toluene.

[0034] Preferably, in step S4, the adhesive comprises polyvinyl butyral.

[0035] Preferably, in step S4, the dispersant is selected from one or both of tributyl phosphate and glycerol trioleate.

[0036] Preferably, in step S4, the plasticizer is selected from one or more of polyethylene glycol 400 (average molecular weight of polyethylene glycol is 400), butyl phthalate or benzyl-n-butyl-phthalate.

[0037] Preferably, in step S4, the mass ratio of the secondary mixed powder to the solvent, the adhesive, the dispersant and the plasticizer is 30-60%:30-50%:2-6%:0.8-1.2%:2-5%.

[0038] Preferably, in step S5, the bubble removal is performed by a vacuum bubble remover, and the bubble removal time is 15-25 min.

[0039] Preferably, in step S5, during the casting, the casting rate is 20-40 cm / min, and the doctor blade height is 10-40 μm, so that the thickness of the single-layer ceramic thick film is 10-30 μm.

[0040] Preferably, in step S6, the shearing is performed by a slicer to cut the single-layer ceramic thick film obtained in step S5 into a square with a side length of 10-14 mm.

[0041] Preferably, in step S6, the layering is performed on the four square single-layer ceramic thick films after shearing.

[0042] Preferably, in step S6, during the hot-pressing treatment, the hot-pressing temperature is 30-80℃, the pressure is 10-50 MPa, and the pressure holding time is 10-30 min.

[0043] Preferably, in step S7, the glue removal process is performed by heating to 400-600℃ at a heating rate of 0.1-0.5℃ / min and holding for 4-8 h, and then cooling in the furnace.

[0044] Preferably, in step S7, the sintering process is performed by heating to 1000-1250℃ at a heating and cooling rate of 1-3℃ / min and holding for 2-4 h, and then cooling in the furnace.

[0045] In a third aspect, the present application provides an application of the high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature energy storage temperature stability and near-zero hysteresis in the field of high-power energy storage components.

[0046] Preferably, the high-entropy perovskite relaxor ferroelectric ceramic can be applied to new high-tech fields and extreme environment scenarios such as electric vehicles, aerospace vehicles and space exploration.

[0047] High-entropy perovskite oxides are a new type of functional ceramic designed by adjusting the configurational entropy and atomic disorder degree of the system. The dielectric energy storage materials designed by using entropy engineering are usually relaxor ferroelectrics. The increase in atomic disorder degree caused by configurational entropy often accompanies the increase in polarization configurational disorder degree, and thus has characteristics such as extremely low loss and high breakdown strength.

[0048] In the field of dielectric energy storage, BaTiO3-BiMO3 is one of the most classic relaxor ferroelectric systems. M is composed of less than or equal to three elements. M is responsible for providing disorder, breaking long-range B-O bond coupling, and improving breakdown strength while maintaining saturated polarization strength together with Bi that creates new A-O bond coupling. Further improving the disorder degree of the system into a high-entropy system, whether it can obtain excellent comprehensive energy storage performance by using extremely disordered polarization configuration is worth further exploring.

[0049] The high-entropy perovskite relaxor ferroelectric ceramic provided by the application contains ten cations, improves the disorder degree of the system, and makes the prepared perovskite relaxor ferroelectric ceramic a high-entropy system. The synergistic effect between the ten cations further improves the comprehensive energy storage performance of the ferroelectric ceramic.

[0050] Compared with the prior art, the application has the following beneficial effects:

[0051] (1) The high-entropy perovskite relaxor ferroelectric ceramic provided by the application has ultra-wide temperature energy storage temperature stability (ΔW rec = ± 4.8%, -85℃ ~ 220℃), high energy storage efficiency (97.8%) and discharge energy density (W rec = 8.9Jcm -1 ).

[0052] (2) The chemical composition of the high-entropy perovskite relaxor ferroelectric ceramic provided by the application is (Ba 0.8-x Na x Bi 0.2 )(Ti 0.8- x Ta x Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3, 0≤x≤0.05, the ten cations contained have synergistic effect, thereby improving the comprehensive energy storage performance of the ferroelectric ceramic.

