Dielectric-fluorescent high-entropy ceramic capable of emitting red light as well as preparation method and application of dielectric-fluorescent high-entropy ceramic

Abstract

The invention discloses a red light emitting dielectric-fluorescent high-entropy ceramic and a preparation method and application thereof, and belongs to the technical field of lead-free dielectric ceramic capacitors. According to the red light emitting dielectric-fluorescent high-entropy ceramic disclosed by the invention, in the aspect of material composition design, the ceramic has the characteristics of low loss, high breakdown electric field, large polarization and the like by adopting a BaTiO3-based high-entropy dielectric system; a high-entropy effect, a cocktail effect and a lattice distortion effect introduced by the high-entropy material system enable the material to present a compact microstructure, stable temperature stability and excellent dielectric properties, so that excellent energy storage and fluorescence characteristics can be obtained; the technical problem that an existing ceramic capacitor is difficult to have low loss, high energy storage density, high energy storage efficiency and excellent red fluorescence emission performance at the same time is solved.

Description

Technical Field

[0001] This invention belongs to the field of lead-free dielectric ceramic capacitor technology, specifically relating to a red light emitting dielectric-fluorescent high-entropy ceramic, its preparation method, and its application. Background Technology

[0002] Dielectric ceramic capacitors play a crucial role in pulse power systems such as new energy vehicles, electromagnetic pulse weapons, and passive power electronic devices due to their ultra-high power density and nanosecond-level charge and discharge speeds. Currently, the mainstream material for commercially available dielectric ceramic capacitors is BaTiO3-based ceramic, but two major technical bottlenecks still need to be overcome: firstly, high losses make it difficult to increase the breakdown electric field (<200kV / cm), resulting in low energy storage density and efficiency (energy storage density <5J / cm). 3 Furthermore, the efficiency is less than 80%, which is not conducive to the miniaturization of devices; secondly, the current dielectric ceramic capacitors have relatively simple functions, only able to utilize their dielectric and ferroelectric properties, and cannot realize real-time optical display of the device's service status. This makes it difficult to meet the technical requirements of non-contact non-destructive testing or remote sensing, thus hindering the multi-functionality and integration of devices.

[0003] Furthermore, in the fields of fluorescent display and lighting technology, red emission is a crucial component of the red, green, and blue (RGB) primary colors. Obtaining excellent red emission is one of the key steps in achieving high-efficiency and energy-saving LED lighting technology. However, currently, achieving high-intensity red emission with dynamically adjustable color temperature and intensity remains challenging, and related industrial technologies urgently need to be tackled and broken through. In summary, developing a multifunctional dielectric capacitor that combines high energy density and red emission has significant commercial application value.

[0004] Chinese patent application CN 119639455 A discloses a fluorescence-converting red phosphor for displays and its preparation method. This method uses alloying and nitriding methods to prepare phosphors containing Sr, Al, Eu, and Li. The disclosed red phosphor exhibits high purity, high luminous efficiency, and good thermal stability, making it suitable for fluorescence-converting laser display devices. Professor Wang Huanping of China Jiliang University investigated the effects of La... 3+ / Eu 3+ The effect of doping on the luminescence properties of KAlSi2O6-based red phosphor was investigated. By adjusting the doping concentration, the changes in luminescence intensity, fluorescence lifetime, and chromaticity of the red phosphor were studied (Wang Zhiyang, et al. La). 3+ / Eu 3+Influence of Doping on the Luminescence Performance of KAlSi2O6-based Red Phosphor [J], Mechanical Engineering Materials, 2025, 49(2), 69-73. However, current energy storage-fluorescence multifunctional dielectric ceramic capacitors still suffer from low energy density, low energy storage efficiency, weak fluorescence intensity, and difficulty in adjusting color temperature. Furthermore, it is difficult to simultaneously obtain excellent energy storage performance and red fluorescence emission characteristics. Therefore, how to utilize the crystal structure evolution and local symmetry changes of barium titanate matrix materials, as well as current high-entropy control strategies, to obtain energy storage-fluorescence high-entropy ceramic capacitors with low loss, high energy density, high energy storage efficiency, and excellent red fluorescence emission, and their fabrication technology, is a hot research direction for promoting the industrial upgrading of multifunctional dielectric capacitors and fluorescence display technologies. Summary of the Invention

[0005] The purpose of this invention is to provide a red-light-emitting dielectric-fluorescent high-entropy ceramic, its preparation method, and its application, in order to solve the technical problem that existing ceramic capacitors are difficult to simultaneously possess low loss, high energy density, high energy storage efficiency, and excellent red fluorescence emission performance.

