Low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic and method of making same
By doping BiDyO3 and Bi(Li1/2Nb1/2)O3 composite perovskite system into BaTiO3-based dielectric ceramics, the sintering temperature is reduced and the breakdown field strength and energy storage density are improved, solving the problem of high-temperature sintering of barium titanate-based ceramics and making it suitable for high-power pulse power supplies.
Patent Information
- Application Number
- CN202510126543.6
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- Filing Date
- 2025-01-27
- Publication Date
- 2025-10-17
- Estimated Expiration
- 2045-01-27
AI Technical Summary
The high sintering temperature of existing barium titanate-based ceramics leads to high production costs and insufficient energy storage density, making it difficult to meet the application requirements of high-power pulse power supplies.
Doping BiDyO3 and Bi(Li1/2Nb1/2)O3 composite perovskite system into BaTiO3-based dielectric ceramics can reduce the sintering temperature and improve the breakdown field strength and energy storage performance.
Low-temperature sintering (960~1060oC) is achieved, which greatly improves the breakdown field strength and energy storage density (up to 10.1 J/cm3) and reduces production costs, making it suitable for high-power pulse power supplies.
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Figure CN119822815B_ABST
Abstract
Description
TECHNICAL FIELD
[0001] The present application relates to the field of functional ceramics, in particular to a low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic and a preparation method thereof. BACKGROUND
[0002] As the core energy storage device of high-power pulse power supply, the dielectric capacitor has high power density, ultra-fast charging and discharging capacity, excellent thermal stability, and strong anti-aging performance, and plays a vital role in the development of military equipment and the realization of scientific research technology, such as heart pacemaker, camera flash, nuclear effect simulation, metal forming, and hybrid electric vehicle.
[0003] With the development of pulse power devices towards miniaturization and light weight and low cost, it is increasingly urgent to develop economical high-energy density dielectric materials. In the field of dielectric energy storage materials, there are four major categories of dielectric materials that can be used for energy storage: linear dielectric (LD), ferroelectric (FE), relaxor ferroelectric (RFE), and antiferroelectric (AFE). Barium titanate (BaTiO3) based ceramics are one of the best candidate materials for preparing ceramic capacitors due to their excellent electrical properties, including high dielectric constant and excellent ferroelectricity. Traditional barium titanate-based ceramics are ferroelectric, and the sintering temperature is high, which is higher than 1150 o C; the energy storage density is small, about 0.3 J / cm 3 , which cannot meet the needs of modern industry, and it is necessary to improve its performance.
[0004] Doping modification is the most effective means to reduce the sintering temperature of BaTiO3-based dielectric ceramics and improve their energy storage performance. Researchers have added Bi(Li 0.5 Nb 0.5 )O3 composite perovskite system to BaTiO3, and the sintering temperature of BaTiO3-xBi(Li 0.5 Nb 0.5 )O3-based dielectric ceramics is reduced to 1150 ° C, and the energy storage density is increased to 4.5 J / cm 3 (ACS Appl. Energy Mater. 2019, 2, 8, 5499-5506); in addition, researchers have also used low-melting-point B2O3-Na2B4O7-Na2SiO3 glass powder doping, which not only effectively reduces the sintering temperature of 0.85BaTiO3-0.15Bi(Mg 2 / 3 Nb 1 / 3 )O3 ceramic (750-1350 o C), but also improves its breakdown field strength, which can reach 220 kV / cm and the energy storage density is about 1.26 J / cm 3(J. Adv. Dielect. 2018, 8, 1850041). These works all show that BaTiO3-based ceramics have great application potential in the field of dielectric energy storage, but the high sintering temperature leads to high production cost and the energy storage density cannot meet the application requirements, which seriously limits its application in high-power pulse power supply. SUMMARY
[0005] To solve the above problems, the present application provides a low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic and a preparation method thereof. By doping BiDyO3 and Bi(Li 1 / 2 Nb 1 / 2 )O3 composite perovskite system in the BaTiO3-based dielectric ceramic component, the sintering temperature of the BaTiO3-based dielectric energy storage material is reduced, and its breakdown field strength and energy storage performance are improved; a high-performance material is provided to meet the development of high-power dielectric energy storage components such as pulse power supply.
