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1.
The electrical hysteresis behaviors and energy storage performance of Pb0.97La0.02(Zr0.58Sn0.335Ti0.085)O3 antiferroelectric (AFE) ceramics were studied under the combined effects of electric field and temperature. It was observed that the temperature dependence of recoverable energy density (Wre) of AFE ceramics depends critically on the applied electric field. While Wre at lower electric fields (<8 kV/mm) shows increasing tendency with increasing temperature from 20°C to 100°C, Wre at higher electric fields (>8 kV/mm) demonstrates decreasing dependence. There exists an appropriate electric field (8 kV/mm) under which the AFE ceramics exhibit nearly temperature‐independent Wre (the variation is less than 0.5% per 10°C). The underlying physical principles were also discussed in this study. These results indicate that the temperature dependence of Wre of AFE materials can be tuned through selecting appropriate electric fields and provide an avenue to obtain thermal stable energy storage capacitors, which should be of great interest to modern energy storage community.  相似文献   

2.
《Ceramics International》2019,45(13):15898-15905
Recently, the (Pb,La)(Zr,Ti)O3 antiferroelectric materials with slim-and-slanted double hysteresis loops have been widely drawn in the application of advanced pulsed power capacitors due to its low strain characteristic. In this work, the energy storage properties of (Pb0.895La0.07)(ZrxTi1-x)O3 ceramics with different Zr contents are researched thoroughly because the substitution of Ti4+ by Zr4+ can reduce the tolerance factor t, enhancing the antiferroelectricity. The polarization-electric field hysteresis loops of the PLZT ceramics become slimmer with increasing Zr content. The highest recoverable energy storage density (Wre) of 3.38 J/cm3 and ultrahigh energy efficiency (η) of 86.5% are achieved in (Pb0.895La0.07)(Zr0.9Ti0.1)O3 ceramic. The (Pb0.895La0.07)(Zr0.9Ti0.1)O3 ceramic also hold fairly thermal stability (relative variation of Wre is less than 28% over 30 °C-120 °C), excellent frequency stability (10–1000 Hz) and good fatigue endurance. These results demonstrate that the (Pb0.895La0.07)(Zr0.9Ti0.1)O3 ceramic can be a desirable material for dielectric energy storage capacitors, especially for pulse power technology.  相似文献   

3.
In this work, Pb1−3x/2LaxZrO3 (x = 0–0.12) (PLZ-x) antiferroelectric thin films were fabricated on Pt(111)/TiO2/SiO2/Si substrates using chemical solution method. Smaller cations (La3+) and vacancies were introduced into A-sites of perovskite structure to construct chemical pressure. According to phenomenological theory, chemical pressure can increase the energy barrier between antiferroelectric (AFE) and ferroelectric (FE) phase, and enhance antiferroelectricity of the system. As a result, a large energy storage density (Wre) of 23.1 J cm−3 and high efficiency (η) of 73% were obtained in PLZ-0.10 films, while PLZ-0 films displayed lower Wre (15.1 J cm−3) and η (56%). More importantly, PLZ-0.10 films exhibited an excellent cycling stability with a variation of ˜2% after 1 × 108 cycles. The results demonstrate that heavily La-doped PbZrO3 films with high energy storage density, high efficiency and excellent cycling stability can be considered as potential candidates for energy storage applications.  相似文献   

