High-entropy ceramic capacitor, ceramic dielectric material for high-entropy ceramic capacitor and preparation method of high-entropy ceramic capacitor

Abstract

The invention relates to a high-entropy ceramic capacitor, a ceramic dielectric material for the high-entropy ceramic capacitor and a preparation method, the raw material composition of the ceramic dielectric material comprises NaNbO3, (Na0. 2Bi0. 2Ba0. 2Mg0. 2Zn0. 2) TiO3, H3BO3, CaZrO3 and the like, by controlling the raw material ratio and preparation process parameters of sodium niobate and adopting a multi-step grinding synthesis method, NaNbO3-based high-entropy ceramic is designed, so that the insulation resistance of the high-entropy ceramic capacitor is effectively improved; on the other hand, chemical modification treatment is carried out by introducing (Na0. 2Bi0. 2Ba0. 2Mg0. 2Zn0. 2) TiO3, H3BO3, CaZrO3 and the like, so that the structural stability of an antiferroelectric phase is enhanced, the compactness of the material is improved, and finally, the energy storage performance of the material is optimized and improved.

Description

Technical Field

[0001] This invention belongs to the field of ceramic capacitor preparation, specifically relating to a high-entropy ceramic capacitor and its ceramic dielectric material and preparation method. Background Technology

[0002] Traditional lead-based antiferroelectric ceramics (such as PbZrO3 and PLZST) face strict environmental restrictions due to their lead content. Among lead-free materials, sodium niobate (NaNbO3) has become the preferred alternative to lead-based materials due to its wide antiferroelectric phase range (-100℃ to +360℃), high polarization intensity, and excellent temperature stability. High-entropy ceramics, by introducing multiple principal elements, can optimize crystal structure, electronic structure, and phase transition behavior through multi-component synergistic effects. For example, doping NaNbO3 with elements such as Ca, Bi, and Ni forms a solid solution, stabilizing the antiferroelectric phase and achieving double hysteresis loop characteristics, significantly improving energy storage performance. The rapid phase transition response (nanosecond level) and low remanent polarization (Pr) of NaNbO3-based high-entropy ceramics make them suitable for high-power pulse systems such as laser weapons and electromagnetic guns. High-entropy design can also suppress grain coarsening, improve material uniformity, and achieve miniaturization and high reliability of ceramic capacitors. NaNbO3-based high-entropy ceramics have broken through the performance bottlenecks of traditional materials, demonstrating great potential in fields such as capacitors, pulse power, and transducers. With increasingly stringent environmental regulations and higher requirements for material performance in high-end manufacturing, this material is expected to become a core medium for next-generation electronic components, driving the green upgrading of industries such as new energy vehicles, 5G communications, and aerospace.

[0003] Sodium niobate (NaNbO3) belongs to a class of antiferroelectric lead-free energy storage ceramic dielectric materials with a perovskite crystal structure, possessing fundamental application value in the field of lead-free energy storage. However, it is important to note that pure-phase NaNbO3 ceramics have significant limitations: when exposed to an external electric field or high-temperature environment, its crystal structure is prone to an irreversible transition from an antiferroelectric phase to a ferroelectric phase. This transition directly leads to significant instability in the overall performance of the material. Furthermore, the poor density of pure-phase NaNbO3 ceramics results in inferior electrical performance, and low insulation resistance leads to increased leakage current, reduced energy storage efficiency, and decreased capacitor reliability. Therefore, effectively stabilizing the intrinsic antiferroelectric phase of high-entropy NaNbO3 ceramics and improving density and insulation resistance have become key issues that need to be addressed in the subsequent research and application of this material. Summary of the Invention

[0004] The purpose of this invention is to overcome the shortcomings of the prior art and provide a high-entropy ceramic capacitor, the ceramic dielectric material used therein, and a preparation method thereof.

[0005] The present invention adopts the following technical solution: A ceramic dielectric material for a high-entropy ceramic capacitor has the following raw material composition percentage: (1-x)wt%NaNbO3+xwt%(Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + a wt% H3BO3 + b wt% CaZrO3, wherein NaNbO3 is the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are modifying additives, H3BO3 is a sintering aid, and 0≤x≤20, 1≤a≤5, 1≤b≤7, where x, a, and b are the mass percentages of each precursor compound.

[0006] Furthermore, the (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 The preparation methods of TiO3 and are as follows; Step 1: Place Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 powders into a ball mill jar in proportion, use deionized water as solvent, and ball mill for 4-6 hours. Step 2: The wet slurry obtained after ball milling is dried in an oven at 100℃~150℃ for 4h~6h. The dried powder is then sieved through a 40~80 mesh sieve to obtain a mixed powder of Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 raw materials. The sieved mixed powder is then placed in a muffle furnace and calcined at 800-950℃ for 2h~6h to obtain (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 precursor powder.

[0007] Furthermore, in step 1, the weight ratio of deionized water to powder is 2:1, the grinding media is zirconia balls, and the weight ratio of zirconia balls to powder is 6:1. The rotation speed of the ball mill is (400-600) rpm / min.

