Pure lead ytterbium niobate anti-ferroelectric laminated ceramic material and preparation method thereof
The preparation of pure lead niobium ytterbate antiferroelectric ceramic materials through the lamination method solved the problem of insufficient breakdown strength in the traditional solid-phase sintering method, achieved high breakdown strength and excellent energy storage performance, and broke through the limitations of traditional methods.
Patent Information
- Application Number
- CN202510425721.5
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2025-04-07
- Publication Date
- 2025-07-04
AI Technical Summary
Pure lead niobium ytterbate antiferroelectric ceramic materials prepared by traditional solid-phase sintering cannot exhibit antiferroelectric properties at room temperature, and the breakdown strength is insufficient, which limits the improvement of its energy storage performance.
Pure lead niobium ytterbate antiferroelectric ceramic materials are prepared by the lamination method. Through ball milling, drying, calcining, slurry preparation, lamination and sintering, the microstructure is optimized to improve breakdown strength and energy storage performance.
At room temperature, a high breakdown strength of 700kV/cm was achieved, an effective energy storage density of 8.44J/cm3, and an energy storage efficiency of 68.29%, which was significantly better than the traditional solid-phase sintering method.
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Figure CN120247555A_ABST
Abstract
Description
Technical Field
[0001] The present invention belongs to the technical field of functional ceramics, and particularly relates to a pure lead niobium ytterbium antiferroelectric laminated ceramic material and a preparation method thereof. Background Art
[0002] With the progress of technology and the development of the military and civilian fields, people have been constantly pursuing the conversion of natural energy into energy with economic benefits. Especially the advent of heat engines such as steam engines and internal combustion engines has enabled the large-scale and effective conversion of the energy of fossil fuels such as coal and oil. Even now, fossil fuels are still the main part of the energy consumption structure of countries around the world. However, as fossil fuels deposited from ancient biological fossils, their extraction and use inevitably cause resource shortages, environmental pollution, and even problems related to people's health and safety. By converting renewable clean energy in nature such as wind energy, solar energy, and tidal energy into secondary energy such as electricity, these problems can be effectively avoided at the source of energy and the end of use. However, due to the intermittency and uncontrollability of such energy sources, the generated electricity has significant fluctuations in time distribution and output power, which seriously limits their practical applications. Therefore, it is necessary to use electrical energy storage devices that can efficiently store renewable clean energy and stably release electrical energy.
[0003] As one of the energy storage devices, the energy storage performance of dielectric capacitors largely depends on the dielectric materials therein. Among them, due to the antiparallel arrangement of adjacent dipoles in antiferroelectric materials, the electric dipole moments cancel each other out, making the remanent polarization close to zero. Also, due to its unique antiferroelectric-ferroelectric phase transition, it can have a high saturation polarization after the phase transition electric field, which plays an important role in improving the energy storage density.
[0004] As a unique antiferroelectric material, pure lead niobium ytterbium has great advantages and potential in the preparation of ceramic dielectric capacitors with high energy storage performance due to its extremely low sintering temperature (about 1050 °C). However, due to the limitation of the high phase transition electric field (i.e., the phase transition electric field is higher than the breakdown strength), it cannot exhibit antiferroelectric properties at room temperature. Therefore, it is of great research significance and application value to improve the antiferroelectricity through composition regulation or to improve its breakdown strength through process improvement. Summary of the Invention
[0005] The purpose of the present invention is to overcome the above problems existing in the traditional technology, and provide a pure lead niobium ytterbium antiferroelectric laminated ceramic material and a preparation method thereof. By using a lamination method different from the traditional solid-phase sintering method, the breakdown strength of pure lead niobium ytterbium is significantly improved to reach 700 kV / cm. Since it is higher than its phase transition electric field, it exhibits the unique double electric hysteresis loop of antiferroelectric materials at room temperature, and the prepared pure lead niobium ytterbium has relatively excellent energy storage performance at room temperature.
[0006] To achieve the above technical objectives and effects, the present invention is realized through the following technical solutions:
[0007] The present invention provides a pure lead ytterbium niobate antiferroelectric laminated ceramic material, and the chemical formula of the pure lead ytterbium niobate antiferroelectric laminated ceramic material is Pb(Yb 0.5 Nb 0.5 )O3.