[0006] To achieve the above objectives, the present invention employs the following technical solution:

[0007] This invention discloses a red-light-emitting dielectric-fluorescent high-entropy ceramic, the chemical formula of which is (Ba 0.7 Bi 0.3-x La x (Ti) 0.6-y Hf 0.11+y Eu 0.1 M′ 0.13 Nb 0.03 Ta 0.03 O3;

[0008] Where: 0≤x≤0.3; 0≤y≤0.1; M′ is a divalent element.

[0009] Furthermore, the divalent element is Zn. 2+ Mg 2+ and Ca 2+ One of them;

[0010] The red-light-emitting dielectric-fluorescent high-entropy ceramic has a configurational entropy value exceeding 1.86R and a photoluminescence color of red.

[0011] This invention also discloses a method for preparing the above-mentioned red-light-emitting dielectric-fluorescent high-entropy ceramic, comprising the following steps:

[0012] BaCO3, Bi2O3, La2O3, TiO2, HfO2, Eu2O3, ZnO, MgO, CaCO3, Nb2O5 and Ta2O5 are weighed according to the stoichiometric ratio of the chemical formula as described in claim 1 or 2 as raw materials;

[0013] The weighed raw materials are ball-milled once to obtain a slurry; the obtained slurry is then dried and pre-fired to obtain a ceramic powder precursor.

[0014] The ceramic powder precursor was subjected to secondary ball milling, sieving, pressing, cold isostatic pressing and sintering to obtain a red light emitting dielectric-fluorescent high-entropy ceramic.

[0015] Furthermore, the purity of BaCO3, Bi2O3, La2O3, TiO2, HfO2, Eu2O3, ZnO, MgO, CaCO3, Nb2O5, and Ta2O5 is not less than 99%.

[0016] Furthermore, the rotation speed of the first and second ball milling is 300-700 r / min, the ball milling time is 15-36 h, and the ball milling medium used is either anhydrous ethanol or distilled water.

[0017] The volume ratio of the added ball milling media to the raw materials is 4:1.

[0018] Furthermore, the drying time is 12-30 hours; the pre-firing treatment temperature is 810-865℃, and the time is 3-6 hours.

[0019] Furthermore, the pressure for tableting is 1.5-4 MPa, and the holding time is 1-5 min.

[0020] Furthermore, the pressure during the cold isostatic pressing process is 200-300 MPa, and the holding time is 5-10 min.

[0021] Furthermore, the sintering treatment is performed at a temperature of 1100-1500℃ for 1-3 hours.

[0022] This invention also discloses the application of the aforementioned red-light-emitting dielectric-fluorescent high-entropy ceramic in dielectric ceramic capacitors, wherein the breakdown electric field of the dielectric ceramic capacitor exceeds 500 kV / cm and the energy storage density exceeds 6 J / cm². 3 .

[0023] Compared with the prior art, the present invention has the following beneficial effects:

[0024] This invention discloses a red-light-emitting dielectric-fluorescent high-entropy ceramic. In terms of material composition design, by employing a BaTiO3-based high-entropy dielectric system, the ceramic exhibits characteristics such as low loss, high breakdown electric field, and large polarization. The high-entropy effect, cocktail effect, and lattice distortion effect introduced by the high-entropy material system result in a dense microstructure, stable temperature stability, and excellent dielectric properties, thus contributing to superior energy storage and fluorescence characteristics. Specifically, the introduction of Bi and Ti, combined with the synergistic effect of other components, provides a high polarization source, while the introduction of La, Hf, Nb, and Ta, combined with the synergistic effect of other components, contributes to high breakdown and low loss. Therefore, the ceramic can achieve a synergistic improvement in both large polarization and high breakdown, resulting in excellent energy storage performance. Furthermore, Eu... 3+ Doping not only introduces lattice distortion but also red luminescent centers. This allows for the dynamic adjustment of the luminescence intensity and color temperature of phosphors by utilizing the crystal structure evolution and local symmetry changes of barium titanate-based high-entropy dielectric materials. Consequently, these phosphors can serve as high-quality red luminescent sources, leading to high-performance fluorescent display materials. Furthermore, La... 3+ Ion pair Bi 3+ The alternative, and Nb with a higher bandgap. 5+ Ta 5+ The introduction of [a substance] can effectively suppress Bi [acidity] during the sintering process. 3+ The volatilization and oxygen vacancy defect formation address the high loss problem of ferroelectric ceramics. The high entropy effect also hinders grain boundary migration, and the resulting fine-grained structure effectively suppresses leakage current. Lower loss ceramics are beneficial for obtaining a high breakdown electric field, thereby achieving high energy storage density and high luminous intensity.