[0008] A method for preparing a ceramic dielectric material for a high-entropy ceramic capacitor includes the following steps: Step 1: Prepare NaNbO3 main matrix material; Step 2, prepare (Na) 0.2 Bi0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 modified additive; Step 3, using NaNbO3 as the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3, H3BO3, and CaZrO3 modified additives are added to a ball mill jar according to the raw material ratio requirements. Anhydrous ethanol is used as the solvent and agate balls are used as the grinding media. The mixture is ball-milled for 9-12 hours. The particle size and dispersibility are controlled by controlling the particle size. Step four: The wet slurry obtained after ball milling in step three is dried in an oven at 50℃~80℃ for 4h~6h. The dried powder is then sieved through a 40~80 mesh sieve to obtain (1-x)wt% NaNbO3+x wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3+a wt% H3BO3+b wt% CaZrO3 ceramic dielectric material.

[0009] Furthermore, in step one, the preparation method of the NaNbO3 main matrix material is as follows: A. Place NaCO3 in an oven at 120℃~150℃ and pre-dry for 2h~5h to dry the adsorbed water in the Na2CO3 raw material; put the dried Na2CO3 powder and Nb2O5 powder into a ball mill jar, use anhydrous ethanol as solvent and zirconium oxide beads as grinding media, and ball mill for 8h-12h. B. The wet slurry obtained after ball milling is dried in an oven at 50℃~80℃ for 4h~6h. The dried powder is then sieved through a 40~80 mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 700℃~900℃ for 2h~6h to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material back into a ball mill jar, use anhydrous ethanol as solvent and zirconia beads as grinding media, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material.

[0010] Furthermore, in step A, the zirconia beads are arranged in a ratio of 2.0mm:1.0mm=5:1; in step C, the zirconia beads are arranged in a ratio of 2.0mm:1.0mm=5:1.

[0011] Furthermore, in steps A and C, the weight ratio of anhydrous ethanol to powder is 2:1, and the weight ratio of zirconia balls to powder is 6:1.

[0012] Furthermore, in steps A and C, the rotational speed of the ball mill is (400-600) rpm / min.

[0013] A high-entropy ceramic capacitor is prepared using the ceramic dielectric material described above.

[0014] A method for preparing a high-entropy ceramic capacitor includes the following steps: (1) The ceramic media material is sieved, and granulated with 10-12 wt% paraffin wax, and pressed into a green body under 6-8 MPa; (2) The green blank is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1110-1130°C at a rate of 2.58°C / min, held for 3 hours, and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes to form a disc-type high-entropy ceramic capacitor.

[0015] As can be seen from the above description of the present invention, compared with the prior art, the beneficial effects of the present invention are: This application, by clearly defining the raw material ratio and preparation process parameters of the ceramic dielectric material, adopts a multi-step grinding synthesis method, and introduces (Na+) into the sodium niobate main matrix material... 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 High-entropy relaxable sodium niobate ceramic dielectric materials obtained by chemically modifying TiO3, H3BO3, and CaZrO3 not only enhance the structural stability of the antiferroelectric phase and improve the material's density, but also effectively improve the insulation resistance, thus optimizing the material's energy storage performance. Furthermore, the synergistic effect of the multi-component elements can optimize the electric field distribution, reduce local electric field concentration, thereby reducing the risk of dielectric breakdown and improving electrical performance and reliability. Specifically, the doped Zr element optimizes the grain boundary structure, reducing the probability of crack formation, and since microcracks are one of the main channels for leakage current, this improves the insulation resistance. In addition, the segregation of the multi-component elements at the grain boundaries can further optimize the grain boundary structure, reduce grain boundary defects, thereby reducing leakage current and improving insulation resistance. Moreover, the doped Ca element can modify the surface to form a denser insulating layer, enhancing the resistance to leakage current. The ceramic capacitor prepared based on the sodium niobate ceramic matrix material of this application has a dielectric constant of approximately 570 and a dielectric loss of approximately 15 × 10⁻⁶. -4 The insulation resistance at room temperature is approximately 3.91 × 10⁻⁶. 6MΩ, and improved sintering density with reduced porosity; Furthermore, the preparation process used in this invention has significant advantages: on the one hand, the process is simple and efficient, and has excellent stability and reproducibility, which can ensure performance consistency in large-scale production; on the other hand, the raw materials used are inexpensive, and the entire process is environmentally friendly. Attached Figure Description

[0016] Figure 1 The microstructure of the ceramic capacitor prepared in Example 1 of this application is shown. Figure 2 The microstructure of the ceramic capacitor prepared in Comparative Example 1 of this application is shown. Figure 3 The microstructure of the ceramic capacitor prepared in Comparative Example 2 of this application is shown. Figure 4 The image shows the microstructure of the ceramic capacitor prepared in Comparative Example 3 of this application. Detailed Implementation

[0017] The present invention will be further described below through specific embodiments.

[0018] A high-entropy ceramic capacitor, made of ceramic dielectric material, is prepared by means of the following steps: (1) The ceramic media material is sieved, and granulated with 10-12 wt% paraffin wax, and pressed into a green body under 6-8 MPa; (2) The round green body is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1110-1130°C at a rate of 2.58°C / min, held for 3 hours, and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes at 720°C to form a disc ceramic capacitor.