[0006] In the first aspect, the present application provides a low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic, wherein the chemical formula of the barium titanate-based dielectric ceramic is (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein 0<x<0.1, 0<y<0.1.
[0007] Preferably, x is 0.04-0.07, and y is 0.03.
[0008] In the present application, by means of doping BiDyO3 and Bi(Li 1 / 2 Nb 1 / 2 )O3 composite perovskite system in the BaTiO3 component, the sintering temperature is reduced, and the breakdown field strength and energy storage density of the BaTiO3-based dielectric ceramic are greatly improved.
[0009] Preferably, the densification sintering temperature of the low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic is 960-1060 o C.
[0010] Preferably, the energy storage density of the low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic is 6.5-12.2 J / cm 3 , and the energy storage efficiency is 90.0-96.5%.
[0011] In the second aspect, the present application provides a preparation method of the low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic, comprising the following steps:
[0012] (1) Selecting barium titanate (BaTiO3), niobium pentoxide (Nb2O5), lithium oxide (Li2O), bismuth oxide (Bi2O3), and dysprosium oxide (Dy2O3) as raw materials, and according to the chemical formula (1-x-y) BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein y=0~0.1, x=0~0.1, after weighing, the raw materials are mixed with a solvent, a dispersant, a binder, and a plasticizer, and then cast to obtain a cast green film A.
[0013] (2) The cast green film A is cut to obtain a cast green film B, an electrode is printed on the surface of the cast green film B by silk screen printing to obtain a green film with an electrode, and the green film with the electrode is laminated by hot pressing to obtain a ceramic green body C.
[0014] (3) The multilayer ceramic green body C is arranged and sintered to obtain a barium titanate-based multilayer dielectric ceramic D.
[0015] (4) The barium titanate-based multilayer ceramic D is polished and coated with an end electrode to obtain the barium titanate-based multilayer dielectric energy storage ceramic.
[0016] Preferably, in step (1), the raw materials are weighed according to the chemical formula (1-x-y) BaTiO3-yBiDyO3-xBi(Li 1 / 2Nb 1 / 2 )O3, and the cast slurry is mixed in a ratio of 100 wt% of powder, 4~10 wt% of binder, 30~50 wt% of solvent, 0.6~1.1 wt% of dispersant, and 2~5 wt% of plasticizer.
[0017] The binder is polyvinyl butyral (PVB) with a molecular weight of 70000-270000; the solvent is a mixed solvent of p-xylene (30%) and anhydrous ethanol (70%), or a mixed solvent of butanone (40%) and anhydrous ethanol (60%), or a mixed solvent of butanone (88.6%) and water (11.4%), or a mixed solvent of anhydrous ethanol (68%) and toluene (32%), or a mixed solvent of anhydrous ethanol (27%) and trichloroethylene (63%), or a mixed solvent of n-propanone (88%) and butanone (12%), or a mixed solvent of acetone (88%) and toluene (12%), or a mixed solvent of P-xylene (17%) and n-propanone (83%), wherein the percentages are all volume fractions; the dispersant is soybean food oil, peanut oil or fish oil; and the plasticizer is a mixture of dibutyl phthalate (DBP) and polyethylene glycol (PEG-400), or a mixture of butyl benzyl phthalate (BBP) and polyethylene glycol (PEG-400), wherein the mass ratio of DBP to PEG-400 and the mass ratio of BBP to PEG-400 are both 1:1.
[0018] The above raw materials are mixed in a ball mill at a rotation speed of 220-300 rpm for 6-12 hours, and zirconia balls are used.
[0019] Preferably, in step (2), the thickness of the cast green film A is 10-50 microns; the electrode in the silk screen printing is an Ag-Pd electrode or a Cu electrode; the hot pressing temperature in the lamination is 60-80 ~80 o C, and the holding time is 1-5 min.
[0020] Preferably, in step (3), the temperature for the plastic removal is 400-600℃, and the time is 1-2 hours.
[0021] Preferably, in step (3), the sintering process is to increase the temperature to 960-1060℃ at a temperature increasing rate of 3-4℃ / min at room temperature, and the holding time is 1-3 hours.
