High-entropy perovskite relaxor ferroelectric ceramic with ultra-wide-temperature energy storage temperature stability and near-zero hysteresis as well as preparation method and application of high-entropy perovskite relaxor ferroelectric ceramic

Abstract

The invention relates to high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide-temperature energy storage temperature stability and near-zero hysteresis as well as a preparation method and application of the high-entropy perovskite relaxor ferroelectric ceramic. The chemical composition of the high-entropy perovskite relaxor ferroelectric ceramic is (Ba0.8-xNaxBi0.2) (Ti (0.8-x) TaxMg (0.04) Zn (0.04) Al (0.04) Sn (0.04) Zr (0.04) O3, and x is greater than or equal to 0 and less than or equal to 0.05. According to the high-entropy perovskite relaxor ferroelectric ceramic, in an electric field of 500kV cm <-1 > and in a temperature range of-85 DEG C to 220 DEG C, the change of discharge energy density is + / -(3-8%), and the change of energy storage efficiency is + / -(8-15)%. Compared with the prior art, the high-entropy ceramic disclosed by the invention has the advantages that on the basis of high energy storage density, the energy storage efficiency close to 100% and the excellent energy storage temperature stability across low-temperature and high-temperature regions are realized; therefore, the method has high adaptability and application potential in novel high-tech fields such as electric automobiles, aerospace crafts and space exploration and in extreme environment scenes.

Description

Technical Field

[0001] The present invention relates to the technical field of dielectric energy storage ferroelectric ceramics, and 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 Art

[0002] Dielectric ceramic capacitors are known for their ultra-high power density and fast charge and discharge capabilities, and are regarded as key components in advanced electronic devices and power systems. Low recyclable energy density is the biggest problem facing ceramic capacitors. According to dielectric energy storage theory, large polarization difference and high breakdown strength can achieve improved energy storage performance. Specific implementation methods include grain refinement, control of grain orientation, domain structure regulation, improvement of electrical uniformity, defect engineering, etc. With the help of these methods, the discharge energy density W has been greatly improved in the past decade. rec It has indeed achieved gradual improvement. However, with the vigorous development of emerging high-tech fields (such as electric vehicles, aerospace vehicles and space exploration, etc.), 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 a focus that needs more urgent attention at this stage. Summary of the invention

[0003] The purpose of the present invention is to provide a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature energy storage 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 invention can be achieved by the following technical solutions:

[0005] On the one hand, the present invention provides a high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage temperature stability and near-zero hysteresis, wherein 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, where 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 -1 Under the electric field, within the temperature range of -85°C to 220°C, the discharge energy density varies between ±(3-8%), and the energy storage efficiency varies between ±(8-15%).

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

[0009] 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;

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

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

[0012] 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;

[0013] S5, degassing and casting the tape casting slurry prepared in step S4 to obtain a single-layer ceramic thick film;

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

[0015] S7, debinding and sintering the ceramic green body prepared in step S6 to obtain a high entropy perovskite relaxor ferroelectric ceramic.

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

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

[0018] Preferably, in step S2, the medium for the primary ball milling comprises ball stone.

[0019] Further preferably, in step S2, the mass of the balls is matched according to the ratio of diameter 6mm:3mm:1mm=3-5:1.5-3:1.

[0020] Preferably, in step S2, the solvent for the first ball milling includes anhydrous ethanol.

[0021] Preferably, in step S2, the mass of the raw material powder of the first ball mill: the mass of anhydrous ethanol: the mass of the ball stone = 1:1.5-6:1-2.

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

[0023] Preferably, in step S2, the pre-sintering is carried out at a temperature of 800-1100° C. for 1-10 hours.

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

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

[0026] Preferably, in step S3, the medium for the secondary ball milling comprises ball stone.

[0027] Further preferably, in step S3, the mass of the balls is matched according to the ratio of diameter 6mm:3mm:1mm=3-5:1.5-3:1.

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

[0029] Preferably, in step S3, the mass of the primary mixed powder of the secondary ball milling: the mass of anhydrous ethanol: the mass of the ball stone = 1:1.5-6:1-2.

[0030] Preferably, in step S3, the drying temperature is 60° C. to 150° C., and the drying time is 12 to 48 hours.

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

[0032] Preferably, in steps S2 and S3, the spherulite is zirconium spherulite.

[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 triolein.