[0019] The percentage composition of the raw materials for the ceramic dielectric material is as follows: (1-x)wt% NaNbO3+x wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + a wt% H3BO3 + b wt% CaZrO3, wherein NaNbO3 is the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2TiO3 and CaZrO3 are used as modifying additives, and H3BO3 is used as a sintering aid, where 0≤x≤20, 1≤a≤5, 1≤b≤7, and x, a, and b are the mass percentages of each precursor compound. Specifically, the preparation method includes the following steps: Step 1: Preparation of NaNbO3 main matrix material: A. Place NaCO3 in an oven at 120℃~150℃ and pre-dry for 2h~5h to dry the adsorbed water in the Na2CO3 raw material; put the dried Na2CO3 powder and Nb2O5 powder into a ball mill jar, use anhydrous ethanol as solvent and zirconium oxide beads as grinding media, and ball mill for 8h-12h. B. The wet slurry obtained after ball milling is dried in an oven at 50℃~80℃ for 4h~6h. The dried powder is then sieved through a 40~80 mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 700℃~900℃ for 2h~6h to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material in a ball mill jar again, use anhydrous ethanol as solvent and zirconium oxide beads as grinding medium, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material. Step 2, prepare (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 modified additives: Step 1: Place Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 powders into a ball mill jar in proportion, use deionized water as solvent, and ball mill for 4-6 hours. Step 2: The wet slurry obtained after ball milling is dried in an oven at 100℃~150℃ for 4h~6h. The dried powder is then sieved through a 40~80 mesh sieve to obtain a mixed powder of Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 raw materials. The sieved mixed powder is then placed in a muffle furnace and calcined at 800-950℃ for 2h~6h to obtain (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 precursor powder; Step 3, using NaNbO3 as the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2TiO3, H3BO3, and CaZrO3 modified additives are added to a ball mill jar according to the raw material ratio requirements. Anhydrous ethanol is used as the solvent and agate balls are used as the grinding media. The mixture is ball-milled for 9-12 hours. The particle size and dispersibility are controlled by controlling the particle size. Step four: The wet slurry obtained after ball milling in step three is dried in an oven at 50℃~80℃ for 4h~6h. The dried powder is then sieved through a 40~80 mesh sieve to obtain (1-x)wt% NaNbO3+x wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3+a wt% H3BO3+b wt% CaZrO3 ceramic dielectric material.

[0020] Furthermore, in step 1, the weight ratio of deionized water to powder is 2:1, the grinding media is zirconia balls, and the weight ratio of zirconia balls to powder is 6:1. The rotation speed of the ball mill is (400-600) rpm / min.

[0021] In steps A and C, the zirconia beads are composed of 2.0 mm: 1.0 mm = 5:1; the weight ratio of anhydrous ethanol to powder is 2:1, and the weight ratio of zirconia balls to powder is 6:1; and the rotation speed of the ball mill is (400-600) rpm / min. Example

[0022] A high-entropy ceramic capacitor, made of ceramic dielectric material, is prepared by means of the following steps: (1) The ceramic media material is sieved, granulated with 12 wt% paraffin, and pressed into a round green body with a diameter of 15 mm and a thickness of 1.5 mm under 6 MPa; (2) The round green body is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1120°C at a rate of 2.58°C / min. It is held for 3 hours and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes at 720°C to form a high-entropy ceramic capacitor.

[0023] The percentage composition of the raw materials for the ceramic dielectric material is as follows: 80 wt% NaNbO3 + 13 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2TiO3 + 6 wt% CaZrO3 + 1 wt% H3BO3, wherein NaNbO3 is the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are used as modifying additives, and H3BO3 is used as a sintering aid. Specifically, the preparation method includes the following steps: Step 1: Preparation of NaNbO3 main matrix material: A. Place NaCO3 in a 135℃ oven and pre-dry for 4 hours to remove adsorbed water from the Na2CO3 raw material; place the dried Na2CO3 powder and Nb2O5 powder in a ball mill jar at a molar ratio of 1:1, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0mm:1.0mm=5:1, and ball mill for 10 hours. B. The wet slurry obtained after ball milling is dried in an oven at 65°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 1100°C for 3 hours to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material in a ball mill jar again, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0 mm: 1.0 mm = 5: 1, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material. Step 2, prepare (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 modified additives: Step 1: Place Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 powders into a ball mill jar in proportion, use deionized water as solvent, and ball mill for 5 hours. Step 2: The wet slurry obtained after ball milling is dried in an oven at 120℃ for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2. The sieved mixed powder is then placed in a muffle furnace and calcined at 800℃ for 3 hours to obtain (Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2). 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 precursor powder; Step 3, using NaNbO3 as the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are modified additives, and H3BO3 is a sintering aid. According to the raw material ratio requirements, they are added to the ball mill jar, anhydrous ethanol is used as solvent, and agate balls are used as grinding media. The mixture is ball-milled for 9 hours. Step four: The wet slurry obtained after ball milling in step three is dried in an oven at 75°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain 80 wt% NaNbO3 + 13 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3+6 wt% CaZrO3+1 wt% H3BO3 ceramic dielectric material.

