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Due to the high demand for dielectric materials with high energy density, the energy storage performance of antiferroelectric ceramic capacitors has always gained much attention. Polarization intensity is a key factor that is closely related to the energy storage density. However, thus far, there has been a lack of research studies or successful methods to effectively modulate polarization intensity. The behavior of the polarization process is complex and contains domain nucleation, growth, and flip-flapping. Based on this finding, the introduction of Nb5+ at the B-site was designed to influence the three stages of antiferroelectric polarization by regulating the balance between the ferroelectric and antiferroelectric phases, and eventually realized regulation of the saturation polarization intensity in the (Pb 1-1.5x La x)(Zr 0.5 Sn 0.43 Ti 0.07)O 3 antiferroelectric ceramics. The saturation polarization intensity has increased from 25.56 to 42 μC/cm2 with Nb5+ content increases from 0 to 4 mol% and the hysteresis was kept low, Pb 0.94 La 0.04 (Zr 0.65 Sn 0.35) 0.975 Nb 0.02 O 3 is the optimal component with a high releasable energy density of 8.26 J/cm3 and an energy storage efficiency of 90.31%. This work provides an in-depth explanation of the microscopic mechanism of antiferroelectric ceramic polarization and presents a novel approach for the composition design of high-energy storage density antiferroelectric ceramics. [ABSTRACT FROM AUTHOR]

The most promising candidates for energy storage capacitor application are relaxor ferroelectrics, among which, the perovskite structure ferroelectric ceramics have witnessed great development progress. However, less attention has been paid on tetragonal tungsten bronze structure (TTBS) ceramics because of their lower breakdown strength and polarization. Herein, a multiscale regulation strategy is proposed to tune the energy storage performances (ESP) of TTBS ceramics from grain, domain, and macroscopic scale. The enhanced relaxor behavior with dynamic polar nanodomains guarantees low remanent polarization, while the refined grains and enlarged bandgap ensure increased breakdown strength. Hence, excellent ESP is realized in unfilled TTBS Sr0.425La0.1□0.05Ba0.425Nb1.4Ta0.6O6 (SLBNT) ceramics with an ultrahigh recoverable energy density of 5.895 J cm−3 and a high efficiency of 85.37%. This achievement notably surpasses previous studies in TTBS ceramics and is comparable to that of perovskite components. Meanwhile, the energy density exhibits a wide temperature, frequency, and cycling fatigue stability. In addition, high power density (257.89 MW cm−3), especially the ultrafast discharge time (t0.9 = 16.4 ns) are achieved. The multiscale regulation strategy unlocks the energy storage potential of TTBS ceramics and thus highlights TTBS ceramics as promising candidates for energy storage, like perovskite structured ceramics. [ABSTRACT FROM AUTHOR]

(Pb, La)(Zr, Ti)O3 antiferroelectric (AFE) materials are promising materials due to their energy‐storage density higher than 10 J cm−3, but their low energy‐storage efficiency and poor temperature stability limit their application. In this paper, the (1 − x)(Pb0.9175La0.055)(Zr0.975Ti0.025)O3–xPb(Yb1/2Nb1/2)O3 (PLZTYN100x) AFE ceramics were prepared via two‐step sintering method and investigated thoroughly. With the doping of Yb3+ and Nb5+, the phase structure transforms from the orthorhombic phase (AFEO) to the coexistence of the orthorhombic‐and‐tetragonal phases. This structure reduces the free energy difference between the AFE and ferroelectric phases and reduces the fluctuation of energy with temperature, improving the energy storage efficiency and temperature stability. When the x = 0.05 (PLZTYN5), the AFE ceramic exhibits excellent temperature stability and ultrahigh energy storage performance, whose recoverable energy density (Wrec) is 6.8–8.2 J cm−3 at 30 kV mm−1 in the temperature range from −55 to 75°C, and efficiency (ƞ) is 78%–86.7%. In addition, the change of Wrec is less than 15%, exceeding the performance of most AFE ceramics. The results demonstrate that the PLZTYN5 ceramic has great potential in pulse power capacitors. [ABSTRACT FROM AUTHOR]