[0053] (3) The high-entropy perovskite relaxor ferroelectric ceramic provided by the application has a widened dielectric temperature Curie peak, and the dielectric temperature stability (TCC < 15%, -66℃-222℃) is improved.

[0054] (4) The high-entropy perovskite relaxor ferroelectric ceramic provided by the application has a smaller grain size, improved resistivity, and greatly improved breakdown strength compared with a dielectric material that is not high-entropy.

[0055] (5) The high-entropy perovskite relaxor ferroelectric ceramic provided by the application exhibits a cocktail effect of high-entropy materials in the field of dielectric energy storage, proving that it is a feasible method to design a dielectric material with excellent comprehensive energy storage performance through entropy engineering. BRIEF DESCRIPTION OF DRAWINGS

[0056] Figure 1 The high-entropy perovskite relaxor ferroelectric ceramic prepared for Example 1 has a discharge energy density, energy storage density, and energy storage efficiency statistical diagram from -85℃ to 240℃ under an electric field of 500kV cm -1

[0057] Figure 2 The high-entropy perovskite relaxor ferroelectric ceramic prepared for Example 1 has a hysteresis loop diagram from -85℃ to 240℃ under an electric field of 500kV cm -1

[0058] Figure 3 The high-entropy perovskite relaxor ferroelectric ceramic prepared for Example 1 has an SEM picture.

[0059] Figure 4 The high-entropy perovskite relaxor ferroelectric ceramic prepared for Example 1 has a complex impedance imaginary part Z" and modulus M" change with frequency diagram and fitted conductivity activation energy diagram.

[0060] Figure 5 The high-entropy perovskite relaxor ferroelectric ceramic prepared for Example 1 has a hysteresis loop diagram under a maximum applicable electric field.

[0061] Figure 6 The high-entropy perovskite relaxor ferroelectric ceramic prepared for Example 1 has a comparison diagram of energy storage temperature stability.

[0062] Figure 7 The dielectric constant temperature stability (TCC) comparison diagram of Example 1 and Example 3.

[0063] Figure 8 The high-entropy perovskite relaxor ferroelectric ceramic prepared for Example 1 has a hysteresis loop diagram under a maximum applicable electric field. DETAILED DESCRIPTION

[0064] ​​The present embodiment is implemented on the basis of the technical scheme of the present application, and gives detailed implementation modes and specific operation processes, but the protection scope of the present application is not limited to the following examples.

[0065] Unless otherwise specified, the reagents, methods, instruments and equipment used in the present application are conventional reagents, methods, instruments and equipment in the art. Unless otherwise specified, the reagents and materials used in the following examples are commercially available.

[0066] A high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature energy storage temperature stability and near-zero hysteresis, the chemical composition of the high-entropy perovskite relaxor ferroelectric ceramic is (Ba 0.8-x Na x Bi 0.2 )(Ti 0.8-x Ta x Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3, wherein 0≤x≤0.05. The high-entropy perovskite relaxor ferroelectric ceramic has a change in discharge energy density of ±(3-8)% and a change in energy storage efficiency of ±(8-15)% in the temperature range of-85℃ to 220℃ under an electric field of 500kV cm -1 .

[0067] The high-entropy perovskite relaxor ferroelectric ceramic is prepared by the following method:

[0068] S1, the raw material powder is weighed according to the stoichiometric ratio of each element in (Ba 0.8-x Na x Bi 0.2 )(Ti 0.8-x Ta x Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3;

[0069] S2, the raw material powder is subjected to primary ball milling, mixing, drying and pre-sintering to obtain a primary mixed powder;

[0070] S3, the primary mixed powder obtained in step S2 is ground and then subjected to secondary ball milling and drying to obtain a secondary mixed powder;

[0071] S4, the secondary mixed powder prepared in step S3 is mixed with a solvent, a binder, a dispersant and a plasticizer respectively to obtain a casting slurry;

[0072] S5, the casting slurry prepared in step S4 is subjected to bubble removal and casting to obtain a single-layer ceramic thick film;

[0073] S6, the single-layer ceramic thick film prepared in step S5 is subjected to shearing, lamination and hot-pressing treatment to obtain a ceramic green body;

[0074] S7, the ceramic green body prepared in step S6 is subjected to degreasing and sintering treatment to obtain a high-entropy perovskite relaxor ferroelectric ceramic.