4.
Antiferroelectric (AFE) ceramics based on Pb(Zr,Sn,Ti)O3 (PZST) have shown great potential for applications in pulsed power capacitors because of their fast charge-discharge rates (on the order of nanoseconds). However, to date, it has been proven very difficult to simultaneously obtain large recoverable energy densities Wre and high energy efficiencies η in one type of ceramic, which limits the range of applications of these materials. Addressing this problem requires the development of ceramic materials that simultaneously offer a large ferroelectric-antiferroelectric (FE-AFE) phase-switching electric field EA, high electric breakdown strength Eb, and narrow polarization-electric field (P-E) hysteresis loops. In this work, via doping of La3+ into (Pb1-1.5xLax)(Zr0.5Sn0.43Ti0.07)O3 AFE ceramics, large EA and Eb due to respectively enhanced AFE phase stability and reduced electric conductivity, and slimmer hysteresis loops resulting from the appearance of the relaxor AFE state, are successfully obtained, and thus leading to great improvement of the Wre and η. The most superior energy storage properties are obtained in the 3?mol% La3+-doped (Pb1-1.5xLax)(Zr0.5Sn0.43Ti0.07)O3 AFE ceramic, which simultaneously exhibits at room temperature a large Wre of 4.2?J/cm3 and a high η of 78%, being respectively 2.9 and 1.56 times those of (Pb1-1.5xLax)(Zr0.5Sn0.43Ti0.07)O3 AFE ceramics with x?=?0 (Wre?=?1.45?J/cm3, η?=?50%) and also being superior to many previously published results. Besides, both Wre and η change very little in the temperature range of 25–125?°C. The large Wre, high η, and their good temperature stability make the Pb0.955La0.03(Zr0.5Sn0.43Ti0.07)O3 AFE ceramic attractive for preparing high pulsed power capacitors useable in various conditions.  相似文献   

5.
Energy storage capacitors with high recoverable energy density and efficiency are greatly desired in pulse power system. In this study, the energy density and efficiency were enhanced in Mn-modified (Pb0.93Ba0.04La0.02)(Zr0.65Sn0.3Ti0.05)O3 antiferroelectric ceramics via a conventional solid-state reaction process. The improvement was attributed to the change in the antiferroelectric-to-ferroelectric phase transition electric field (EF) and the ferroelectric-to-antiferroelectric phase transition electric field (EA) with a small Mn addition. Mn ions as acceptors, which gave rise to the structure variation, significantly influenced the microstructures, dielectric properties and energy storage performance of the antiferroelectric ceramics. A maximum recoverable energy density of 2.64 J/cm3 with an efficiency of 73% was achieved when x = 0.005, which was 40% higher than that (1.84 J/cm3, 68%) of the pure ceramic counterparts. The results demonstrate that the acceptor modification is an effective way to improve the energy storage density and efficiency of antiferroelectric ceramics by inducing a structure variation and the (Pb0.93Ba0.04La0.02)(Zr0.65Sn0.3Ti0.05)O3-xMn2O3 antiferroelectric ceramics are a promising energy storage material with high-power density.  相似文献   

6.
Enhancing the efficiency in energy storage capacitors minimizes energy dissipation and improves device durability. A new efficiency-enhancement strategy for antiferroelectric ceramics, imposing relaxor characteristics through forming solid solutions with relaxor compounds, is demonstrated in the present work. Using the classic antiferroelectric (Pb0.97La0.02)(Zr1-x-ySnxTiy)O3 as model base compositions, Bi(Zn2/3Nb1/3)O3 is found to be most effective in producing the “relaxor antiferroelectric” behavior and minimizing the electric hysteresis. Specifically, a remarkable energy storage efficiency of 95.6% (with an energy density of 2.19 J/cm3 at 115 kV/cm) is achieved in the solid solution 0.90(Pb0.97La0.02)(Zr0.65Sn0.30Ti0.05)O3–0.10Bi(Zn2/3Nb1/3)O3. The validated new strategy, hence, can guide the design of future relaxor antiferroelectric dielectrics for next generation energy storage capacitors.  相似文献   

7.
Lead-free dielectric materials with high breakdown electric field strength and energy density are required for pulsed power devices with high level of integration. This work describes: (Ag0.94La0.02)(Nb1-xTax)O3 lead-free antiferroelectric ceramics, which were prepared by rolling process. Following composition engineering, an outstanding energy density of 6.9 J cm-3 at electric field of 490 kV cm-1 was achieved, coupled with remarkable frequency stability (<1% over 1-100 Hz under E = 420 kV cm-1) for (Ag0.94La0.02)(Nb0.80Ta0.20)O3 ceramics. Moreover, it also shows excellent charge-discharge properties (discharge density = 1429 A cm-2, power density = 144 MW cm-3). The addition of La3+ and Ta5+ induced a disordered local structure, which gradually decreased the phase transition temperature of M2-M3 to room temperature, reflecting the enhanced antiferroelectricity. All advantageous properties observed for the La and Ta co-doped AgNbO3 ceramics highlight their significant potential for energy storage applications.  相似文献   