[0036] Preferably, in step S4, the plasticizer is selected from one or more of polyethylene glycol 400 (the 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 binder, the dispersant and the plasticizer is 30-60%: 30-50%: 2-6%: 0.8-1.2%: 2-5%.

[0038] Preferably, in step S5, the debubbling refers to removing bubbles by a vacuum debubbling machine, and the debubbling time is 15 to 25 minutes.

[0039] Preferably, 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.

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

[0041] Preferably, in step S6, the lamination refers to laminating four square single-layer ceramic thick films that have been cut.

[0042] Preferably, 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.

[0043] Preferably, 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 the temperature for 4-8h, and then cool with the furnace.

[0044] Preferably, in step S7, the sintering process is specifically to heat the material to 1000-1250°C at a heating rate of 1-3°C / min and keep the temperature for 2-4h, and then cool the material in the furnace.

[0045] In a third aspect, the present invention provides an application of the high-entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature energy storage 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 in 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 ceramics designed by regulating the system's configurational entropy and atomic disorder. Dielectric energy storage materials designed using entropy engineering are usually relaxor ferroelectrics. The increase in atomic-level disorder caused by configurational entropy is often accompanied by an increase in polarization configurational disorder, resulting in 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. Among them, M is composed of less than or equal to 3 elements. M is responsible for providing disorder, breaking the long-range BO bond coupling, and together with Bi that creates new AO bond coupling, it improves the breakdown strength while maintaining the saturation polarization strength. Further improving the disorder of the system to become a high entropy system, whether it is possible to use extremely chaotic polarization configurations to obtain excellent comprehensive energy storage performance is worth further exploration.

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

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

[0051] (1) The high entropy perovskite relaxor ferroelectric ceramic provided by the present invention has ultra-wide temperature 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 present invention 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 a 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 present invention has a broadened dielectric Curie peak and improved dielectric temperature stability (TCC<15%, -66°C-222°C).

[0054] (4) Compared with non-high entropy dielectric materials, the high entropy perovskite relaxor ferroelectric ceramics provided by the present invention have smaller grain size, higher resistivity, and significantly improved breakdown strength of the samples.

[0055] (5) The high-entropy perovskite relaxor ferroelectric ceramics provided by the present invention demonstrate the cocktail effect of high-entropy materials in the field of dielectric energy storage, proving that entropy engineering is a feasible method for designing dielectric materials with excellent comprehensive energy storage performance. BRIEF DESCRIPTION OF THE DRAWINGS

[0056] Figure 1 The high entropy perovskite relaxor ferroelectric ceramic prepared in Example 1 is subjected to 500 kV cm -1 Statistical graphs of discharge energy density, energy storage density and energy storage efficiency from -85℃ to 240℃ under electric field;

[0057] Figure 2 The high entropy perovskite relaxor ferroelectric ceramic prepared in Example 1 is subjected to 500 kV cm -1 Hysteresis loop diagram from -85℃ to 240℃ under electric field;

[0058] Figure 3 This is a SEM image of the high entropy perovskite relaxor ferroelectric ceramic prepared in Example 1;

[0059] Figure 4 The graphs of the imaginary part of complex impedance Z" and modulus M" of the high entropy perovskite relaxor ferroelectric ceramic prepared in Example 1 as a function of frequency and the fitted conductivity activation energy graph;

[0060] Figure 5 The hysteresis loop diagram of the high entropy perovskite relaxor ferroelectric ceramic prepared in Example 1 under the maximum applicable electric field;

[0061] Figure 6 This is a comparison chart of the energy storage temperature stability of the high entropy perovskite relaxor ferroelectric ceramics prepared in Example 1;

[0062] Figure 7 The figure is a comparison diagram of the temperature stability of dielectric constant (TCC) of Example 1 and Example 3;

[0063] Figure 8 This is the hysteresis loop diagram of the relaxor ferroelectric ceramic prepared in Comparative Example 1 under the maximum applicable electric field. DETAILED DESCRIPTION

[0064] This embodiment is implemented based on the technical solution of the present invention, and provides a detailed implementation method and a specific operation process, but the protection scope of the present invention is not limited to the following embodiments.

[0065] Unless otherwise specified, the reagents, methods, instruments and equipment used in the present invention 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 storage stability and near-zero hysteresis, wherein 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 high conductivity at 500 kV cm -1 Under the electric field, within the temperature range of -85°C to 220°C, the discharge energy density varies between ±(3-8%), and the energy storage efficiency varies between ±(8-15%).