[0075] The application will be described in detail below with reference to the accompanying drawings and specific examples.

[0076] Example 1 x = 0.04

[0077] (1) According to the stoichiometric ratio of (Ba 0.76 Na 0.04 Bi 0.2 )(Ti 0.76 Ta 0.04 Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3, the raw material powders are weighed and mixed, and the mixed powders are subjected to primary ball milling for 24 h, the mass ratio of the ball stones is 6 mm:3 mm:1 mm = 3:2:1, anhydrous ethanol is used as the solvent, and the mass ratio of the raw material powders: anhydrous ethanol: ball stones is 1:3:1, the rotation speed is 350 rpm, and then the powders are dried at 80℃ for 24 h and pre-sintered at 950℃ for 4 h to obtain the synthesis main crystal phase powders (primary ball milling powders);

[0078] (2) The main crystal phase powders are ground and crushed, and subjected to secondary ball milling (the ball milling parameters are the same as in step 1), and then dried at 80℃ for 24 h to obtain the secondary ball milling powders;

[0079] (3) The secondary ball milling powders obtained in step 2 are put into a ball milling tank, a solvent (butanone and ethanol) and a dispersant (tributyl phosphate) are added, and ball milling is carried out at a rotation speed of 280 rpm for 12 h to make them uniformly mixed; then a binder (polyvinyl butyral) and a plasticizer (polyethylene glycol 400, butyl phthalate) are added to the slurry, and ball milling is carried out at a rotation speed of 280 rpm for 6 h to obtain a casting slurry, wherein the mass percentages of the secondary ball milling powders, butanone, ethanol, tributyl phosphate, polyvinyl butyral, polyethylene glycol and butyl phthalate are 50%, 20%, 20%, 5%, 1%, 2% and 2% respectively. The casting slurry is subjected to vacuum debubbling to remove air bubbles, and the debubbling time is 20 min; then the casting slurry is subjected to casting through a casting machine, the doctor blade height is 200 μm, and the casting rate is 30 cm / min, and a single-layer ceramic thick film is obtained after drying.

[0080] (4) The monolayer ceramic thick film obtained in step (3) is cut into a square with a side length of 12 mm by a slicer; then the four cut square thick films are stacked and subjected to hot-pressing treatment to form a ceramic green body; wherein the hot-pressing temperature is 45℃, the pressure is 30 MPa, and the pressure maintaining time is 20 min.

[0081] (5) The ceramic green body obtained in step (4) is placed in a box furnace for degassing, and heated to 600℃ at a heating rate of 0.5℃ / min and kept for 6h, and then cooled with the furnace. Then the degassed sample is placed in an alumina crucible, and the crucible is placed in a box furnace and heated to 1180℃ at a heating rate of 2℃ / min and kept for 3h for sintering treatment, to obtain a high-entropy perovskite relaxor ferroelectric ceramic.

[0082] Example 2 x = 0.02

[0083] The experimental steps are carried out according to the method of Example 1, except that the various raw material powders of (Ba 0.78 Na 0.02 Bi 0.2 )(Ti 0.78 Ta 0.02 Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3 are weighed according to the stoichiometric ratio and mixed.

[0084] Example 3 x = 0

[0085] The experimental steps are carried out according to the method of Example 1, except that the various raw material powders of (Ba 0.8 Bi 0.2 )(Ti 0.8 Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3 are weighed according to the stoichiometric ratio and mixed.

[0086] The high-entropy perovskite relaxor ferroelectric ceramic in Example 1 has a discharge energy density (W -1 ), energy storage density (W rec ) and energy storage efficiency (η) from -85℃ to 240℃ under an electric field of 500kV cm st ), as shown in the statistical chart of Figure 1 From the chart, it can be seen that the discharge energy density of the high-entropy perovskite relaxor ferroelectric ceramic changes by less than 5% and the energy storage efficiency changes by less than 10% within the range from -85℃ to 220℃;