[0022] Preferably, in step (4), the end electrode is a nickel electrode, a copper electrode or a silver electrode.
[0023] In a third aspect, the application provides a low-temperature sintered barium titanate-based multilayer dielectric element, which comprises the low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic and an electrode distributed on the surface of the barium titanate-based multilayer dielectric energy storage ceramic.
[0024] The application has the following beneficial effects:
[0025] Compared with the prior art, the application dopes BiDyO3 and Bi(Li 1 / 2 Nb 1 / 2)O3 composite perovskite system, effectively reduces the sintering temperature of BaTiO3 ceramic, and obtains excellent energy storage density (up to 10.1 J / cm 3 )and energy storage efficiency (energy storage efficiency up to 96.5%) of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based multilayer dielectric energy storage material, wherein the introduction of Bi(Li 1 / 2 Nb 1 / 2 )O3 can effectively reduce the sintering temperature of the ceramic; and the introduction of BiDyO3 can not only reduce the sintering temperature, but also effectively improve the breakdown field strength of the ceramic. The obtained material has the advantages of low cost, high voltage resistance, lead-free environmental protection, high energy storage density and energy storage efficiency, and is suitable for high-power pulse power field, and has very important application value. BRIEF DESCRIPTION OF DRAWINGS
[0026] In order to more clearly illustrate the technical solutions in the embodiments of the present application, the drawings needed in the embodiment description will be briefly introduced below. Obviously, the drawings in the following description are only some embodiments of the present application, and other drawings can also be obtained by those skilled in the art without creative labor.
[0027] Figure 1 It is the XRD pattern of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based dielectric energy storage material of Example 1, wherein x=0.04, y=0.03.
[0028] Figure 2 It is the SEM pattern of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based dielectric energy storage material of Example 1, wherein x=0.04, y=0.03.
[0029] Figure 3 It is the dielectric temperature spectrum of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based dielectric energy storage material of Example 1, wherein x=0.04, y=0.03.
[0030] Figure 4 It is the single-pole hysteresis loop of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based dielectric energy storage material of Example 1, wherein x=0.04, y=0.03.
[0031] Figure 5 XRD pattern of (1-x-y)BaTi03-yBiDy03-xBi(Li 1 / 2 Nb 1 / 2 )03-based dielectric energy storage material for Example 2, where x = 0.06, y = 0.03.
[0032] Figure 6 SEM image of (1-x-y)BaTi03-yBiDy03-xBi(Li 1 / 2 Nb 1 / 2 )03-based dielectric energy storage material for Example 2, where x = 0.06, y = 0.03.
[0033] Figure 7 Dielectric permittivity spectrum of (1-x-y)BaTi03-yBiDy03-xBi(Li 1 / 2 Nb 1 / 2 )03-based dielectric energy storage material for Example 2, where x = 0.06, y = 0.03.
[0034] Figure 8 Unipolar hysteresis loop of (1-x-y)BaTi03-yBiDy03-xBi(Li 1 / 2 Nb 1 / 2 )03-based dielectric energy storage material for Example 2, where x = 0.06, y = 0.03.
[0035] Figure 9 XRD pattern of (1-x-y)BaTi03-yBiDy03-xBi(Li 1 / 2 Nb 1 / 2 )03-based dielectric energy storage material for Example 3, where x = 0.07, y = 0.03.
[0036] Figure 10 SEM image of (1-x-y)BaTi03-yBiDy03-xBi(Li 1 / 2 Nb 1 / 2 )03-based dielectric energy storage material for Example 3, where x = 0.07, y = 0.03.
[0037] Figure 11 Dielectric permittivity spectrum of (1-x-y)BaTi03-yBiDy03-xBi(Li 1 / 2 Nb 1 / 2 )03-based dielectric energy storage material for Example 3, where x = 0.07, y = 0.03.
[0038] Figure 12For Example 3, (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based dielectric energy storage material, where x = 0.07, y = 0.03.
[0039] Figure 13 For Comparative Example 1, the dielectric temperature spectrum of pure BaTiO3-based dielectric energy storage material.
[0040] Figure 14 For Comparative Example 1, the unipolar hysteresis loop of pure BaTiO3-based dielectric energy storage material.