8.
《Ceramics International》2022,48(12):16933-16943
A novel strategy to improve the energy-storage density and efficiency of the antiferroelectric (Pb0.93Ba0.04La0.02)(Zr0.65Sn0.3Ti0.05)O3 (PBLZST) ceramics is presented by forming ceramic solid solutions. The introduction of linear dielectric Ca(Zr0.5Ti0.5)O3 into PBLZST can effectively increase the breakdown strength, the antiferroelectric-to-ferroelectric phase transition field (EF) and the ferroelectric-to-antiferroelectric phase transition field (EA), while decreasing ΔE = EF - EA and the dielectric loss. This novel strategy leads to an ultrahigh efficiency of 94% and a remarkably high density of 4.14 J/cm3 in the PBLZST-based ceramics. The fundamental origins of high energy-storage density and efficiency are attributed to the enhanced tolerance factor and electronegativity difference in the complex perovskite structure, as well as the linear dielectric properties of Ca(Zr0.5Ti0.5)O3. Our results qualify the antiferroelectric PBLZST ceramics as innovative and promising candidate for energy storage applications. Furthermore, it points out an effective approach to achieve high efficiency in antiferroelectric by forming ceramics with linear dielectric.  相似文献   

9.
The lead-free Ba0.53Sr0.47TiO3 (BST) thin films buffered with La0.67Sr0.33MnO3 (LSMO) bottom electrode of different thicknesses were fabricated by pulsed laser deposition method on a (001) SrTiO3 substrate. It was found that the roughness of electrode decreases and substrate stress relaxes gradually with the increase of LSMO thickness, which is beneficial for weakening local high electric field and achieving higher Eb. Therefore, the recoverable energy density (Wrec) of BST films can be greatly improved up to 67.3 %, that is, from 30.6 J/cm3 for the LSMO thickness of 30 nm up to 51.2 J/cm3 for the LSMO thickness of 140 nm after optimizing the LSMO thickness. Furthermore, the thin film capacitor with a 140 nm LSMO bottom electrode shows an outstanding thermal stability from 20 °C to 160 °C and superior fatigue resistance after 108 electrical cycles with only a slightly decrease of Wrec below 1.6 % and 3.7 %, respectively. Our work demonstrates that optimizing bottom electrodes thickness is a promising way for enhancing energy storage properties of thin-film capacitors.  相似文献   

10.
Dielectric capacitors have drawn increasing attention due to their fast charge/discharge rates and high power density. Among all known ceramic dielectric materials, antiferroelectrics are more attractive for their unique double ferroelectric hysteresis loops and higher energy densities. Here, a series of antiferroelectric ceramics x(0.95Bi0.5Na0.5TiO3-0.05SrZrO3)-(1-x)NaNbO3 (xBNTSZ-(1-x)NN, x = 0.23, 0.30, 0.35, 0.50) have been prepared. By stabilizing the antiferroelectric phase and postponing the critical electric field of the antiferroelectric-ferroelectric phase transition, an impressive discharge energy storage density of 4.08 J/cm3 at a breakdown strength of 370 kV/cm was achieved for the 0.35BNTSZ-0.65 N N. A superior comprehensive performance for the 0.50BNTSZ-0.50 N N ceramic with a discharge energy storage density (Wdis) of 3.78 J/cm3 and an efficiency of 86 % at an electric field strength of 320 kV/cm along with excellent frequency, temperature, and fatigue stabilities (fluctuations of Wdis≤±5% within 0.01∼100 Hz, Wdis≤10 % over 20∼140 °C, and Wdis≤1% over 106 cycle numbers) is realized. Furthermore, 0.50BNTSZ-0.50 N N ceramics simultaneously exhibit a high current density (622.5 A/cm2), high power density (112 MW/cm3), and fast discharge rate (t = 47 ns), all of which make it an excellent candidate for the pulsed power devices.  相似文献   