[0008] Further, under the test conditions of 20 °C and 10 Hz, the effective energy storage density of the pure lead ytterbium niobate antiferroelectric laminated ceramic material is 8.44 J / cm 3 (which is 10.23 times that of the traditional solid-phase sintering method with an effective energy storage density of 0.825 J / cm 3 ), and the energy storage efficiency is 68.29%.
[0009] The present invention also provides a preparation method of a pure lead ytterbium niobate antiferroelectric laminated ceramic material, including the following steps:
[0010] S1. Mix a lead source, a ytterbium source, and a niobium source to obtain a mixed material;
[0011] S2. After ball milling, discharging, drying, and calcining the obtained mixed material in sequence, obtain a calcined powder;
[0012] S3. Subject the obtained calcined powder to secondary ball milling and drying in sequence to obtain a dried powder, and then mix the dried powder with an organic solvent, a binder, a dispersant, and a homogenizer to obtain a slurry;
[0013] S4. Perform vacuum defoaming on the obtained slurry, flow the defoamed slurry into a film, and obtain a pure lead ytterbium niobate thick film after drying;
[0014] S5. Subject the obtained pure lead ytterbium niobate thick film to processes of slicing, laminating, hot pressing, debinding, and sintering in sequence, and obtain a pure lead ytterbium niobate laminated ceramic material after sintering.
[0015] Further, in step 1, the lead source is Pb3O4, the ytterbium source is Yb2O3, and the niobium source is Nb2O5. Pb3O4, Yb2O3, and Nb2O5 are weighed respectively according to the chemical composition of Pb(Yb 0.5 Nb 0.5 )O3. The purity of Pb3O4 is 98%, and the purities of Yb2O3 and Nb2O5 are both 99.99%.
[0016] Further, the ball milling time in step S2 is 12 - 24 h; the secondary ball milling time in step S3 is 12 - 24 h. The ball milling medium is zirconia balls, and the mass ratio of the mixture, the ball milling medium, and alcohol is 1:1.5:1. For both ball milling and secondary ball milling, the raw materials are placed in a rubber ball milling tank, zirconia ball milling medium and alcohol are added, and then it is put into a planetary ball mill with a rotation speed of 400 r / min.
[0017] Further, in step S2, the temperature of the calcination process is 850 °C, the calcination time is 2 h, and the calcination is carried out in a muffle furnace.
[0018] Further, in step S3, first, the pure lead niobate ytterbium dry powder is mixed with an organic solvent, a dispersant, and zirconia balls, and mixed evenly for 200 - 300 min to obtain a preliminary slurry, and then mixed with a binder and a homogenizer, and mixed evenly for 200 - 300 min to obtain the final slurry; wherein, the organic solvent is toluene - ethanol, the dispersant is tributyl phosphate, the binder is polyethylene glycol, and the homogenizer is butyl phthalate.
[0019] Further, in step S4, defoaming is carried out by a vacuum defoaming machine, the defoaming time is 25 - 60 min, and the drying time is 6 - 12 h.
[0020] Further, in step S5, the pure lead niobate ytterbium thick film is cut into pieces of 1 cm × 1 cm for lamination, and the laminated thick film is compacted by hot pressing, with a pressure of 6 - 12 MPa, a time of 10 - 20 min, and a temperature of 60 - 80 °C; the specific process of debinding is as follows: the hot - pressed pure lead niobate ytterbium laminated sheet is put into a muffle furnace, kept at 500 - 600 °C for 300 - 600 min, with a heating rate of 1 - 5 °C / min and a cooling rate of 5 - 10 °C / min.
[0021] Further, the specific process of sintering in step S5 is as follows: sintering is carried out in a muffle furnace, set to rise from room temperature to 1060 - 1100 °C, with a heating rate of 1 - 5 °C / min, a holding time of 200 - 400 min, and a cooling rate of 5 - 10 °C / min. When it cools down to 200 °C, it is cooled to room temperature with the furnace, and then the pure lead niobate ytterbium antiferroelectric laminated ceramic is obtained.