[0041] Figure 15 For Comparative Example 2, the dielectric temperature spectrum of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based dielectric energy storage material, where x = 0.00, y = 0.03.
[0042] Figure 16 For Comparative Example 2, the unipolar hysteresis loop of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based dielectric energy storage material, where x = 0.00, y = 0.03. DETAILED DESCRIPTION
[0043] To make the technical problems, technical solutions and advantages to be solved by the present application clearer, specific embodiments will be described in detail below with reference to the accompanying drawings.
[0044] The present application provides a low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic, having a molecular formula of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, where 0 < x < 0.1, 0 < y < 0.1. The multilayer dielectric energy storage ceramic has a low sintering temperature of about 960-1060 o C, excellent energy storage properties, an energy storage density of 6.5-12.2 J / cm 3 , and an energy storage efficiency of 96.5%. In particular, the (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based ceramic of the present application has a high breakdown field strength, high energy storage density and energy storage efficiency, and is low in price, making it a low-cost, high-performance pulsed high-power power supply element material.
[0045] Example 1
[0046] Preparation of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein x = 0.04, y = 0.03.
[0047] The ceramic material of the embodiment is prepared by solid phase sintering, and the following steps are specifically followed:
[0048] (1) The ingredients are calculated according to the formula: (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein x = 0.04, y = 0.03, and the required raw materials are: barium titanate (BaTiO3), niobium pentoxide (Nb2O5), lithium oxide (Li2O), bismuth oxide (Bi2O3), and dysprosium oxide (Dy2O3); the electronic balance is used for weighing, and the weighing is accurate to 0.001 g;
[0049] (2) The weighed raw materials are mixed and placed in a nylon tank, and anhydrous ethanol not higher than 1 / 3 of the tank height is added for mixing, and zirconia balls are used as the medium, and the nylon tank is placed on a horizontal ball mill for mixing for 8 hours, the zirconia ball particle sizes are 3 mm, 5 mm and 8 mm, and the mass ratio is 3:4:3. Pour the milled slurry into a tray and place it in an oven for drying; crush the dried powder to obtain a fine ceramic powder.
[0050] (3) The casting slurry is prepared according to the mass ratio of ceramic powder: PVB: solvent: dispersant: plasticizer = 100:4.2:35:0.61:2.4, wherein the solvent is a mixed solvent of butanone (40%) and anhydrous ethanol (60%), the dispersant is fish oil, and the plasticizer is dibutyl phthalate (DBP) and polyethylene glycol (PEG-400).
[0051] (4) Pour the casting slurry into a casting machine, wherein the knife edge height is 135 microns and the speed is 0.7 cm / s, to obtain a casting film.
[0052] (5) The film strip is cut and the platinum electrode is screen printed; the film strip with the printed electrode is laminated.
[0053] (6) The laminated sheet is cut and plasticized, and the plasticizing temperature is 600 o C and the holding time is 1 hour.
[0054] (7) The plasticized green body is sintered in an atmosphere, the sintering temperature is 1060°C, the sintering time is 3 hours, and the sample is taken out after natural cooling to room temperature.
[0055] The prepared barium titanate-based ceramic material is polished to expose the inner electrode; then a silver end electrode is coated on the exposed inner electrode to obtain a barium titanate-based multilayer dielectric energy storage material, which is subjected to structure and performance testing.
[0056] Example 2
[0057] (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein x = 0.06 and y = 0.03. Except that the value of x in step (1) and the sintering temperature in step (7) are different, the other steps are the same as in Example 1. The sintering temperature of this sample is 1030°C, and the sintering time is 3 hours.
[0058] Example 3
[0059] (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein x = 0.07 and y = 0.03. Except that the value of x in step (1) and the sintering temperature in step (7) are different, the other steps are the same as in Example 1. The sintering temperature of this sample is 980°C, and the sintering time is 3 hours.
[0060] Comparative Example 1
[0061] (1), according to the molecular formula: (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein x = 0.00 and y = 0.00, the raw materials required are only barium titanate (BaTiO3).
[0062] The sintering temperature of step (7) is 1360 o C, and the holding time is 2 hours. The other preparation processes are the same as in Example 1.