[0025] This invention also discloses a method for preparing the aforementioned red-emitting dielectric-fluorescent high-entropy ceramic. The raw materials used in this method are all lead-free and environmentally friendly. Through ball milling, cold isostatic pressing, and high-temperature sintering, the resulting dielectric ceramic has a dense structure, small grain size, and uniform element distribution. As a result, it exhibits excellent characteristics such as a large dielectric constant, good energy storage performance, high fluorescence intensity, and emission light located in the red light region. This method is environmentally friendly, simple to operate, and has broad application prospects.

[0026] This invention also discloses the application of the above-mentioned red light emitting dielectric-fluorescent high-entropy ceramic in the preparation of dielectric ceramic capacitors. Due to the use of a two-stage ball milling process, the powder raw materials are mixed more uniformly and the particles are milled finer. Furthermore, the powder sieving, cold isostatic pressing, and two sintering processes (pre-sintering and sintering) ensure a more complete ceramic reaction, guaranteeing uniform diffusion during the phase formation, ceramicization, and high-temperature reaction of the dielectric ceramic. This results in a dense, flat ceramic with few pores. The dielectric capacitor prepared using this dielectric ceramic has advantages such as uniform and small ceramic grain size distribution, fewer defects such as pores and cracks, and less incident light scattering. It is suitable for applications such as high energy density pulse power devices in power electronics technology and phosphors and light-emitting diodes in the display field. It has broad application prospects in the tuning and energy storage of dielectric capacitors, and light-emitting devices for displays and lighting. Attached Figure Description

[0027] Figure 1 The X-ray diffraction pattern of the red-emitting dielectric-fluorescent high-entropy ceramic prepared in Example 4 of this invention is shown.

[0028] Figure 2 The excitation spectrum of the red-emitting dielectric-fluorescent high-entropy ceramic prepared in Example 4 of this invention is shown.

[0029] Figure 3 The emission spectrum of the red-emitting dielectric-fluorescent high-entropy ceramic prepared in Example 4 of this invention is shown.

[0030] Figure 4 The hysteresis loop diagram and corresponding energy storage performance calculation results of the dielectric ceramic capacitor prepared by the red light emitting dielectric-fluorescent high-entropy ceramic in Example 4 of this invention are shown.

[0031] Wherein: the solid line is the hysteresis loop of BTH-1La; the dashed line is the hysteresis loop of BTH-0La. Detailed Implementation

[0032] To enable those skilled in the art to understand the features and effects of the present invention, the terms and expressions used in the specification and claims are explained and defined in general below. Unless otherwise specified, all technical and scientific terms used herein have the ordinary meaning understood by those skilled in the art regarding the present invention, and in case of conflict, the definitions in this specification shall prevail.

[0033] The theories or mechanisms described and disclosed herein, whether right or wrong, should not in any way limit the scope of the invention, that is, the contents of the invention can be implemented without being limited by any particular theory or mechanism.

[0034] In this document, all features defined by numerical ranges or percentage ranges, such as numerical values, quantities, contents, and concentrations, are for the sake of brevity and convenience only. Accordingly, descriptions of numerical ranges or percentage ranges should be considered as covering and specifically disclosing all possible sub-ranges and individual numerical values ​​(including integers and fractions) within those ranges.

[0035] In this article, unless otherwise specified, “contains,” “includes,” “containing,” “has,” or similar terms cover the meanings of “composed of” and “mainly composed of,” for example, “A contains a” covers the meanings of “A contains a and others” and “A contains only a.”

[0036] For the sake of brevity, not all possible combinations of the technical features in each implementation scheme or embodiment are described herein. Therefore, as long as there is no contradiction in the combination of these technical features, the technical features in each implementation scheme or embodiment can be combined arbitrarily, and all possible combinations should be considered within the scope of this specification.