[0022] Further, the ceramic material obtained in step S5 is polished with sandpapers of different meshes to obtain a smooth and flat - surfaced antiferroelectric laminated ceramic material.
[0023] The beneficial effects of the present invention are: by the lamination method, the microstructure of the pure lead niobate ytterbium antiferroelectric ceramic is improved, its grains are made more uniform, the generation of impurities is reduced, and finally the breakdown strength is increased so that it can induce a phase change from antiferroelectric to ferroelectric before breakdown, obtaining excellent energy storage performance that cannot be obtained by the traditional solid - phase sintering method.
[0024] The laminated structure designed by the present invention is reasonable. All kinds of dispersants, binders, homogenizers, etc. used in the slurry can make the powder distribution more uniform. At the same time, through the method of thick-film rotary lamination layer by layer, the uniformity of substances can be maximally ensured in the three-dimensional x-axis direction, y-axis direction, and z-axis direction. Finally, the sintered antiferroelectric ceramic material has a very good microstructure.
[0025] Of course, it is not necessary for any product implementing the present invention to achieve all of the above advantages simultaneously. BRIEF DESCRIPTION OF THE DRAWINGS
[0026] In order to more clearly illustrate the technical solutions of the comparative examples and embodiments of the present invention, the drawings required for describing the comparative examples and embodiments will be briefly introduced below. Obviously, the drawings in the following description are only some embodiments of the present invention. For those of ordinary skill in the art, other drawings can be obtained based on these drawings without creative efforts.
[0027] Figure 1 XRD diagram of the pure lead niobium ytterbium antiferroelectric laminated ceramic material prepared in the comparative example and Example 1 at room temperature;
[0028] Figure 2 SEM diagram of the pure lead niobium ytterbium antiferroelectric laminated ceramic material prepared in the comparative example and Example 1;
[0029] Among them, ×500 and ×1000 represent 500 times and 1000 times respectively;
[0030] Figure 3 Electric hysteresis loop of the pure lead niobium ytterbium antiferroelectric laminated ceramic material prepared in the comparative example;
[0031] Among them, the abscissa E is the electric field strength, and the ordinate P is the polarization intensity;
[0032] Figure 4 Electric hysteresis loop of the pure lead niobium ytterbium antiferroelectric laminated ceramic material prepared in Example 1;
[0033] Among them, the abscissa E is the electric field strength, and the ordinate P is the polarization intensity;
[0034] Figure 5 Dielectric temperature spectrum diagram of the pure lead niobium ytterbium antiferroelectric laminated ceramic material prepared in the comparative example and Example 1;
[0035] Among them, the abscissa is the temperature, and the ordinates are the dielectric constant and dielectric loss respectively;
[0036] Figure 6 Electric hysteresis loop of the pure lead niobium ytterbium antiferroelectric laminated ceramic material prepared in Example 2;
[0037] Among them, the abscissa E is the electric field strength, and the ordinate P is the polarization intensity;
[0038] Figure 7 is the electric hysteresis loop of the pure lead ytterbium niobate antiferroelectric laminated ceramic material prepared in Example 3;
[0039] Among them, the abscissa E is the electric field strength, and the ordinate P is the polarization intensity;
[0040] Figure 8 is a data schematic diagram of the pure lead ytterbium niobate antiferroelectric laminated ceramic materials prepared in the comparative example and Examples 1-3 in terms of effective energy storage density, energy storage efficiency, and breakdown strength. Specific Embodiments
[0041] Next, the technical solutions in the comparative examples and examples of the present invention will be clearly and completely described in conjunction with the accompanying drawings in the comparative examples and examples of the present invention. Obviously, the described embodiments are only a part of the embodiments of the present invention, rather than all the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those of ordinary skill in the art without creative efforts belong to the scope of protection of the present invention.
[0042] Comparative Example
[0043] This embodiment provides a pure lead ytterbium niobate antiferroelectric ceramic material prepared by a traditional solid-phase sintering method, and its chemical formula is Pb(Yb 0.5 Nb 0.5 )O3.