[0063] The prepared BaTiO3 ceramic is subjected to performance testing.
[0064] Comparative Example 2
[0065] (1), according to the molecular formula: (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein x = 0.00 and y = 0.03, the raw materials required are: barium titanate (BaTiO3), bismuth oxide (Bi2O3), and dysprosium oxide (Dy2O3); an electronic balance is used for weighing, and the weighing is accurate to 0.001 g.
[0066] The sintering temperature of step (7) is 1200o C, and other preparation processes are the same as those of Example 1.
[0067] The prepared (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3 ceramics, wherein x = 0.00, y = 0.03, were subjected to performance tests.
[0068] The sintering temperature and performance of the (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based dielectric energy storage materials prepared in Examples 1-3 were compared with those of Comparative Example 1-2, and the results are shown in Table 1. As can be seen from Examples 1 to 3, the sintering temperature of the (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3 ceramics is 960-1060 o C, wherein 0 < x < 0.1 mol, 0 < y < 0.1 mol; which is much lower than the sintering temperature of the BaTiO3 provided in Comparative Example 1 and the (1-y)BaTiO3-yBiDyO3 ceramics provided in Comparative Example 2, which are 1360 o C and 1200 o C, respectively. In addition, the breakdown field strength, energy storage density and energy storage efficiency of the Example ceramics are much greater than those of the BaTiO3 and (1-y)BaTiO3-yBiDyO3 ceramics.
[0069] Table 1 (0.97-x)BaTiO3-0.03BiDyO3-xBi(LiNb) 1 / 2 O3-based dielectric energy storage material performance comparison
[0070]
[0071] Figures 1-12 The phase structure and performance of the ceramics of Examples 1-3, wherein the components of Examples 1, 2 and 3 are (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein x = 0.04, y = 0.03, x = 0.06, y = 0.03 and x = 0.07, y = 0.03. Figure 1 、 5 and 9 are the XRD patterns of the ceramics of Examples 1-3, respectively, indicating that they are pure perovskite structures. Figure 2 、 6 and 10 are the SEM patterns of the ceramics of Examples 1-3, respectively, indicating that the ceramic samples are dense, and the grain size is about 2 μm. Figure 3 、7 and 11 are the dielectric temperature spectra of the ceramics of Examples 1-3, indicating that the sintering temperature of the ceramics is 960-1060 o C. Figure 4 , 8 and 12 are the monopolar hysteresis loops of the ceramics of Examples 1-3, indicating that the hysteresis is very small. Therefore, the ceramics of Examples 1-3 have high density and uniform grain size distribution at the sintering temperature of 960-1060 o C. In addition, the hysteresis of the hysteresis loop is very small. By comparing Examples 1-3, it can be seen that as the content of x increases, the sintering temperature of the ceramic sample decreases significantly. In addition, as the content of x increases, the energy storage efficiency of the ceramic sample also increases accordingly.
[0072] Figures 13-16 are the phase structures and properties of the comparative ceramic. Comparative Example 1 is pure BaTiO3, and x and y are both 0.00. Figure 13 is the dielectric temperature spectrum of the pure BaTiO3-based dielectric energy storage material, indicating that the sintering temperature of the pure BaTiO3 ceramic is relatively high, about 1360 o C. And the hysteresis of the hysteresis loop is large, as shown in Figure 14 . Similar to Comparative Example 1, Figure 15 is the dielectric temperature spectrum of the (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based dielectric energy storage material of Comparative Example 2, wherein x=0.00 and y=0.03, and the sintering temperature is 1200 o C. And the hysteresis of the hysteresis loop is also large, as shown in Figure 16 .
[0073] In addition to the above examples and comparative examples, the applicant also conducted the following comparative tests:
[0074] 1) (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based ceramic with x=0.2 and y=0.03 was prepared. Due to the high content of Bi(Li 1 / 2 Nb 1 / 2 )O3, a large amount of liquid phase appeared during sintering of the ceramic, and the ceramic after sintering appeared warped sheet, etc., and could not be tested for performance.