[0024] Comparative Example 1 A high-entropy ceramic capacitor, made of ceramic dielectric material, is prepared by means of the following steps: (1) The ceramic media material is sieved, granulated with 12 wt% paraffin, and pressed into a round green body with a diameter of 15 mm and a thickness of 1.5 mm under 6 MPa; (2) The round green body is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1120°C at a rate of 2.58°C / min. It is held for 3 hours and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes at 720°C to form a disc ceramic capacitor.

[0025] The percentage composition of the raw materials for the ceramic dielectric material is as follows: 80 wt% NaNbO3 + 19 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + 1 wt% H3BO3, wherein NaNbO3 is the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 is used as a modified additive, and H3BO3 is used as a sintering aid. Specifically, its preparation method includes the following steps: Step 1: Preparation of NaNbO3 main matrix material: A. Place NaCO3 in a 135℃ oven and pre-dry for 4 hours to remove adsorbed water from the Na2CO3 raw material; place the dried Na2CO3 powder and Nb2O5 powder in a ball mill jar at a molar ratio of 1:1, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0mm:1.0mm=5:1, and ball mill for 10 hours. B. The wet slurry obtained after ball milling is dried in an oven at 65°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 1100°C for 3 hours to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material in a ball mill jar again, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0 mm: 1.0 mm = 5: 1, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material. Step 2, prepare (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 modified additives: Step 1: Place Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 powders into a ball mill jar in proportion, use deionized water as solvent, and ball mill for 5 hours. Step 2: The wet slurry obtained after ball milling is dried in an oven at 120℃ for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2. The sieved mixed powder is then placed in a muffle furnace and calcined at 800℃ for 3 hours to obtain (Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2). 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 precursor powder; Step 3, using NaNbO3 as the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are modified additives, and H3BO3 is a sintering aid. According to the raw material ratio requirements, they are added to the ball mill jar, anhydrous ethanol is used as solvent, and agate balls are used as grinding media. The mixture is ball-milled for 9 hours. Step four: The wet slurry obtained after ball milling in step three is dried in an oven at 75°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain 80 wt% NaNbO3 + 19 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + 1 wt% H3BO3 ceramic dielectric material.

[0026] Comparative Example 2 A high-entropy ceramic capacitor, made of ceramic dielectric material, is prepared by means of the following steps: (1) The ceramic media material is sieved, granulated with 12 wt% paraffin, and pressed into a round green body with a diameter of 15 mm and a thickness of 1.5 mm under 6 MPa; (2) The round green body is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1120°C at a rate of 2.58°C / min. It is held for 3 hours and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes at 720°C to form a disc ceramic capacitor.

[0027] The percentage composition of the raw materials for the ceramic dielectric material is as follows: 80 wt% NaNbO3 + 14 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + 6 wt% CaZrO3, wherein NaNbO3 is the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are used as modifying additives. Specifically, their preparation method includes the following steps: Step 1: Preparation of NaNbO3 main matrix material: A. Place NaCO3 in a 135℃ oven and pre-dry for 4 hours to remove adsorbed water from the Na2CO3 raw material; place the dried Na2CO3 powder and Nb2O5 powder in a ball mill jar at a molar ratio of 1:1, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0mm:1.0mm=5:1, and ball mill for 10 hours. B. The wet slurry obtained after ball milling is dried in an oven at 65°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 1100°C for 3 hours to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material in a ball mill jar again, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0 mm: 1.0 mm = 5: 1, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material. Step 2, prepare (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 modified additives: Step 1: Place Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 powders into a ball mill jar in proportion, use deionized water as solvent, and ball mill for 5 hours. Step 2: The wet slurry obtained after ball milling is dried in an oven at 120℃ for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2. The sieved mixed powder is then placed in a muffle furnace and calcined at 800℃ for 3 hours to obtain (Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2). 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 precursor powder; Step 3, using NaNbO3 as the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 modified additives were added to a ball mill jar, anhydrous ethanol was used as solvent, and agate balls were used as grinding media. The mixture was ball-milled for 9 hours. Step four: The wet slurry obtained after ball milling in step three is dried in an oven at 75°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain 80 wt% NaNbO3 + 14 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + 6 wt% CaZrO3 ceramic dielectric material.

[0028] Comparative Example 3 A high-entropy ceramic capacitor, made of ceramic dielectric material, is prepared by means of the following steps: (1) The ceramic media material is sieved, granulated with 12 wt% paraffin, and pressed into a round green body with a diameter of 15 mm and a thickness of 1.5 mm under 6 MPa; (2) The round green body is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1120°C at a rate of 2.58°C / min. It is held for 3 hours and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes at 720°C to form a disc ceramic capacitor.