[0044] The preparation method of the pure lead ytterbium niobate antiferroelectric ceramic material includes the following steps:
[0045] S1. Select Pb3O4 with a purity of 98% and Yb2O3 and Nb2O5 with a purity of 99.99% as raw materials for preparing the antiferroelectric ceramic, weigh them according to the chemical composition and mix them to obtain a mixed material
[0046] S2. The mixed material is ball-milled at a rotation speed of 400 r / min for 18 h, dried, and calcined at 850 °C for 2 h to obtain a calcined powder.
[0047] S3. The calcined powder is subjected to secondary ball-milling and drying processes to obtain a dried powder.
[0048] S4. By granulation, that is, the dried powder is fully mixed with a 9 wt% polyvinyl alcohol solution (the mixing process is 0.2 mL of polyvinyl alcohol solution / g of dried powder), and then pressed into a ceramic green body under a pressure of 6 MPa.
[0049] S5. Place the ceramic green body in a muffle furnace, keep it at 600 °C for 10 h for debinding treatment, and then sinter it. First, raise the temperature to 1080 °C at a heating rate of 2 °C / min and keep it for 3 h, then cool it to 200 °C at a rate of 5 °C / min, and finally cool it to room temperature with the furnace, thus obtaining the antiferroelectric ceramic material.
[0050] In this example, the XRD pattern, SEM photos, ferroelectric hysteresis loop, dielectric temperature spectrum, energy storage density, and energy storage efficiency of the obtained antiferroelectric ceramic samples are respectively shown in Figure 1 、 Figure 2 、 Figure 3 、 Figure 5 and Figure 7 . In terms of structure, Figure 1 The XRD pattern in Figure 2 shows that the prepared sample has a pure perovskite structure and no obvious impurity phases, and the SEM photos in Figure 3 show that the prepared sample has good crystallization performance and a dense structure, but there are a certain amount of impurities. Through the electrical property test, it can be seen from the ferroelectric hysteresis loop in Figure 7 and 3 that the sample in the comparative example has no obvious phase change, the breakdown strength is 500 kV / cm, the energy storage density is 0.82 J / cm 3 , and the energy storage efficiency is 83.34%.
[0051] Example 1
[0052] This example provides a pure lead ytterbium niobate antiferroelectric laminated ceramic material prepared by the lamination method, and its chemical formula is Pb(Yb 0.5 Nb 0.5 )O3.
[0053] The preparation method of the pure lead ytterbium niobate antiferroelectric ceramic material includes the following steps:
[0054] S1. Select Pb3O4 with a purity of 98% and Yb2O3 and Nb2O5 with a purity of 99.99% as the raw materials for preparing the antiferroelectric ceramic, weigh them according to the chemical composition respectively and mix them to obtain a mixed material
[0055] S2. Ball-mill the mixed material at a rotation speed of 400 r / min for 18 h, dry it, and calcine it at 850 °C for 2 h to obtain a calcined powder.
[0056] S3. Subject the calcined powder to secondary ball-milling and drying processes to obtain a dried powder.
[0057] S4. Mix the dried powder with the organic solvents toluene-ethanol and the dispersant tributyl phosphate, add zirconia balls, and put them into a three-dimensional powder mixer for powder mixing. Among them, the powder quality: zirconia ball quality: solvent quality: dispersant quality = 18:27:25:2. The powder mixing time is 360 min to obtain a preliminary slurry.
[0058] Polyethylene glycol and dibutyl phthalate are added to the preliminary slurry, and their mass ratio is: raw powder: polyethylene glycol: dibutyl phthalate = 18:10:3. Then, the powders are mixed for 360 min to obtain the final slurry.
[0059] The slurry is defoamed by a vacuum defoamer for 50 min, and then the defoamed slurry is cast into a film on a tape.
[0060] S5. The prepared pure lead niobium ytterbium acid thick film is cut into 1 cm × 1 cm pieces for lamination, and the laminated thick film is compacted by hot pressing at a pressure of 6 MPa for 20 min at a temperature of 60 °C.
[0061] The hot-pressed pure lead niobium ytterbium acid laminated sheet is put into a muffle furnace for debinding, kept at 600 °C for 360 min, with a heating rate of 3 °C / min and a cooling rate of 5 °C / min.