The energy storage performance of antiferroelectric ceramic capacitors has always gain much attention. Hysteresis, transition field, and polarization intensity are crucial factors influencing energy storage performance. A‐site doped small radius ions have been shown in numerous investigations to enhance the switching field, minimize hysteresis, but decrease maximum polarization intensity. How to maintain the high polarization while optimizing other parameters is a great challenge, and this problem has received scant attention in the research literature to date. In this work, Pb1‐xSrx(Zr0.54Sn0.46)0.975Nb0.02O3 (x = 0, 0.02, 0.06, 0.08, 0.1, 0.12, 0.14, 0.16, 0.20) antiferroelectric ceramics show high polarization stability. When the Sr2+ content is within 12 mol%, the saturation polarization intensity always remains at a large value (> 44μC/cm2), and the rate of change is as low as 6%. Pb0.92Sr0.08(Zr0.54Sn0.46)0.975Nb0.02O3 also displays great polarization temperature stability with a minimal change rate of 8.5% in a wide temperature range from ‐55 to 85°C. Additionally, this ceramic also has a superior energy storage performance that the recoverable energy density and energy storage efficiency and 8.95 J/cm3 and 80.4%, respectively. This work paves the way for practical simultaneous polarization and other parameter optimization. [ABSTRACT FROM AUTHOR]

• Achieving ultrahigh W rec of 10.0 J/cm3 and η of 91 % in BST-based ceramics. • The variation of relaxor feature is analyzed by multi-polarization mechanism model. • Simultaneously toughening and enhanced energy storage performance are realized. Lead-free ceramic capacitors offer ultrahigh power density and ultrafast discharging rates, making them critical energy storage components for advanced pulsed power systems. However, the greatest obstacle to broader applications remains the relatively low energy storage density. In this study, a relaxor ferroelectric ceramic based on (0.6-x)Ba 0.55 Sr 0.45 TiO 3 -0.4Bi 0.5 Na 0.5 TiO 3 -xSrZrO 3 ((0.6-x)BST-0.4BNT-xSZ) is prepared using the tape casting method, resulting in an excellent energy density (W rec ≈ 10.0 J cm−3) and high energy storage efficiency (η ≈ 91 %). The solid solution of linear dielectrics SrZrO 3 synergistically regulates both relaxor properties and breakdown strength. The variation of relaxor property was explored utilizing New Glass model and the multi-polarization model, with confirmation provided by piezoresponse force microscopy. Furthermore, the breakdown strength could be attributed to improvements in electric insulation and the widening of the bandgap. As SrZrO 3 content increases, the in-situ emergence of the second phase ZrO 2 , accompanied by a martensitic transformation, not only improves the fracture toughness of ceramics but also serves to elongate the breakdown path. Encouragingly, x = 0.20 ceramics also achieve excellent temperature stability (−95–125 ℃), frequency stability (1–1000 Hz), cycling reliability (1–106 cycles), and great charging-discharging properties. This multiscale synergic regulation strategy plays a guiding role in the screening of high-performance energy storage dielectric materials. [ABSTRACT FROM AUTHOR]