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

[0068] 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;

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

[0070] S3, grinding the primary mixed powder obtained in step S2, performing secondary ball milling and drying to obtain secondary mixed powder;

[0071] 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;

[0072] S5, degassing and casting the tape casting slurry prepared in step S4 to obtain a single-layer ceramic thick film;

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

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

[0075] The present invention is described in detail below with reference to the accompanying drawings and specific embodiments.

[0076] Example 1x=0.04

[0077] (1) According to (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 stoichiometric ratio of raw material powders are weighed and mixed, the mixed powders are ball-milled for 24 hours, the mass of the balls is in the ratio of diameter 6mm:3mm:1mm=3:2:1, anhydrous ethanol is used as the solvent, the mass of the raw material powder: the mass of anhydrous ethanol: the mass of the balls=1:3:1, the rotation speed is 350rpm, and then dried at 80°C for 24h, pre-calcined at 950°C for 4h to obtain the powder of the synthetic main crystal phase (one-ball-milled powder);

[0078] (2) grinding the main crystalline phase powder, performing a secondary ball milling (the ball milling parameters are the same as those in step 1), and then drying at 80° C. for 24 h to obtain a secondary ball milled powder;

[0079] (3) The secondary ball-milled powder obtained in step 2 is placed in a ball milling jar, solvent (methyl ethyl ketone and ethanol) and dispersant (tributyl phosphate), and ball milled at a speed of 280 rpm for 12 hours to make it uniformly mixed; then a binder (polyvinyl butyral) and a plasticizer (polyethylene glycol 400, butyl phthalate) are added to the slurry, and ball milled at a speed of 280 rpm for 6 hours to obtain a casting slurry, wherein the mass percentages of the secondary ball-milled powder, 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 debubbled by a vacuum debubbler for 20 minutes; then it is cast by a casting machine, the scraper height is 200 μm, the casting rate is 30 cm / min, and a single-layer ceramic thick film is obtained after drying.

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

[0081] (5) The ceramic green body obtained in step (4) is placed in a box-type furnace for debinding, and the temperature is increased to 600°C at a heating rate of 0.5°C / min and kept at this temperature for 6 hours, and then cooled with the furnace. The debinded sample is then placed in an alumina crucible, and the crucible is placed in a box-type furnace and heated to 1180°C at a heating rate of 2°C / min and kept at this temperature for 3 hours for sintering treatment to obtain a high entropy perovskite relaxor ferroelectric ceramic.

[0082] Example 2x=0.02

[0083] The experimental steps were carried out according to the method of Example 1, except that the stoichiometric ratio (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 ) Various raw material powders of O3 are mixed.

[0084] Example 3 x=0

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

[0086] The high entropy perovskite relaxor ferroelectric ceramic in Example 1 is subjected to a 500 kV cm -1 Discharge energy density (W) from -85℃ to 240℃ under electric field rec ), energy storage density (W st ) and energy storage efficiency (η) statistics are shown in the figure below: Figure 1 As shown in the figure, it can be seen that within the range of -85°C to 220°C, 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%;

[0087] The high entropy perovskite relaxor ferroelectric ceramic in Example 1 is subjected to a 500 kV cm -1 The hysteresis loop from -85℃ to 240℃ under electric field is shown in the figure Figure 2 As shown in the figure, it can be seen that the shape of the hysteresis loop remains basically unchanged within the range of -85℃ to 220℃, and the saturation polarization intensity is almost unchanged, which intuitively shows the excellent energy storage temperature stability of the ceramic;

[0088] The SEM image of the high entropy perovskite relaxor ferroelectric ceramic in Example 1 is as follows: Figure 3 As shown, it can be seen that the grain size of the ceramic is substantially less than 1 micron, which is beneficial to the improvement of the breakdown strength;

[0089] The frequency variation diagram of the complex impedance imaginary part Z" and modulus M" of the high entropy perovskite relaxor ferroelectric ceramic in Example 1 and the fitted conductivity activation energy diagram are shown in FIG. Figure 4 As shown, it can be seen that the conductivity activation energies of the grains and grain boundaries of the ceramic are both large and close, which is beneficial to improving electrical uniformity and thus improving breakdown strength;

[0090] The hysteresis loop of the high entropy perovskite relaxor ferroelectric ceramic in Example 1 under the maximum applicable electric field is shown in FIG. Figure 5 As shown in the figure, it can be seen that the ceramic hysteresis loop is slender, the maximum polarization intensity is large, and the residual polarization intensity is almost zero, which makes it have a high energy storage efficiency and its maximum electric field intensity can reach 833kV cm -1 ;

[0091] The energy storage temperature stability comparison of the high entropy perovskite relaxor ferroelectric ceramics in Example 1 is shown in FIG. Figure 6 As shown in the figure, 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 The ceramics prepared by TiO3-based, SrTiO3-based, and HEC systems have extremely small changes in energy storage performance within a wide temperature range and excellent temperature stability.