[0062] The debound laminated sheet is put into a muffle furnace for sintering. It is set to heat from room temperature to 1080 °C at a heating rate of 2 °C / min, keep the temperature for 360 min, and cool at a cooling rate of 5 °C / min. When it cools down to 200 °C, it is cooled to room temperature with the furnace. The obtained ceramic material is polished with sandpapers of different mesh numbers to obtain a smooth and flat antiferroelectric laminated ceramic material.
[0063] The XRD pattern, SEM photograph, ferroelectric hysteresis loop, dielectric temperature spectrum, energy storage density, and energy storage efficiency of the antiferroelectric ceramic sample obtained in this example are respectively shown in Figure 1 、 Figure 2 、 Figure 3 、 Figure 4 and Figure 7 . Figure 1 The XRD pattern in Figure 2 shows that the prepared sample has a pure perovskite structure and no obvious impurity phases. The SEM photograph in Figure 4 shows that the prepared sample has good crystallization performance, a dense structure, and no obvious impurities. Through electrical property tests, it can be seen from the ferroelectric hysteresis loop in Figure 7 and Figure 5 that the sample in Example 1 has obviously undergone a phase transition from antiferroelectric to ferroelectric, with a breakdown strength of 700 kV / cm and an energy storage density of 8.44 J / cm 3 , and an energy storage efficiency of 68.29%. It can be seen from the dielectric temperature spectrum in Figure 5 that the phase transition temperature of the sample in Example 1 is lower than that of the comparative example, that is, the antiferroelectric stability of the sample in Example 1 is stronger, which is also the reason for its ability to exhibit a double ferroelectric hysteresis loop.
[0064] Example 2
[0065] This embodiment provides a pure lead ytterbium niobate antiferroelectric laminated ceramic material prepared by a lamination method, with the chemical formula Pb(Yb 0.5 Nb 0.5 )O3.
[0066] The preparation method of the pure lead ytterbium niobate antiferroelectric ceramic material includes the following steps:
[0067] S1. Select Pb3O4 with a purity of 98% and Yb2O3 and Nb2O5 with a purity of 99.99% as raw materials for preparing the antiferroelectric ceramic. Weigh and mix them according to the chemical composition to obtain a mixed material
[0068] S2. Ball-mill the mixed material at a speed of 400 r / min for 18 h, dry it, and calcine it at 850 °C for 2 h to obtain a calcined powder.
[0069] S3. Subject the calcined powder to secondary ball-milling and drying processes to obtain a dried powder.
[0070] S4. Mix the dried powder with the organic solvents toluene-ethanol and the dispersant tributyl phosphate, add zirconia balls, and place them in a three-dimensional powder mixer for powder mixing. Among them, the powder quality: zirconia ball quality: solvent quality: dispersant quality = 18:27:25:2. The powder mixing time is 360 min to obtain a preliminary slurry.
[0071] Add polyethylene glycol and dibutyl phthalate to the preliminary slurry, and their mass ratio is: original powder: polyethylene glycol: dibutyl phthalate = 18:10:3. Then mix the powder for another 360 min to obtain the final slurry.
[0072] Use a vacuum degassing machine to degas the slurry for 50 min, and then cast the degassed slurry into a film on a tape.
[0073] S5. Cut the pure lead ytterbium niobate thick film prepared above into pieces of 1 cm × 1 cm and stack them. Compact the stacked thick film by hot pressing, with a pressure of 6 MPa, a time of 20 min, and a temperature of 60 °C.
[0074] Put the hot-pressed pure lead ytterbium niobate laminated sheet into a muffle furnace for debinding, keep it at 600 °C for 360 min, with a heating rate of 3 °C / min and a cooling rate of 5 °C / min.
[0075] Put the debound laminated sheet into a muffle furnace for sintering. Set the temperature to rise from room temperature to 1060 °C at a rate of 2 °C / min, keep it for 360 min, and cool it at a rate of 5 °C / min. When it cools down to 200 °C, let it cool down to room temperature with the furnace. Grind the obtained ceramic material with sandpapers of different meshes to obtain a smooth and flat antiferroelectric laminated ceramic material.