[0037] This invention provides a red-light-emitting dielectric-fluorescent high-entropy ceramic with the chemical composition (Ba). 0.7 Bi 0.3-x La x (Ti) 0.6-y Hf 0.11+y Eu 0.1 M′ 0.13 Nb 0.03 Ta 0.03 O3; where: 0≤x≤0.3; 0≤y≤0.1; M′ is a divalent element, and the divalent element is Zn. 2+ Mg 2+ and Ca 2+ Any one of them.

[0038] This invention also provides a method for preparing the above-mentioned red-light-emitting dielectric-fluorescent high-entropy ceramic, comprising the following steps:

[0039] Step 1: According to chemical composition (Ba 0.7 Bi 0.3-x La x (Ti) 0.6-y Hf 0.11+y Eu 0.1 M′ 0.13 Nb 0.03 Ta 0.03 O3; where: 0≤x≤0.3; 0≤y≤0.1; M′ is a divalent element, and the divalent element is Zn. 2+ Mg 2+ and Ca 2+For any one of the components, weigh out the raw materials BaCO3, Bi2O3, La2O3, TiO2, HfO2, Eu2O3, ZnO, MgO, CaCO3, Nb2O5 and Ta2O5 respectively as raw materials;

[0040] Step 2: Place the raw materials weighed in Step 1 into a planetary ball mill and grind them evenly once. Then, dry and pre-fire the resulting slurry in sequence to obtain ceramic powder precursor.

[0041] Step 3: The ceramic powder precursor obtained in Step 2 is subjected to secondary ball milling, sheet forming and cold isostatic pressing to obtain a cylindrical ceramic green body; the cylindrical ceramic green body is placed in a muffle furnace for sintering to obtain a red light emitting dielectric-fluorescent high-entropy ceramic.

[0042] Preferably, in step 1, the purity of BaCO3, Bi2O3, La2O3, TiO2, HfO2, Eu2O3, ZnO, MgO, CaCO3, Nb2O5 and Ta2O5 is not less than 99%.

[0043] Preferably, the mixture after ball milling is dried in a glass dish for 24 hours, and then pre-fired in a muffle furnace at 845°C for 5 hours.

[0044] Preferably, the primary and secondary ball milling methods are planetary ball milling with a rotation speed of 500 r / min and a milling time of 36 h, using either anhydrous ethanol or distilled water as the medium.

[0045] Preferably, the pressure for tableting is 1.5-4 MPa, and the holding time is 1-5 min.

[0046] More preferably, the pressure for tableting is 2.5 MPa and the holding time is 2 min.

[0047] Preferably, the pressure during cold isostatic pressing is 200-300 MPa, and the holding time is 5-10 min.

[0048] More preferably, the pressure during cold isostatic pressing is 200 MPa, and the holding time is 10 min.

[0049] Preferably, the sintering temperature is 1100-1500℃ and the time is 1-3h.

[0050] More preferably, the sintering process involves placing the sample in a muffle furnace and sintering it at 1200°C for 2.5 hours.

[0051] The present invention will be further illustrated below with reference to specific embodiments. It should be understood that these embodiments are for illustrative purposes only and are not intended to limit the scope of the invention. Furthermore, it should be understood that after reading the teachings of this invention, those skilled in the art can make various alterations or modifications to the invention, and these equivalent forms also fall within the scope defined by the appended claims.

[0052] The following examples use instruments and equipment conventional in the art. Experimental methods in the following examples, unless otherwise specified, are generally performed under conventional conditions or as recommended by the manufacturer. All raw materials used in the following examples are conventional commercially available products with specifications conventional in the art. In this specification and the following examples, unless otherwise specified, "%" refers to weight percentage, "parts" refers to parts by weight, and "ratio" refers to weight proportion.

[0053] Example 1

[0054] A method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic includes the following steps:

[0055] Step 1: According to (Ba 0.7 Bi 0.2 La 0.1 (Ti) 0.5 Hf 0.21 Eu 0.1 Zn 0.13 Nb 0.03 Ta 0.03 The chemical formula of O3 is stoichiometrically calculated using BaCO3, Bi2O3, La2O3, TiO2, HfO2, Eu2O3, ZnO, Nb2O5 and Ta2O5 from Alfa Company with a purity higher than 99% as raw materials;

[0056] Step 2: Place the weighed raw material into a nylon ball mill jar containing zirconia balls, add 100 mL of distilled water as the ball milling medium, and perform one ball milling at a speed of 600 r / min for 36 h to obtain a slurry; place the obtained slurry in a petri dish and dry it at 70 °C for 24 h, then put the dried powder into an alumina crucible and pre-fire it at 860 °C for 5 h to obtain a ceramic powder precursor;