[0075] 2) (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based ceramic with x=0.1 and y=0.15 was prepared. Compared with (1-x-y)BaTiO3-yBiDyO3-xBi(Li1 / 2 Nb 1 / 2 )O3-based ceramic phase, x=0.1, y=0.15 of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based ceramic is also prone to warping due to excessive liquid phase content, and the ceramic cannot be tested for performance. Therefore, the suitable composition of (1-x-y)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3-based ceramic is 0
[0076] The above merely describes specific embodiments of the present application, but the protection scope of the present application is not limited thereto, and any person skilled in the art can easily think of changes or replacements within the technical range disclosed by the present application, which should be encompassed in the protection scope of the present application. Therefore, the protection scope of the present application should be subject to the protection scope of the claims.
Claims
1. A low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic, characterized in that: The chemical formula of the ceramic is (1-xy)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, where 0 < x< 0.1, 0 < y< 0.
1.
2. The low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic according to claim 1, characterized in that: Where x is 0.04~0.07, and y is 0.
03.
3. The low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic according to claim 1 or 2, characterized in that: The densification sintering temperature of the low temperature sintered barium titanate based multilayer dielectric energy storage ceramic is 960~1060 o C, energy storage density is 6.5~12.2 J / cm 3 , the energy storage efficiency is 90.0~96.5%.
4. The method for preparing the low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramic according to any one of claims 1 to 3, characterized in that: The following steps are involved: (1) Barium titanate, niobium pentoxide, lithium oxide, bismuth oxide, and dysprosium oxide were selected as raw materials and the mixture was prepared according to the chemical formula (1-xy)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3, wherein 0 < x < 0.1, 0 < y < 0.1, is weighed, mixed evenly with a solvent, a dispersant, a binder and a plasticizer, and then cast to obtain a cast green film A; (2) Slicing the obtained cast green film A to obtain cast green film B, printing electrodes on the surface of the cast green film B by screen printing to obtain a green film printed with electrodes, and hot pressing the green film printed with electrodes by hot pressing lamination technology to obtain a ceramic green film C; (3) The multilayer ceramic green body C is subjected to plastic removal and sintering to obtain a barium titanate-based multilayer dielectric ceramic D; (4) The barium titanate-based multilayer ceramic D is polished and coated with terminal electrodes to obtain the barium titanate-based multilayer dielectric energy storage ceramic.
5. The method for preparing low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramics according to claim 4, characterized in that: In step (1), the raw materials are prepared according to the chemical formula (1-xy)BaTiO3-yBiDyO3-xBi(Li 1 / 2 Nb 1 / 2 )O3 is weighed, and the ratio of the casting slurry is as follows: based on 100 wt% of the powder, the amount of the binder added is 4-10 wt%, the solvent is 30-50 wt%, the dispersant is 0.6-1.1 wt%, and the plasticizer is 2-5 wt%.
6. The method for preparing low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramics according to claim 5, characterized in that: The binder is polyvinyl butyral; the dispersant is soybean food oil, peanut oil or fish oil; and the plasticizer is a mixture of dibutyl phthalate and polyethylene glycol, or a mixture of butyl benzyl phthalate and polyethylene glycol.
7. The method for preparing low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramics according to claim 4, characterized in that: In step (2), the thickness of the cast green film A is 10-50 microns; the electrode in the screen printing is an Ag-Pd electrode or a Cu electrode; the hot pressing temperature in the lamination is 60-80 o C, insulation time 1~5min.
8. The method for preparing low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramics according to claim 4, characterized in that: In step (3), the temperature of the plastic discharge is 400-600°C, and the time is 1-2 hours; the sintering process is to increase the temperature to 960-1060°C at a heating rate of 3-4°C / min at room temperature and keep the temperature for 1-3 hours.
9. The method for preparing low-temperature sintered barium titanate-based multilayer dielectric energy storage ceramics according to claim 4, characterized in that: In step (4), the terminal electrode is a nickel electrode, a copper electrode or a silver electrode.
10. A low-temperature sintered barium titanate-based multilayer dielectric component, characterized in that: The invention comprises a barium titanate-based multilayer dielectric energy storage ceramic as described in any one of claims 1 to 3 or obtained by the preparation method according to any one of claims 4 to 9, and electrodes distributed on the surface of the barium titanate-based multilayer dielectric energy storage ceramic.
Citation Information
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