[0076] In this embodiment, the polarization-electric field hysteresis loops, energy storage density, and energy storage efficiency of the obtained antiferroelectric ceramic samples are respectively shown in Figure 5 and Figure 7 . It can be seen that a phase transition occurred in the sample of Example 2, but it was not a phase transition from antiferroelectric to ferroelectric, which may be related to a certain intermediate phase. The breakdown strength was 550 kV / cm, the energy storage density was 1.76 J / cm 3 , and the energy storage efficiency was 71%.
[0077] Example 3
[0078] This embodiment provides a pure lead ytterbium niobate antiferroelectric laminated ceramic material prepared by a lamination method, and its chemical formula is Pb(Yb 0.5 Nb 0.5 )O3.
[0079] The preparation method of the pure lead ytterbium niobate antiferroelectric ceramic material includes the following steps:
[0080] S1. Select Pb3O4 with a purity of 98%, Yb2O3 and Nb2O5 with a purity of 99.99% as raw materials for preparing the antiferroelectric ceramic, weigh them according to the chemical composition and mix them to obtain a mixed material
[0081] S2. Ball-mill the mixed material at a rotation speed of 400 r / min for 18 h, dry it, and calcine it at 850 °C for 2 h to obtain a calcined powder.
[0082] S3. Subject the calcined powder to secondary ball-milling and drying processes to obtain a dried powder.
[0083] S4. Mix the dried powder with the organic solvents toluene-ethanol and the dispersant tributyl phosphate, add zirconia balls, and put them into a three-dimensional powder mixer for powder mixing. Among them, the powder mass: zirconia ball mass: solvent mass: dispersant mass = 18:27:25:2. The powder mixing time is 360 min to obtain a preliminary slurry.
[0084] Add polyethylene glycol and dibutyl phthalate to the preliminary slurry, and their mass ratio is raw powder: polyethylene glycol: dibutyl phthalate = 18:10:3. Then mix the powder for another 360 min to obtain the final slurry.
[0085] Use a vacuum defoamer to defoam the slurry for 50 min, and then flow the defoamed slurry onto a tape to form a film.
[0086] S5. Cut the pure lead ytterbium niobate thick film prepared above into 1 cm × 1 cm pieces for lamination, and compact the laminated thick film by hot pressing, with a pressure of 6 MPa, a time of 20 min, and a temperature of 60 °C.
[0087] The hot-pressed pure lead ytterbium niobate laminated sheets are placed in a muffle furnace for debinding, held at 600 °C for 360 min, with a heating rate of 3 °C / min and a cooling rate of 5 °C / min.
[0088] The debound laminated sheets are placed in a muffle furnace for sintering. It is set to heat from room temperature to 1100 °C at a heating rate of 2 °C / min, hold for 360 min, and cool at a cooling rate of 5 °C / min. When it cools down to 200 °C, it is cooled to room temperature with the furnace. The obtained ceramic material is polished with sandpapers of different mesh numbers to obtain a smooth and flat antiferroelectric laminated ceramic material.
[0089] The polarization-electric field hysteresis loops, energy storage density, and energy storage efficiency of the antiferroelectric ceramic samples obtained in this example are respectively shown in Figure 6 and Figure 7 . It can be seen that the samples in Example 3 significantly undergo an antiferroelectric to ferroelectric phase transition, with a breakdown strength of 550 kV / cm and an energy storage density of 6.76 J / cm 3 , and an energy storage efficiency of 71%.
[0090] Referring to the comparative example and Example 1, the pure lead ytterbium niobate antiferroelectric laminated ceramic material obtained by the lamination method has an energy storage density that is 1029% of that of the traditional solid-phase sintering method, and the energy storage efficiency slightly decreases due to the intrinsic characteristics of the antiferroelectric to ferroelectric phase transition.
[0091] Referring to Example 1, Example 2, and Example 3, their only difference lies in the sintering temperature. The pure lead ytterbium niobate antiferroelectric laminated ceramic material with a sintering temperature of 1080 °C has the best performance.