[0057] Step 3: Crush the above ceramic powder precursor and ball mill it a second time using 100mL of distilled water as the medium. The ball milling speed is 600r / min and the ball milling time is 36h. After the ball milling is completed, process the slurry with the same drying process as in Step 2. Then, grind the dried powder thoroughly and pass it through a 200-mesh sieve to obtain uniform and fine powder. Weigh 0.22g of the above powder and put it into a cylindrical mold with a diameter of 10mm. Then, use an electric tablet press to form ceramic discs at 2.5MPa and a holding time of 3min. Then, use a cold isostatic press at 300MPa and a holding time of 10min to obtain dense and crack-free unsintered sheet ceramic.

[0058] Step 4: Place the above ceramic sheet in a muffle furnace for sintering. The process is to hold at 1300℃ for 3 hours in an air atmosphere. The heating rate of the muffle furnace during sintering is 3℃ / min. The cooling method is natural cooling with the furnace. After sintering, the dielectric ceramic sheet is polished with 600-grit and 1500-grit sandpaper until smooth to obtain a red light emitting dielectric-fluorescent high-entropy ceramic.

[0059] Example 2

[0060] A method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic includes the following steps:

[0061] Step 1: According to (Ba 0.7 La 0.3 (Ti) 0.6 Hf 0.11 Eu 0.1 Ca 0.13 Nb 0.03 Ta 0.03 The chemical formula of O3 was determined by weighing out BaCO3, La2O3, TiO2, HfO2, Eu2O3, CaCO3, Nb2O5 and Ta2O5 with a purity of over 99% from Aladdin as raw materials.

[0062] Step 2: Place the weighed raw material into a nylon ball mill jar containing zirconia balls, add 80 mL of anhydrous ethanol as the ball milling medium, and perform one ball milling at a speed of 400 r / min for 20 h to obtain a slurry; place the obtained slurry in a petri dish and dry it at 120 °C for 24 h, then put the dried powder into an alumina crucible and pre-calcine it at 840 °C for 4 h to obtain a ceramic powder precursor;

[0063] Step 3: Crush the above ceramic powder precursor and ball mill it a second time using 80 mL of anhydrous ethanol as the medium. The ball milling speed is 400 r / min and the ball milling time is 20 h. After the ball milling is completed, process the slurry with the same drying process as in Step 2. Then, grind the dried powder thoroughly and pass it through a 100-mesh sieve to obtain uniform and fine powder. Weigh 0.23 g of the above powder and put it into a cylindrical mold with a diameter of 10 mm. Then, use an electric tablet press to form ceramic discs at 5 MPa and a holding time of 1 min. Then, use a cold isostatic press at 200 MPa and a holding time of 7 min to obtain dense and crack-free unsintered sheet ceramics.

[0064] Step 4: Place the above ceramic sheet in a muffle furnace for sintering. The process is to hold at 1400℃ for 3 hours in an air atmosphere. The heating rate of the muffle furnace during sintering is 8℃ / min. The cooling method is natural cooling with the furnace. After sintering, the dielectric ceramic sheet is polished with 400-grit and 1500-grit sandpaper until smooth to obtain a red light emitting dielectric-fluorescent high-entropy ceramic.

[0065] Example 3

[0066] A method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic includes the following steps:

[0067] Step 1: According to (Ba 0.7 Bi 0.1 La 0.2 (Ti) 0.4 Hf 0.31 Eu 0.1 Mg 0.13 Nb 0.03 Ta 0.03 The chemical formula of O3 is stoichiometrically calculated using BaCO3, Bi2O3, La2O3, TiO2, HfO2, Eu2O3, MgO, Nb2O5 and Ta2O5 from Aladdin with a purity higher than 99.5% as raw materials;

[0068] Step 2: Place the weighed raw material into a nylon ball mill jar containing zirconia balls, add 90 mL of anhydrous ethanol as the ball milling medium, and perform one ball milling at a speed of 700 r / min for 12 h to obtain a slurry; place the obtained slurry in a petri dish and dry it at 80 °C for 24 h, then put the dried powder into an alumina crucible and pre-calcine it at 830 °C for 3 h to obtain a ceramic powder precursor;

[0069] Step 3: Crush the above ceramic powder precursor and ball mill it a second time using 90 mL of anhydrous ethanol as the medium. The ball milling speed is 700 r / min and the ball milling time is 12 h. After the ball milling is completed, process the slurry according to the same drying process as in Step 2. Then, grind the dried powder thoroughly and pass it through a 100-mesh sieve to obtain uniform and fine powder. Weigh 0.25 g of the above powder and put it into a cylindrical mold with a diameter of 10 mm. Then, use an electric tablet press to form ceramic discs at 4 MPa and a holding time of 2 min. Then, use a cold isostatic press at 300 MPa and a holding time of 5 min to obtain dense and crack-free unsintered sheet ceramics.