11.
The different Si-Mg co-doping content was explored to improve the dielectric properties of amorphous Al2O3 thin film. According to the analysis of DSC, FT-IR, and XPS spectra, it can be confirmed that a novel structure of glass network is formed in the co-doped Al2O3 thin film. More importantly, compared to Al2O3 thin film, the leakage current of (Al.97Si.02Mg.01)2Oy thin film is reduced by 2 orders of magnitude and the breakdown strength is improved from 276?MV/m to 544?MV/m. The corresponding energy density of the modified sample is up to 9.2?J/cm3, which is an enhancement of 6.2?J/cm3 over that of the undoped Al2O3 thin film. Based on finite element analysis, the simulation results show that the applied electric field is mainly focused on the glass network, which could strengthen the stability of Al2O3 structure and decrease the breakdown probability of the films. From the viewpoint of defect chemistry, another reason for the enhancement of the dielectric properties is that Si-Mg co-doping results in the generation of cation vacancies and thus the formation of oxygen vacancies could be effectively prevented. This work could provide a new design strategy for high-performance dielectric capacitor devices.  相似文献   

12.
The antiferroelectric/ferroelectric (PbZrO3/PbZr0.52Ti0.48O3) bilayer thin films were fabricated on a Pt(111)/Ti/SiO2/Si substrate using sol‐gel method. PbZr0.52Ti0.48O3 layer acts as a buffered layer and template for the crystallization of PbZrO3 layer. The PbZrO3 layer with improved quality can share the external voltage due to its smaller dielectric constant and thinner thickness, resulting in the enhancements of electric field strength and energy storage density for the PbZrO3/PbZr0.52Ti0.48O3 bilayer thin film. The greatly improved electric breakdown strength value of 2615 kV/cm has been obtained, which is more than twice the value of individual PbZr0.52Ti0.48O3 film. The enhanced energy storage density of 28.2 J/cm3 at 2410 kV/cm has been achieved in PbZrO3/PbZr0.52Ti0.48O3 bilayer film at 20°C, which is higher than that of individual PbZr0.52Ti0.48O3 film (15.6 J/cm3). Meanwhile, the energy storage density and efficiency of PbZrO3/PbZr0.52Ti0.48O3 bilayer film increase slightly with the increasing temperature from 20°C to 120°C. Our results indicate that the design of antiferroelectric/ferroelectric bilayer films may be an effective way for developing high power energy storage density capacitors with high‐temperature stability.  相似文献   

13.
Dielectric capacitors possessing large energy storage density, high efficiency and high thermal stability simultaneously are very attractive in modern electronic devices to be operated in harsh environment. Here, it is demonstrated that large energy storage density (W?~?15.5?J/cm3), ultra-high efficiency (η ~93.7%) and high thermal stability (the variation of both W from 20?°C to 260?°C and η from 20?°C to 140?°C is less than 5%) have been simultaneously achieved in the La-doped (Ba0.904Ca0.096)0.9775+xLa0.015(Zr0.136Ti0.864)O3 (x?=?0.0075) lead-free relaxor ferroelectric thin film capacitors deposited on LaNiO3/Pt composite bottom electrodes by using a sol-gel method. The good energy storage property of the thin film capacitors at x?=?0.0075 is mainly ascribed to the diversity of the structure of the nano-clusters around the three-phases coexisting component point (Ba0.904Ca0.096)(Zr0.136Ti0.864)O3 where cubic, tetragonal and rhombohedral phases coexisted, as well as the ultra-high quality of thin film due to the utilization of the LaNiO3/Pt composite bottom electrode, making it a promising candidate for dielectric capacitors working in harsh environments.  相似文献   