[0092] The preferred embodiments of the present invention disclosed above are only used to help illustrate the present invention. The preferred embodiments do not elaborate on all details and do not limit the invention to only the specific embodiments. Obviously, many modifications and variations can be made according to the content of this specification. These embodiments are selected and specifically described in this specification to better explain the principle and practical application of the present invention, so that those skilled in the art can well understand and utilize the present invention. The present invention is only limited by the claims and their full scope and equivalents.
Claims
1. A pure lead niobium ytterbium antiferroelectric laminated ceramic material, characterized in that, The chemical formula of the pure lead ytterbium niobate antiferroelectric laminated ceramic material is Pb(Yb 0.5 Nb 0.5 )O3.
2. The lead niobium ytterbium pure antiferroelectric laminated ceramic material according to claim 1, characterized in that, The effective energy storage density of the pure lead niobium ytterbiumate antiferroelectric laminated ceramic material is 8.44 J / cm under the test conditions of 20 °C and 10 Hz. 3 The energy storage efficiency is 68.29%.
3. A method for preparing a pure lead niobium ytterbium antiferroelectric laminated ceramic material as described in claim 1 or 2, characterized in that, It includes the following steps: S1. Mix a lead source, a ytterbium source, and a niobium source to obtain a mixed material; S2. Subject the obtained mixed material to ball milling, discharging, drying, and calcination in sequence to obtain a calcined powder; S3. Subject the obtained calcined powder to secondary ball milling and drying in sequence to obtain a dried powder. Then, mix the dried powder with an organic solvent, a binder, a dispersant, and a homogenizer to obtain a slurry; S4. Remove bubbles from the obtained slurry under vacuum, flow the de-bubbled slurry into a film, and dry it to obtain a pure lead ytterbium niobate thick film; S5. Subject the obtained pure lead ytterbium niobate thick film to processes of slicing, laminating, hot pressing, debinding, and sintering in sequence. After sintering, obtain a pure lead ytterbium niobate laminated ceramic material.
4. The preparation method according to claim 3, characterized in that, In step 1, the lead source is Pb3O4, the ytterbium source is Yb2O3, and the niobium source is Nb2O5.
5. The preparation method according to claim 3, characterized in that, In step S2, the ball milling medium is zirconia balls. The mass ratio of the mixed material, the ball milling medium, and alcohol is 1:1.5:1, and the ball milling time is 12 - 24 h; in step S3, the time for secondary ball milling is 12 - 24 h.
6. The preparation method according to claim 3, wherein In step S2, the temperature of the calcination process is 850 °C, and the calcination time is 2 h.
7. The preparation method according to claim 3, characterized in that, In step S3, first mix the pure lead ytterbium niobate dried powder with an organic solvent, a dispersant, and zirconia balls, and mix them evenly for 200 - 300 min to obtain a preliminary slurry. Then, mix it with a binder and a homogenizer, and mix them evenly for 200 - 300 min to obtain a final slurry; wherein, the organic solvent is toluene - ethanol, the dispersant is tributyl phosphate, the binder is polyethylene glycol, and the homogenizer is butyl phthalate.
8. The preparation method according to claim 3, characterized in that, In step S4, bubble removal is performed by a vacuum de-bubbling machine. The de-bubbling time is 25 - 60 min, and the drying time is 6 - 12 h.
9. The preparation method according to claim 3, characterized in that, In step S5, cut the pure lead ytterbium niobate thick film into pieces of 1 cm × 1 cm for lamination, and compact the laminated thick film by hot pressing. The pressure is 6 - 12 MPa, the time is 10 - 20 min, and the temperature is 60 - 80 °C; the specific process of debinding is as follows: put the hot-pressed pure lead ytterbium niobate laminated sheet into a muffle furnace, keep it at 500 - 600 °C for 300 - 600 min, the heating rate is 1 - 5 °C / min, and the cooling rate is 5 - 10 °C / min.
10. The preparation method according to claim 3, characterized in that, The specific process of sintering in step S5 is as follows: perform sintering in a muffle furnace, set the temperature from room temperature to 1060 - 1100 °C, the heating rate is 1 - 5 °C / min, the holding time is 200 - 400 min, the cooling rate is 5 - 10 °C / min. When it cools down to 200 °C, cool it to room temperature with the furnace, and then obtain a pure lead ytterbium niobate antiferroelectric laminated ceramic.