[0087] The high-entropy perovskite relaxor ferroelectric ceramic in Example 1 has a maximum electric field of 833 kV cm -1 The electric hysteresis loop graph of the high-entropy perovskite relaxor ferroelectric ceramic in Example 1 under electric field from -85℃ to 240℃ is shown in Figure 2 From the graph, it can be seen that the shape of the electric hysteresis loop remains basically unchanged and the saturation polarization intensity is almost unchanged within the range of -85℃ to 220℃, and the excellent energy storage temperature stability of the ceramic is visually observed;

[0088] The SEM picture of the high-entropy perovskite relaxor ferroelectric ceramic in Example 1 is shown in Figure 3 It can be seen that the grain size of the ceramic is basically less than 1 micron, which is conducive to the improvement of the breakdown strength;

[0089] The complex impedance imaginary part Z" and modulus M" change graph and the fitted conductivity activation energy graph of the high-entropy perovskite relaxor ferroelectric ceramic in Example 1 with frequency are shown in Figure 4 It can be seen that the conductivity activation energy of the grain and the grain boundary of the ceramic is large and close, which is conducive to the improvement of the electrical uniformity and the improvement of the breakdown strength;

[0090] The electric hysteresis loop graph of the high-entropy perovskite relaxor ferroelectric ceramic in Example 1 under the maximum electric field is shown in Figure 5 From the graph, it can be seen that the electric hysteresis loop of the ceramic is slender, the maximum polarization intensity is large, and the residual polarization intensity is almost zero, so that it has a high energy storage efficiency, and the maximum electric field strength can reach 833 kV cm -1 ;

[0091] The energy storage temperature stability comparison graph of the high-entropy perovskite relaxor ferroelectric ceramic in Example 1 is shown in Figure 6 From the graph, it can be seen that compared with the reported NaNbO3-based, BiFeO3-based, AgNbO3-based, BaTiO3-based, Na 0.5 Bi 0.5 TiO3-based, K 0.5 Bi 0.5 TiO3-based, SrTiO3-based, and HEC system, the prepared ceramic has a very small change in energy storage performance within a wide temperature range, and the temperature stability is very excellent.

[0092] Figure 7 The dielectric constant temperature stability (TCC) graph of Example 1 and Example 3, wherein Example 1, i.e. x = 0.04, has a wide dielectric temperature stability (TCC < 15%, -66℃-222℃).

[0093] Comparative Example 1:

[0094] The experimental steps refer to the method of Example 1, except that (Ba 0.8 Bi0.2 )(Ti 0.8 Mg 0.1 Zr 0.1 )O3 and mixed. Figure 8 The electric hysteresis loop diagram of the non-high-entropy perovskite relaxor ferroelectric ceramic prepared for Comparative Example 1 under the maximum applicable electric field. It is tested that the breakdown electric field (480 kV / cm 3 ) of the prepared non-high-entropy perovskite relaxor ferroelectric ceramic at room temperature is much smaller than that (830 kV / cm 3 ) of the ceramic prepared in Example 1, and the energy storage performance is not excellent enough.

[0095] In summary, the high-entropy perovskite relaxor ferroelectric ceramic prepared by the present application has excellent comprehensive energy storage performance, has high energy storage density, at the same time has nearly 100% energy storage efficiency and excellent energy storage temperature stability across low and high temperature regions, and is helpful to improve the application in the field of high-power energy storage components.

[0096] The above description of the embodiments is for facilitating the ordinary skilled person in the art to understand and use the present application. The person skilled in the art can obviously easily make various modifications to the embodiments, and apply the general principles described herein to other embodiments without creative labor. Therefore, the present application is not limited to the above embodiments, and the improvements and modifications made by the person skilled in the art according to the disclosure of the present application without departing from the scope of the present application should be within the protection scope of the present application.

Claims

1. A high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis, characterized in that: The chemical composition of the high entropy perovskite relaxor ferroelectric ceramic is (Ba 0.8-x Na x Bi 0.2 )(Ti 0.8-x Ta x Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3, where 0 <x≤0.05。 2. The high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis according to claim 1, characterized in that: The chemical composition of the high entropy perovskite relaxor ferroelectric ceramic is (Ba 0.76 Na 0.04 Bi 0.2 )(Ti 0.76 Ta 0.04 Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 )O3, x=0.

04.