[0029] The percentage composition of the raw materials for the ceramic dielectric material is as follows: 80 wt% NaNbO3 + 12 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + 6 wt% CaZrO3 + 2 wt% H3BO3, wherein NaNbO3 is the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are used as modifying additives, and H3BO3 is used as a sintering aid. Specifically, the preparation method includes the following steps: Step 1: Preparation of NaNbO3 main matrix material: A. Place NaCO3 in a 135℃ oven and pre-dry for 4 hours to remove adsorbed water from the Na2CO3 raw material; place the dried Na2CO3 powder and Nb2O5 powder in a ball mill jar at a molar ratio of 1:1, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0mm:1.0mm=5:1, and ball mill for 10 hours. B. The wet slurry obtained after ball milling is dried in an oven at 65°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 1100°C for 3 hours to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material in a ball mill jar again, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0 mm: 1.0 mm = 5: 1, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material. Step 2, prepare (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 modified additives: Step 1: Place Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 powders into a ball mill jar in proportion, use deionized water as solvent, and ball mill for 5 hours. Step 2: The wet slurry obtained after ball milling is dried in an oven at 120℃ for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2. The sieved mixed powder is then placed in a muffle furnace and calcined at 800℃ for 3 hours to obtain (Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2). 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 precursor powder; Step 3, using NaNbO3 as the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are modified additives, and H3BO3 is a sintering aid. According to the raw material ratio requirements, they are added to the ball mill jar, anhydrous ethanol is used as solvent, and agate balls are used as grinding media. The mixture is ball-milled for 9 hours. Step four: The wet slurry obtained after ball milling in step three is dried in an oven at 75°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain 80 wt% NaNbO3 + 12 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3+6 wt% CaZrO3+2 wt% H3BO3 ceramic dielectric material.

[0030] Comparative Example 4 A high-entropy ceramic capacitor, made of ceramic dielectric material, is prepared by means of the following steps: (1) The ceramic media material is sieved, granulated with 12 wt% paraffin, and pressed into a round green body with a diameter of 15 mm and a thickness of 1.5 mm under 6 MPa; (2) The round green body is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1120°C at a rate of 2.58°C / min. It is held for 3 hours and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes at 720°C to form a disc ceramic capacitor.

[0031] The raw material composition of the ceramic dielectric material is as follows: 93 wt% NaNbO3 + 6 wt% CaZrO3 + 1 wt% H3BO3, wherein NaNbO3 is the main matrix material, CaZrO3 is a modifying additive, and H3BO3 is a sintering aid. Specifically, its preparation method includes the following steps: Step 1: Preparation of NaNbO3 main matrix material: A. Place NaCO3 in a 135℃ oven and pre-dry for 4 hours to remove adsorbed water from the Na2CO3 raw material; place the dried Na2CO3 powder and Nb2O5 powder in a ball mill jar at a molar ratio of 1:1, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0mm:1.0mm=5:1, and ball mill for 10 hours. B. The wet slurry obtained after ball milling is dried in an oven at 65°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 1100°C for 3 hours to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material in a ball mill jar again, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0 mm: 1.0 mm = 5: 1, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material. Step 2: Add NaNbO3 main matrix material and H3BO3 to the ball mill jar according to the raw material ratio requirements, use anhydrous ethanol as solvent and agate balls as grinding media, and ball mill for 9 hours. Step 3: The wet slurry obtained after ball milling in step 2 is dried in an oven at 75°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a ceramic dielectric material of 93 wt% NaNbO3 + 6 wt% CaZrO3 + 1 wt% H3BO3.

[0032] Comparative Example 5 A high-entropy ceramic capacitor, made of ceramic dielectric material, is prepared by means of the following steps: (1) The ceramic media material is sieved, granulated with 12 wt% paraffin, and pressed into a round green body with a diameter of 15 mm and a thickness of 1.5 mm under 6 MPa; (2) The round green body is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1120°C at a rate of 2.58°C / min. It is held for 3 hours and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes at 720°C to form a disc ceramic capacitor.

[0033] The percentage composition of the raw materials for the ceramic dielectric material is as follows: 72 wt% NaNbO3 + 21 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + 6 wt% CaZrO3 + 1 wt% H3BO3, wherein NaNbO3 is the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are used as modifying additives, and H3BO3 is used as a sintering aid. Specifically, the preparation method includes the following steps: Step 1: Preparation of NaNbO3 main matrix material: A. Place NaCO3 in a 135℃ oven and pre-dry for 4 hours to remove adsorbed water from the Na2CO3 raw material; place the dried Na2CO3 powder and Nb2O5 powder in a ball mill jar at a molar ratio of 1:1, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0mm:1.0mm=5:1, and ball mill for 10 hours. B. The wet slurry obtained after ball milling is dried in an oven at 65°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 1100°C for 3 hours to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material in a ball mill jar again, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0 mm: 1.0 mm = 5: 1, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material. Step 2, prepare (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2Zn 0.2 TiO3 modified additives: Step 1: Place Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 powders into a ball mill jar in proportion, use deionized water as solvent, and ball mill for 5 hours. Step 2: The wet slurry obtained after ball milling is dried in an oven at 120℃ for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2. The sieved mixed powder is then placed in a muffle furnace and calcined at 800℃ for 3 hours to obtain (Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2). 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 precursor powder; Step 3, using NaNbO3 as the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are modified additives, and H3BO3 is a sintering aid. According to the raw material ratio requirements, they are added to the ball mill jar, anhydrous ethanol is used as solvent, and agate balls are used as grinding media. The mixture is ball-milled for 9 hours. Step four: The wet slurry obtained after ball milling in step three is dried in an oven at 75°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain 77 wt% NaNbO3 + 16 wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + 6 wt% CaZrO3 + 1 wt% H3BO3 ceramic media powder.