14.
Antiferroelectric (AFE) ceramic materials possess ultrahigh energy storage density due to their unique double hysteresis characteristics, and PbZrO3 is one of the promising systems, but previous materials still suffer from the problem that energy storage density and energy storage efficiency can hardly be improved synergistically. In this work, a multiple optimization strategy is proposed to substantially improve the energy storage efficiency while maintaining the high energy storage density of PZ-based AFE ceramics. Sr2+-doped (Pb0.90La0.02Sr0.08)[(Zr0.5Sn0.5)0.9Ti0.1]0.995O3 ceramics was successfully synthesized by viscous polymer process and two-step sintering. The diffuse phase transition constructed in this ceramic depleted the threshold electric field hysteresis and current while the breakdown field strength was increased again. An ultrahigh recoverable energy density (Wrec) of 7.9 J/cm3 with a high energy storage efficiency (η) of 96.4 % are achieved synchronously at an electric field of 510 kV/cm. Moreover, the AFE ceramics possess remarkable discharge energy storage properties with a high discharge energy density (Wd) of 7.4 J/cm3 and a large power density (Pd) of 224 MW/cm3.  相似文献   

15.
The applications of antiferroelectric (AFE) materials in miniaturized and integrated electronic devices are limited by their low energy density. To address the above issue, the antiferroelectricity of the reinforced material was designed to improve its AFE-ferroelectric (FE) phase transition under electric fields. In this present study, the composition of Zr4+ (0.72 Å) and Ti4+ (0.605 Å) at B-site of Pb0.97La0.02(ZrxSn0.05Ti0.95-x)O3 ceramics with orthogonal reflections are synthesized via the tape-casting method. These ceramics are modified to enhance their antiferroelectricity by reducing their tolerance factor. A recoverable energy storage density Wrec 12.1 J/cm3 was obtained for x = 0.93 under 376 kV/cm, which is superior value than reported until now in lead-based energy storage systems. Moreover, the discharge energy density can reach 10.23 J/cm3, and 90 % of which can be released within 5.66 μs. This work provides a new window and potential materials for further industrialization of pulse power capacitors.  相似文献   

16.
A series of (1-x)(Sr0.7Ba0.3)5LaNb7Ti3O30x(Bi0.5Na0.5)TiO3 (x = 0.1–0.4) ceramics with tungsten bronze structure were prepared by solid state reaction. Phase composition, microstructure and energy storage properties were studied. When x = 0.3, excellent thermal stability satisfying the X7R specification was obtained and its energy storage as well as charge-discharge performances were further evaluated. Release energy density (Wre) of 0.77 J/cm3 and an energy storage efficiency of 97.3 % were detected at a low electric field of 20 kV/mm. Under the electric field of 10 kV/mm, the change of Wre in the temperature range of −55 °C to 125 °C is less than 15 % compared to room temperature. Short discharge period (∼0.17 μs), high power density (61.2 MW/cm3) and high discharge energy density (2.45 J/cm3) were evaluated by charge-discharge tests. Excellent thermal stability, high energy storage efficiency and high power density indicate that 0.7(Sr0.7Ba0.3)5LaNb7Ti3O30–0.3(Bi0.5Na0.5)TiO3 ceramic is a promising pulse capacitor for working over a wide temperature range.  相似文献   

17.
Antiferroelectric (AFE) materials have superior energy storage properties in high power multilayer ceramic capacitors (MLCCs). To adapt to the sintering temperature of inner metal electrodes with less palladium content, in this work, Al2O3 was added to Pb0.95La0.02Sr0.02(Zr0.50Sn0.40Ti0.10)O3 (PLSZST) AFE ceramics, in an attempt to reduce the sintering temperature. Results of this study demonstrate that the optimal composition of PLSZST-0.8 wt% Al2O3 sintered at a lower temperature 1040 ℃, has a high recoverable energy density (Wre, 3.23 J/cm3) and a high efficiency (η, 90 %) at room temperature. It is also high in pulse discharge energy density (Wdis, 2.45 J/cm3), current density (1369 A/cm2), and has an extremely short period of discharge (less than 500 ns). In addition, both Wre and η demonstrate a good stability in temperature within a wide range of 30 ℃-100 ℃. In sum, this novel AFE composition has great potentials for energy storage applications such as high energy density MLCCs.  相似文献   