[0092] Figure 7 The dielectric constant temperature stability (TCC) diagram of Example 1 and Example 3, wherein Example 1, ie, when x=0.04, has a wider dielectric temperature stability (TCC<15%, -66°C-222°C).

[0093] Comparative Example 1:

[0094] The experimental steps were carried out according to the method of Example 1, except that the stoichiometric ratio (Ba 0.8 Bi0.2 )(Ti 0.8 Mg 0.1 Zr 0.1 ) Various raw material powders of O3 are mixed. Figure 8 The hysteresis loop diagram of the non-high entropy perovskite relaxor ferroelectric ceramic prepared in Comparative Example 1 under the maximum applicable electric field. After testing, the prepared non-high entropy perovskite relaxor ferroelectric ceramic has a breakdown electric field (480 kV / cm 3 ) is much smaller than the ceramic prepared in Example 1 (830 kV / cm 3 ), it no longer has sufficiently excellent energy storage performance.

[0095] In summary, the high-entropy perovskite relaxor ferroelectric ceramics prepared by the present invention have excellent comprehensive energy storage performance. On the basis of high energy storage density, they also have energy storage efficiency close to 100% and excellent energy storage temperature stability across low and high temperature zones, which helps to improve their application in the field of high-power energy storage components.

[0096] The above description of the embodiments is to facilitate the understanding and use of the invention by those skilled in the art. It is obvious that those skilled in the art can easily make various modifications to these embodiments and apply the general principles described herein to other embodiments without creative work. Therefore, the present invention is not limited to the above embodiments, and improvements and modifications made by those skilled in the art based on the disclosure of the present invention without departing from the scope of the present invention should be within the scope of protection of the present invention.

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. 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 high entropy perovskite relaxor ferroelectric ceramics have a high -1 Under the electric field, within the temperature range of -85°C to 220°C, the discharge energy density varies between ±(3-8%), and the energy storage efficiency varies between ±(8-15%).

4. A method for preparing a high entropy perovskite relaxor ferroelectric ceramic having ultra-wide temperature energy storage stability and near-zero hysteresis as claimed in any one of claims 1 to 3, 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 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 tape 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, debinding and sintering the ceramic green body prepared in step S6 to obtain a high entropy perovskite relaxor ferroelectric ceramic.

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 4, 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.

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 4, characterized in that: In step S2, the rotation speed of the first ball milling is 200-600rpm, and the time is 4-48h; the medium of the first ball milling includes ball stones, and the solvent includes anhydrous ethanol; the mass of the ball stones is in the ratio of diameter 6mm:3mm:1mm=3-5:1.5-3:1; the mass of the raw material powder of the first ball milling: the mass of anhydrous ethanol: the mass of the ball stones=1:1.5-6:1-2; the drying is carried out at 60°C-150°C for 12-48h; the pre-calcination is carried out at a temperature of 800-1100°C for 1-10h; The particle size of the powder mixed once is 1 μm to 1.6 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 4, characterized in that: In step S3, the rotation speed of the secondary ball milling is 200-600rpm, and the time is 4-48h; the medium of the secondary ball milling includes ball stones, and the solvent includes anhydrous ethanol. The mass of the ball stones is in the ratio of diameter 6mm:3mm:1mm=3-5:1.5-3:1, and the mass of the primary mixed powder of the secondary ball milling: the mass of anhydrous ethanol: the mass of the ball stones=1:1.5-6:1-2; The particle size of the secondary mixed powder is 0.3 μm to 0.8 μm.

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 4, 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; 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%.

9. The method for preparing a high entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature storage stability and near-zero hysteresis according to claim 4, 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 10-50MPa, 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.

10. Application of the high entropy perovskite relaxor ferroelectric ceramic with ultra-wide temperature stability and near-zero hysteresis as claimed in any one of claims 1 to 3 in the field of high-power energy storage components.

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