[0034] Comparative Example 6 A high-entropy ceramic capacitor, made of ceramic dielectric material, is prepared by means of the following steps: (1) The ceramic media material is sieved, granulated with 12 wt% paraffin, and pressed into a round green body with a diameter of 15 mm and a thickness of 1.5 mm under 6 MPa; (2) The round green body is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1120°C at a rate of 2.58°C / min. It is held for 3 hours and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes at 720°C to form a disc ceramic capacitor.

[0035] The percentage composition of the raw materials for the ceramic dielectric material is as follows: 80 wt% NaNbO3 + 13 wt% Bi(Zn) 0.5 Ti 0.5 The mixture consists of 6 wt% NaNbO3 + 1 wt% CaZrO3 + 1 wt% H3BO3, where NaNbO3 is the main matrix material and Bi(ZnO3) is the main component. 0.5 Ti 0.5 O3 and CaZrO3 are used as modifying additives, and H3BO3 is used as a sintering aid. Specifically, the preparation method includes the following steps: Step 1: Preparation of NaNbO3 main matrix material: A. Place NaCO3 in a 135℃ oven and pre-dry for 4 hours to remove adsorbed water from the Na2CO3 raw material; place the dried Na2CO3 powder and Nb2O5 powder in a ball mill jar at a molar ratio of 1:1, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0mm:1.0mm=5:1, and ball mill for 10 hours. B. The wet slurry obtained after ball milling is dried in an oven at 65°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 1100°C for 3 hours to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material in a ball mill jar again, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0 mm: 1.0 mm = 5: 1, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material. Step 2, prepare (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 modified additives: Step 1: Place Bi2O3, ZnO and TiO2 powders into a ball mill jar in proportion, use deionized water as solvent, and ball mill for 5 hours. Step 2: The wet slurry obtained after ball milling is dried in an oven at 120℃ for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Bi₂O₃, ZnO, and TiO₂ raw materials. The sieved mixed powder is then placed in a muffle furnace and calcined at 800℃ for 3 hours to obtain Bi(ZnO)₂. 0.5 Ti 0.5 O3 precursor powder.

[0036] Step 3: Add NaNbO3 as the main matrix material and Bi(Zn)0.5 Ti 0.5 O3 and CaZrO3 are modified additives, and H3BO3 is a sintering aid. According to the raw material ratio requirements, they are added to the ball mill jar, anhydrous ethanol is used as solvent, and agate balls are used as grinding media. The mixture is ball-milled for 9 hours. Step four: The wet slurry obtained after ball milling in step three is dried in an oven at 75°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain 80 wt% NaNbO3 + 13 wt% Bi(Zn) 0.5 Ti 0.5 O3+6 wt% CaZrO3+1 wt% H3BO3 ceramic dielectric material.

[0037] Comparative Example 7 A high-entropy ceramic capacitor, made of ceramic dielectric material, is prepared by means of the following steps: (1) The ceramic media material is sieved, granulated with 12 wt% paraffin, and pressed into a round green body with a diameter of 15 mm and a thickness of 1.5 mm under 6 MPa; (2) The round green body is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1120°C at a rate of 2.58°C / min. It is held for 3 hours and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes at 720°C to form a high-entropy ceramic capacitor.

[0038] The raw material composition of the ceramic dielectric material is as follows: 80 wt% NaNbO3 + 13 wt% (0.1 Na2CO3 + 0.1 Bi2O3 + 0.2 BaCO3 + 0.2 MgO + 0.2 ZnO + 0.2 TiO2) + 6 wt% CaZrO3 + 1 wt% H3BO3, wherein NaNbO3 is the main matrix material, Na2CO3, Bi2O3, BaCO3, MgO, ZnO, TiO2 and CaZrO3 are modifying additives, and H3BO3 is a sintering aid. Specifically, its preparation method includes the following steps: Step 1: Preparation of NaNbO3 main matrix material: A. Place NaCO3 in a 135℃ oven and pre-dry for 4 hours to remove adsorbed water from the Na2CO3 raw material; place the dried Na2CO3 powder and Nb2O5 powder in a ball mill jar at a molar ratio of 1:1, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0mm:1.0mm=5:1, and ball mill for 10 hours. B. The wet slurry obtained after ball milling is dried in an oven at 65°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 1100°C for 3 hours to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material in a ball mill jar again, use anhydrous ethanol as solvent and zirconia beads as grinding media, with a zirconia bead ratio of 2.0 mm: 1.0 mm = 5: 1, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material. Step 2: Add the main matrix material NaNbO3, the modifying additives Na2CO3, Bi2O3, BaCO3, MgO, ZnO, TiO2, CaZrO3, and the sintering aid H3BO3 into a ball mill jar according to the raw material ratio requirements. Use anhydrous ethanol as solvent and agate balls as grinding media, and ball mill for 9 hours. Step 3: The wet slurry obtained after ball milling in Step 2 is dried in an oven at 75°C for 5 hours. The dried powder is then sieved through an 80-mesh sieve to obtain a ceramic dielectric material of 80wt% NaNbO3+13wt%(0.1Na2CO3+0.1Bi2O3+0.2BaCO3+0.2MgO+0.2ZnO+0.2TiO2)+6wt% CaZrO3+1wt% H3BO3.