18.
Lead-free NaNbO3 (NN) antiferroelectric ceramics provide superior energy storage performance and good temperature/frequency stability, which are solid candidates for dielectric capacitors in high power/pulse electronic power systems. However, their conversion of the antiferroelectric P phase to the ferroelectric Q phase at room temperature is always accompanied with large remnant polarization (Pr), which significantly reduces their effective energy storage density and efficiency. In this study, to optimize the energy storage properties, short-range antiferroelectric (0.95-x)NaNbO3-xBi(Mg2/3Nb1/3)O3-0.05CaZrO3 (xBMN) ceramics were designed to stabilize the antiferroelectric phase, in which the local random fields were simultaneously constructed. The results showed that the antiferroelectric orthorhombic P phase was transformed into the R phase, and the local short-range random fields were generated, which effectively inhibited the hysteresis loss and Pr. Of great interest is that the 0.12BMN ceramics displayed a large recoverable energy storage density (Wrec) of 5.9 J/cm3 and high efficiency (η) of 85% at the breakdown strength (Eb) of 640 kV/cm. The material also showed good frequency stability in the frequency range of 2–300 Hz, excellent temperature stability in the temperature range of 20–110 ℃, and a very short discharge time (t0.9∼4.92 μs). These results indicate that xBMN ceramics have great potential for advanced energy storage capacitor applications.  相似文献   

19.
The polarization hysteresis loops and the dynamics of domain switching in ferroelectric Pb(Zr0.52Ti0.48)O3 (PZT), antiferroelectric PbZrO3 (PZ) and relaxor-ferroelectric Pb0.9La0.1(Zr0.52Ti0.48)O3 (PLZT) thin films deposited on Pt/Ti/SiO2/Si substrates were investigated under various bipolar electric fields during repetitive switching cycles. Fatigue behavior was observed in PZT thin films and was accelerated at higher bipolar electric fields. Degradation of energy storage performance observed in PZ thin films corresponds to the appearance of a ferroelectric state just under a high bipolar electric field, which could be related to the nonuniform strain buildup in some regions within bulk PZ. Meanwhile, PLZT thin films demonstrated fatigue-free in both polarization and energy storage performance and independent bipolar electric fields, which are probably related to the highly dynamic polar nanodomains. More importantly, PLZT thin films also exhibited excellent recoverable energy-storage density and energy efficiency, extracted from the polarization hysteresis loops, making them promising dielectric capacitors for energy-storage applications.  相似文献   

20.
《Ceramics International》2021,47(18):25794-25799
To develop and fabricate environmentally friendly dielectric capacitors used in high-temperature environment, in this work, we prepare La3+ doped 0.94Na0.5Bi0.5TiO3-0.06BaTiO3 lead-free relaxor ferroelectric ceramics with high and wide phase transition temperature. With the introduction of La3+, due to the enhancement of the A- and B- site cation ion disorder, the dielectric relaxation characteristics of the ceramics are more obvious. Therefore, the polarization-electric field loops become slimmer and the remnant polarization (Pr) reduces. In addition, because La3+ as a donor dopant has lower mobility than A-site cation ions in the ceramic matrix, the grain sizes decrease with increasing La3+ content, which significantly leads to an increase in the breakdown strength (Eb). As a result, both a large recoverable energy density (Wrec) of 1.92 J/cm3 and a high energy efficiency (η) of 85.7% are obtained in the ceramic with 12 mol% La3+ content. More importantly, even at 200 °C and a low driving electric field of 155 kV/cm, the Wrec and η of this kind of ceramic are still as high as 1.2 J/cm3 and 89.4%, indicating good temperature stability. This work provides an effective and simple way to prepare environmentally friendly dielectric capacitors that are applicable in high-temperature environment.  相似文献   

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