[0070] Step 4: Place the above ceramic sheet in a muffle furnace for sintering. The process is to hold at 1140℃ for 2 hours in an air atmosphere. The heating rate of the muffle furnace during sintering is 4℃ / min. The cooling method is natural cooling with the furnace. After sintering, the dielectric ceramic sheet is polished with 1200-grit and 1500-grit sandpaper until smooth to obtain a red light emitting dielectric-fluorescent high-entropy ceramic.

[0071] Example 4

[0072] A method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic includes the following steps:

[0073] Step 1: According to (Ba 0.7 Bi 0.3 (Ti) 0.55 Hf 0.16 Eu 0.1 Mg 0.13 Nb 0.03 Ta 0.03 O3 (abbreviated as BTH-0La), (Ba 0.7 Bi 0.2 La 0.1 (Ti) 0.55 Hf 0.16 Eu 0.1 Mg 0.13 Nb 0.03 Ta 0.03 The chemical formula of O3 (abbreviated as BTH-1La) is stoichiometrically measured using BaCO3, Bi2O3, La2O3, TiO2, HfO2, Eu2O3, MgO, Nb2O5 and Ta2O5 with a purity higher than 99.5% from Alfa Company as raw materials;

[0074] Step 2: Place the weighed raw material into a nylon ball mill jar containing zirconia balls, add 100 mL of distilled water as the ball milling medium, and perform one ball milling at a speed of 500 r / min for 18 h to obtain a slurry; place the obtained slurry in a petri dish and dry it at 100 °C for 24 h, then put the dried powder into an alumina crucible and pre-fire it at 865 °C for 3 h to obtain a ceramic powder precursor;

[0075] Step 3: Crush the above ceramic powder precursor and ball mill it a second time using 100mL of distilled water as the medium. The ball milling speed is 500r / min and the ball milling time is 18h. After the ball milling is completed, process the slurry according to the same drying process as in Step 2. Then, grind the dried powder thoroughly and pass it through a 200-mesh sieve to obtain uniform and fine powder. Weigh 0.24g of the above powder and put it into a cylindrical mold with a diameter of 10mm. Then, use an electric tablet press to form ceramic discs at 5MPa and a holding time of 1min. Immediately afterwards, use a cold isostatic press at 250MPa and a holding time of 10min to obtain dense and crack-free unsintered sheet ceramics.

[0076] Step 4: Place the above ceramic sheet in a muffle furnace for sintering. The process is to hold at 1350℃ for 3 hours in an air atmosphere. The heating rate of the muffle furnace during sintering is 6℃ / min. The cooling method is natural cooling with the furnace. After sintering, the dielectric ceramic sheet is polished with 600-grit and 1500-grit sandpaper until smooth to obtain a red light emitting dielectric-fluorescent high-entropy ceramic.

[0077] Figure 1 The image shows the X-ray diffraction pattern of the red-emitting dielectric-fluorescent high-entropy ceramic prepared in Example 4. As can be seen from the image, the red-emitting dielectric-fluorescent high-entropy ceramics prepared in this invention all exhibit a standard perovskite structure with good crystallinity and no second phase. They also match well with the standard PDF card (PDF#05-0626) for barium titanate, indicating that the ceramic has a tetragonal phase structure. This result demonstrates that the component design of this invention is correct, the preparation process is reasonable, and the target product was successfully synthesized.

[0078] Figure 2 The image shows the excitation spectrum of the red-emitting dielectric-fluorescent high-entropy ceramic prepared in Example 4, with a monitoring wavelength of 614 nm. As can be seen from the image, the Eu... 3+ The ion excitation spectrum has high intensity and clear peak shape, with two main excitation peaks at 394 nm and 464 nm, proving that the multifunctional energy storage-fluorescent ceramic capacitor has good fluorescence performance.