[0039] The dimensions and dielectric properties of the ceramic capacitors prepared in Example 1, Comparative Example 1, Comparative Example 2, Comparative Example 3, Comparative Example 4, Comparative Example 5, Comparative Example 6, and Comparative Example 7 were tested, and the results are shown in the table below: Table 1 Detection data for each embodiment

[0040] In summary, the ceramic capacitor prepared based on the sodium niobate ceramic matrix material of this application has a dielectric constant of approximately 570 and a dielectric loss of approximately 15 × 10⁻⁶. -4 The insulation resistance at room temperature is approximately 3.91 × 10⁻⁶. 6 MΩ.

[0041] Comparing Example 1 with Comparative Examples 2 and 3, it is evident that the addition of 1 wt% H3BO3 in Example 1, compared to Comparative Example 1 without H3BO3, significantly increases the sintering shrinkage rate, improves density, and reduces the sample diameter of the formulation system. Figure 1 and Figure 3 This phenomenon can be observed through comparison. However, in Comparative Example 2, the addition of 2 wt% H3BO3 did not significantly reduce the diameter. Figure 1 and Figure 4This phenomenon can also be seen by comparison, thus proving that the addition of H3BO3 has the effect of improving the sintering density of the system, and the optimal proportion of 1 wt% H3BO3 is the best.

[0042] Comparing Example 1 with Comparative Example 1, it is evident that Zr and Ca can significantly improve insulation resistance. This is because Zr undergoes a martensitic transformation at high temperatures, accompanied by changes in volume and shape, which absorbs energy and reduces stress concentration at crack tips, preventing crack propagation. Microcracks are one of the main channels for leakage current. Furthermore, for high-entropy ceramics, the segregation of multiple elements at grain boundaries can further optimize the grain boundary structure, reduce grain boundary defects, thereby lowering leakage current and improving insulation resistance. Ca can form acceptor impurities (Ca1) on the ceramic surface. 2+ The diffusion layer, after heat treatment, transforms into an insulating dielectric layer, preventing leakage current from passing through and thus improving the overall insulation resistance. It also suppresses voltage effects and optimizes the grain boundary layer, indirectly increasing the insulation resistance. For high-entropy ceramics, the introduction of various metal ions can produce similar surface modification effects, forming a denser insulating layer and enhancing leakage resistance.

[0043] Comparing Example 1 with Comparative Examples 4, 5, and 6, it can be seen that the multiphase high-entropy ceramic material (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 Doping with TiO3 can reduce dielectric loss and increase insulation resistance in products. Because doping reduces grain size and alleviates grain agglomeration, the design of high-entropy systems effectively promotes grain refinement in the ceramic system. Furthermore, the "slow diffusion effect" of high-entropy materials slows grain growth, resulting in a more uniform grain distribution. Therefore, high-entropy ceramic capacitors with smaller grain sizes and a uniform, dense structure can reduce leakage current and exhibit higher insulation resistance. When an excessive amount of multiphase high-entropy ceramic material is introduced, the dielectric constant gradually decreases with increasing multi-element doping concentration, and the dielectric loss increases significantly. This may be because excessive doping leads to the disappearance of the NaNbO3 phase and the easy formation of the Mg2Nb2O7 phase precipitate, which becomes the dominant crystalline phase, thus reducing the dielectric constant. In addition, the increased doping amount forms a multiphase structure in the ceramic matrix, increasing the number of interfaces between crystalline phases. The increased migration speed of charge carriers at these interfaces leads to a gradual increase in loss and a decrease in insulation resistance. Furthermore, the same proportion of high-entropy ceramic material (Na... 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 replaced with Bi(Zn) 0.5 Ti 0.5As clearly seen in Comparative Example 6, O3, a non-high-entropy material, exhibits a significant decrease in dielectric constant and insulation resistance, coupled with an increase in loss. Furthermore, (Na... 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 The raw materials for the high-entropy component of TiO3, Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2, were directly added in proportion and mixed with the main matrix material. As can be seen from Comparative Example 7 in Table 1, its performance deteriorated to some extent compared with Example 1. Therefore, (Na2CO3, Bi2O3, BaCO3, MgO, ZnO, and TiO2) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 The high-entropy design of TiO3 can significantly improve the insulation resistance of the product and reduce dielectric loss.

[0044] This application clarifies the raw material ratio and preparation process parameters of the ceramic dielectric material, adopts a multi-step grinding synthesis method, and introduces (Na) into the sodium niobate matrix material. 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 High-entropy relaxable sodium niobate ceramic dielectric material obtained by chemically modifying TiO3, H3BO3, and CaZrO3 not only enhances the structural stability of the antiferroelectric phase and improves the material's density, but also effectively improves the material's insulation resistance, thus optimizing the material's energy storage performance. Furthermore, the multi-component synergistic effect can optimize the electric field distribution, reduce local electric field concentration, thereby lowering the risk of dielectric breakdown and improving electrical performance and reliability. In the preparation of the NaNbO3 main matrix material, zirconia beads of different sizes are used for synergistic grinding. The process is simple and efficient, while possessing excellent stability and reproducibility, ensuring consistent performance in large-scale production. On the other hand, the selected raw materials are inexpensive, and the entire process is environmentally friendly.

[0045] The above description is merely a preferred embodiment of the present invention and should not be construed as limiting the scope of the present invention. All equivalent changes and modifications made in accordance with the scope of the present invention and the contents of the specification should still fall within the scope of the present invention.