3. A method for preparing a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis according to any one of claims 1 to 2, characterized in that: The following steps are involved: S1, according to (Ba 0.8-x Na x Bi 0.2 )(Ti 0.8-x Ta x Mg 0.04 Zn 0.04 Al 0.04 Sn 0.04 Zr 0.04 ) Weigh the raw material powder according to the stoichiometric ratio of each element in O3; S2, ball milling, mixing, drying, and pre-calcining the raw material powder to obtain a primary mixed powder; S3, grinding the primary mixed powder obtained in step S2, performing secondary ball milling, and drying to obtain a secondary mixed powder; S4, mixing the secondary mixed powder prepared in step S3 with a solvent, a binder, a dispersant, and a plasticizer respectively to obtain a casting slurry; S5, degassing and casting the casting slurry prepared in step S4 to obtain a single-layer ceramic thick film; S6, shearing, laminating and hot pressing the single-layer ceramic thick film prepared in step S5 to obtain a ceramic green body; S7, performing debinding and sintering treatment on the ceramic green body prepared in step S6 to obtain a high entropy perovskite relaxor ferroelectric ceramic.

4. The method for preparing a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis according to claim 3, characterized in that: In step S1 , the raw material powders containing the elements Ba and Na are their corresponding carbonates, and the raw material powders containing the elements Zn, Mg, Al, Sn, Zr, Ti, Ta, and Bi are their corresponding oxides.

5. The method for preparing a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis according to claim 3, characterized in that: In step S2, the primary ball milling is performed at a rotation speed of 200-600 rpm for a time of 4-48 hours; the primary ball milling medium includes balls, and the solvent includes anhydrous ethanol; the mass of the balls is in a ratio of 6 mm diameter: 3 mm: 1 mm = 3-5: 1.5-3: 1; the mass of the raw material powder for the primary ball milling: the mass of anhydrous ethanol: the mass of the balls = 1: 1.5-6: 1-2; the drying is performed at 60° C. to 150° C. for 12-48 hours; and the pre-calcination is performed at a temperature of 800° C. to 1100° C. for 1-10 hours. The particle size of the powder mixed once is 1 μm to 1.6 μm.

6. The method for preparing a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis according to claim 3, characterized in that: In step S3, the secondary ball milling is performed at a rotation speed of 200-600 rpm for a time of 4-48 hours. The medium for the secondary ball milling includes balls, and the solvent includes anhydrous ethanol. The mass of the balls is in a ratio of 6 mm diameter: 3 mm: 1 mm = 3-5: 1.5-3:

1. The mass of the primary mixed powder in the secondary ball milling: the mass of anhydrous ethanol: the mass of the balls = 1: 1.5-6: 1-2. The particle size of the secondary mixed powder is 0.3 μm to 0.8 μm.

7. The method for preparing a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis according to claim 3, characterized in that: In step S4, the solvent is selected from one or more of butanone, ethanol or toluene; the adhesive includes polyvinyl butyral; the dispersant is selected from one or two of tributyl phosphate and triolein; the plasticizer is selected from one or more of polyethylene glycol 400, butyl phthalate or benzyl-n-butyl-phthalate; and the mass ratio of the secondary mixed powder to the solvent, adhesive, dispersant and plasticizer is 30-60%: 30-50%: 2-6%: 0.8-1.2%: 2-5%.

8. The method for preparing a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis according to claim 3, characterized in that: In step S5, during the casting process, the casting rate is 20-40 cm / min, the scraper height is 10-40 μm, and the thickness of the obtained single-layer ceramic thick film is 10-30 μm; In step S6, during the hot pressing process, the hot pressing temperature is 30-80°C, the pressure is 10-50 MPa, and the holding time is 10-30 minutes; In step S7, the debinding process is specifically to heat the temperature to 400-600°C at a heating rate of 0.1-0.5°C / min and keep it at that temperature for 4-8 hours, and then cool it with the furnace; the sintering process is specifically to heat the temperature to 1000-1250°C at a heating rate of 1-3°C / min and keep it at that temperature for 2-4 hours, and then cool it with the furnace.

9. Application of the high-entropy perovskite relaxor ferroelectric ceramic according to any one of claims 1 to 2 with ultra-wide temperature stability and near-zero hysteresis in the field of high-power energy storage components.

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