[0079] Figure 3The image shows the emission spectrum of the red-emitting dielectric-fluorescent high-entropy ceramic prepared in Example 4, with an excitation wavelength of 395 nm. As can be seen from the image, there are two high-intensity emission peaks at 593 nm and 614 nm, corresponding to orange and red light emission, respectively. The emission peaks are sharp, and the peak at 614 nm is stronger than that at 593 nm, indicating that this energy storage-fluorescent ceramic possesses excellent red light characteristics.

[0080] Figure 4 The figure shows the hysteresis loop diagram and corresponding energy storage performance calculation results of the dielectric ceramic capacitor prepared using the red-emitting dielectric-fluorescent high-entropy ceramic in Example 4. As can be seen from the figure, BTH-1La exhibits a higher breakdown electric field, greater polarization characteristics, and lower hysteresis loss than BTH-0La, thus achieving a breakdown field of 550 kV / cm and a hysteresis loss of 6.24 J / J / cm. 3 The energy storage density is high. Furthermore, both exhibit energy storage efficiencies exceeding 93%. The superior breakdown electric field and energy storage performance demonstrate the immense potential of the high-entropy ceramic of this invention for dielectric energy storage.

[0081] The above content is only for illustrating the technical concept of the present invention and should not be construed as limiting the scope of protection of the present invention. Any modifications made to the technical solution based on the technical concept proposed in this invention shall fall within the scope of protection of the claims of this invention.

Claims

1. A red-light-emitting dielectric-fluorescent high-entropy ceramic, characterized in that, The chemical formula of the red-light-emitting dielectric-fluorescent high-entropy ceramic is (Ba 0.7 Bi 0.3-x La x (Ti) 0.6-y Hf 0.11+ y Eu 0.1 M′ 0.13 Nb 0.03 Ta 0.03 O3; Where: 0≤x≤0.3; 0≤y≤0.1; M′ is a divalent element.

2. The red-light-emitting dielectric-fluorescent high-entropy ceramic according to claim 1, characterized in that, The divalent element is Zn. 2+ Mg 2+ and Ca 2+ One of them; The red-light-emitting dielectric-fluorescent high-entropy ceramic has a configurational entropy value exceeding 1.86R and a photoluminescence color of red.

3. The method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic according to claim 1 or 2, characterized in that, Includes the following steps: BaCO3, Bi2O3, La2O3, TiO2, HfO2, Eu2O3, ZnO, MgO, CaCO3, Nb2O5 and Ta2O5 are weighed according to the stoichiometric ratio of the chemical formula as described in claim 1 or 2 as raw materials; The weighed raw materials are ball-milled once to obtain a slurry; the obtained slurry is then dried and pre-fired to obtain a ceramic powder precursor. The ceramic powder precursor was subjected to secondary ball milling, sieving, pressing, cold isostatic pressing and sintering to obtain a red light emitting dielectric-fluorescent high-entropy ceramic.

4. The method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic according to claim 3, characterized in that, The purity of BaCO3, Bi2O3, La2O3, TiO2, HfO2, Eu2O3, ZnO, MgO, CaCO3, Nb2O5 and Ta2O5 shall not be less than 99%.

5. The method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic according to claim 3, characterized in that, The rotation speed of the first and second ball milling is 300-700 r / min, the ball milling time is 15-36 h, and the ball milling medium used is either anhydrous ethanol or distilled water. The volume ratio of the ball milling media to the raw materials is 4:

1.

6. The method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic according to claim 3, characterized in that, The drying time is 12-30 hours; the pre-firing treatment temperature is 810-865℃ and the time is 3-6 hours.

7. The method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic according to claim 3, characterized in that, The pressure for tablet compression is 1.5-4 MPa, and the holding time is 1-5 min.

8. The method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic according to claim 3, characterized in that, The pressure during the cold isostatic pressing process is 200-300 MPa, and the holding time is 5-10 min.

9. The method for preparing a red-light-emitting dielectric-fluorescent high-entropy ceramic according to claim 3, characterized in that, The sintering process is carried out at a temperature of 1100-1500℃ for 1-3 hours.

10. The application of a red-light-emitting dielectric-fluorescent high-entropy ceramic as described in claim 1 or 2 in a dielectric ceramic capacitor, characterized in that, The dielectric ceramic capacitor has a breakdown electric field exceeding 500 kV / cm and an energy storage density exceeding 6 J / cm². 3 .

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