Claims

1. A ceramic dielectric material for high-entropy ceramic capacitors, characterized in that: The percentage composition of its raw materials is as follows: (1-x)wt% NaNbO3 +x wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 + a wt% H3BO3 + b wt% CaZrO3, wherein NaNbO3 is the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 and CaZrO3 are modifying additives, H3BO3 is a sintering aid, and 0≤x≤20, 1≤a≤5, 1≤b≤7, where x, a, and b are the mass percentages of each precursor compound.

2. The ceramic dielectric material for a high-entropy ceramic capacitor according to claim 1, characterized in that: Said (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 The preparation methods of TiO3 and are as follows; Step 1: Place Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 powders into a ball mill jar in proportion, use deionized water as solvent, and ball mill for 4-6 hours. Step 2: The wet slurry obtained after ball milling is dried in an oven at 100℃~150℃ for 4h~6h. The dried powder is then sieved through a 40~80 mesh sieve to obtain a mixed powder of Na2CO3, Bi2O3, BaCO3, MgO, ZnO and TiO2 raw materials. The sieved mixed powder is then placed in a muffle furnace and calcined at 800-950℃ for 2h~6h to obtain (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 precursor powder.

3. The method for preparing a ceramic dielectric material for a high-entropy ceramic capacitor according to claim 2, characterized in that: In step 1, the weight ratio of deionized water to powder is 2:1, the grinding media is zirconia balls, and the weight ratio of zirconia balls to powder is 6:

1. The rotation speed of the ball mill is (400-600) rpm / min.

4. The method for preparing a ceramic dielectric material for a high-entropy ceramic capacitor according to claim 1, characterized in that: Includes the following steps: Step 1: Prepare NaNbO3 main matrix material; Step 2, prepare (Na) 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3 modified additive; Step 3, using NaNbO3 as the main matrix material, (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3, H3BO3, and CaZrO3 modified additives are added to a ball mill jar according to the raw material ratio requirements. Anhydrous ethanol is used as the solvent and agate balls are used as the grinding media. The mixture is ball-milled for 9-12 hours. The particle size and dispersibility are controlled by controlling the particle size. Step four: The wet slurry obtained after ball milling in step three is dried in an oven at 50℃~80℃ for 4h~6h. The dried powder is then sieved through a 40~80 mesh sieve to obtain (1-x)wt% NaNbO3 +x wt% (Na 0.2 Bi 0.2 Ba 0.2 Mg 0.2 Zn 0.2 TiO3+awt% H3BO3+bwt% CaZrO3 ceramic dielectric material.

5. The method for preparing a ceramic dielectric material for a high-entropy ceramic capacitor according to claim 3, characterized in that: In step one, the preparation method of the NaNbO3 main matrix material is as follows: A. Place NaCO3 in an oven at 120℃~150℃ and pre-dry for 2h~5h to dry the adsorbed water in the Na2CO3 raw material; put the dried Na2CO3 powder and Nb2O5 powder into a ball mill jar, use anhydrous ethanol as solvent and zirconium oxide beads as grinding media, and ball mill for 8h-12h. B. The wet slurry obtained after ball milling is dried in an oven at 50℃~80℃ for 4h~6h. The dried powder is then sieved through a 40~80 mesh sieve to obtain a mixed powder of Na2CO3 and Nb2O5 raw materials. The sieved mixed powder is placed in a muffle furnace and calcined at 700℃~900℃ for 2h~6h to obtain sodium niobate powder. C. Place the obtained NaNbO3 matrix material back into a ball mill jar, use anhydrous ethanol as solvent and zirconia beads as grinding media, and perform a second ball milling for 6 hours. After drying, sieve to obtain the NaNbO3 main matrix material.

6. The method for preparing a ceramic dielectric material for a high-entropy ceramic capacitor according to claim 4, characterized in that: In step A, the zirconia beads are arranged in a ratio of 2.0mm:1.0mm=5:1; in step C, the zirconia beads are arranged in a ratio of 2.0mm:1.0mm=5:

1.

7. The method for preparing a ceramic dielectric material for a high-entropy ceramic capacitor according to claim 4, characterized in that: In steps A and C, the weight ratio of anhydrous ethanol to powder is 2:1, and the weight ratio of zirconia balls to powder is 6:

1.

8. The method for preparing a ceramic dielectric material for a high-entropy ceramic capacitor according to claim 4, characterized in that: In steps A and C, the rotational speed of the ball mill is (400-600) rpm / min.

9. A high-entropy ceramic capacitor, characterized in that: It is prepared using the ceramic dielectric material described in claim 1 or 2.

10. A method for preparing a high-entropy ceramic capacitor according to claim 9: characterized in that: Includes the following steps: (1) The ceramic media material is sieved, and granulated with 10-12 wt% paraffin wax, and pressed into a green body under 6-8 MPa; (2) The green blank is heated to 500°C in air at a rate of 2.78°C / min, and then heated to 1110-1130°C at a rate of 2.58°C / min, held for 3 hours, and sintered into ceramic sheets. (3) The ceramic sheet is sintered with silver electrodes to form a disc-type high-entropy ceramic capacitor.

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