• An ever-unadoped strategy was employed to design superparaelectric phase in AgNbO 3. • A new simple composition to obtain high ESP ceramic materials is proposed. • High W rec of 7.6 J/cm3 and E b of 522 kV/cm are obtained. Ceramics capacitors, especially featuring antiferroelectric (AFE) structure, are widely used in pulsed power electronic systems due to distinctive high-power density and external field stability. Lead-free AFE material AgNbO 3 has seized substantial research attention owing to its unique temperature driven multi-level phase transitions, and many works have greatly improved the energy storage properties by engineering these temperature-dependent phase boundaries. In this work, an ever-unadopted strategy was proposed to modulate the relaxor structure in AgNbO 3 by designing room-temperature (RT) superparaelectric phase via Bi incorporation into AN lattice matrix. Structural analysis shows M phase (space group Pbcm) evolves into O phase (space group Cmcm) with 12 mol.% Bi-substitution, breaking the long-range AFE order into polar nanoregions. Hence, an ultra-high recoverable energy density (7.6 J/cm3) and a high efficiency (79 %) are simultaneously achieved in the Ag 0.64 Bi 0.12 NbO 3 ceramics under 52.2 kV/mm. Moreover, the excellent energy storage properties are accompanied with good temperature and frequency stability, with the variation of W rec less than ± 15% (over 25–120 °C) and ± 10% (over 1–200 Hz) under 25 kV/mm, respectively. The novel approach reported herein provides a new guidance for designing AgNbO 3 -based and other AFE materials for high-performance energy storage applications. [ABSTRACT FROM AUTHOR]

Barium Strontium Titanate (Ba 1-x Sr x TiO 3 , BST) possesses the advantages of high permittivity, low remnant polarization and dielectric loss, suggesting great potential in the application of power capacitors. However, the low maximum polarization severely restricts the achievement of outstanding energy storage properties (ESP). Herein, we design a lead-free bulk ceramic: (1-x)Ba 0. 55 Sr 0 · 45 TiO 3 -xBi 0.5 Na 0. 5 TiO 3 [(1-x)BST-xBNT] (x = 0.1–0.4), prepared by two-step solid-state reaction method. The introduction of BNT contributes to (1) the boost of maximum polarization (from 21 μC/cm2 up to 32.6 μC/cm2) due to Bi3+ lone pair covalent effect (2) strong relaxor behavior (1.71≪ γ 1.84) derived from weakly coupled nanopolar regions, which can be verified by high activation energy E a = 0.341 eV at x = 0.3, improves the ESP and thermal stability of the ceramics. According to the above strategies, high W rec = 1.73 J/cm3 and η = 84.4% are achieved in the 0.7BST-0.3BNT ceramics at 206 kV/cm, which is preferable to the previous results regarding BST-based bulk ceramics. The excellent thermal stability (20–120 °C), frequency stability (1–500 Hz), as well as anti-fatigue characteristic (cycling number: 105) were obtained in the 0.7BST-0.3BNT. Furthermore, 0.7BST-0.3BNT ceramics exhibit high-power density (P D = 44.9 MW/cm3) and rapid discharge rate (t 0.9 = 99.2 ns) from 20 °C to 120 °C. This work provides a feasible way to achieve good energy storage and charge-discharge properties for pulse power energy storage systems. [ABSTRACT FROM AUTHOR]

Ceramic‐based dielectric capacitor are highly suitable for pulsed power applications due to their high power density and excellent reliability. However, the ultrahigh applied electric field limit their applications in integrated electronic devices. In this work, (1−x){0.96(Bi0.5Na0.5)(Ti0.995Mn0.005)O3‐0.04BiAlO3}‐xNaNbO3 (BNT‐BA‐xNN, x = 0, 0.04, 0.08, 0.12, and 0.16) ternary ceramics were designed to achieve excellent energy storage properties. It was found that the introduction of NaNbO3 (NN) effectively increase the difference (ΔP) between Pmax and Pr, resulting in an obvious enhancement of the energy storage properties. High recoverable energy storage density, responsivity, and power density, that is, Wrec = 2.01 J/cm3, ξ = Wrec/E = 130.69 J/(kV⋅m2), and PD = 25.59 MW/cm3, accompanied with superior temperature stability were realized at x = 0.14 composition. In addition, the thermal stable dielectric properties of the sample can be prominently improved with increasing NN content. The temperature coefficient of capacitance (TCC) of x = 0.16 composition is lower than 15% over the temperature range from 49°C to 340°C, with a high dielectric permittivity of 1647 and a low dielectric loss (0.0107) at 150°C. All these features show that the BNT‐BA‐xNN ceramics are promising materials for energy storage application. [ABSTRACT FROM AUTHOR]

(Pb, La)(Zr, Sn, Ti)O 3 (PLZST) ceramic is one of the most prospective antiferroelectric (AFE) materials for variety of functional applications including energy storage and converter. Systematic structural investigation of domain structures should be of fundamental importance for understanding the structure-property relationship in AFE ceramics. In this study, the hierarchical domain structures and modulated structures correlated to the compositional variation in (Pb 0.97 La 0.02) (Zr 0.50 Sn x Ti 0.50-x)O 3 (x = 0.375, 0.45 and 0.50) were observed and investigated in details by transmission electron microscopy. The PLZST ceramics show exclusively incommensurate modulated structures (IMS) whose modulation period changed from 9.37 to 6.15 and to 4.04 with increasing of the x value. The hierarchical domain structures include, in decreasing scales, AFE domains, incommensurate domains and nanodomains. The elementary domains in PLZST ceramics are pinstriped nanodomains which were formed based on IMS configuration but by frequent modulation of IMS periodicity and formation of faults. Nanodomains accumulated and then dissociated into incommensurate domains and AFE domains successively. The presently revealed structural characteristics in antiferroelectric PLZST may stimulate future researches on the evolution of IMS-based hierarchical domains under external physical fields, e.g. thermal or electrical, and their correlation to the physical performance. [ABSTRACT FROM AUTHOR]

In this work, TiO 2 nanowire arrays embedded in PbZrO 3 -based antiferroelectric (AFE) films were fabricated on FTO/glass substrates using a facile two-step method. The energy storage performance was modulated by changing the density and morphology of TiO 2 nanowire arrays. A large recoverable energy density (W re) of 50.6 J/cm3 and efficiency (η) of 61% were achieved, which was attributed to the enhancement of maximum polarization and breakdown strength by constructing TiO 2 nanowire arrays in AFE films. More importantly, the composite films exhibited excellent thermal stability with the variation of energy storage density (<5%) and efficiency (<7%) in a wide temperature range (−120 to 130 °C) at the operating electric field of 1300 kV/cm. The results demonstrate that the composite films have huge potential in the future energy storage applications, whether in cold polar regions or high temperature regions. [ABSTRACT FROM AUTHOR]

Recently, the (Pb,La)(Zr,Ti)O 3 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 (Pb 0.895 La 0.07)(Zr x Ti 1- x)O 3 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 (W re) of 3.38 J/cm3 and ultrahigh energy efficiency (η) of 86.5% are achieved in (Pb 0.895 La 0.07)(Zr 0.9 Ti 0.1)O 3 ceramic. The (Pb 0.895 La 0.07)(Zr 0.9 Ti 0.1)O 3 ceramic also hold fairly thermal stability (relative variation of W re is less than 28% over 30 °C-120 °C), excellent frequency stability (10–1000 Hz) and good fatigue endurance. These results demonstrate that the (Pb 0.895 La 0.07)(Zr 0.9 Ti 0.1)O 3 ceramic can be a desirable material for dielectric energy storage capacitors, especially for pulse power technology. [ABSTRACT FROM AUTHOR]

• The composite ceramics Bi 0.5 Na 0.5 TiO 3 -Sm 2 Ti 2 O 7 were successfully prepared. • Excellent electrical properties and stability are obtained in BNT-STO ceramics. • A new effective method to design high ESP ceramic materials is proposed. The comprehensive performance of ferroelectric ceramic materials is a significant factor limiting the practical application. In this work, a novel strategy of constructing diphase compounds is proposed to significantly enhance the energy storage properties of Bi 0.5 Na 0.5 TiO 3 -based ceramics. A composite ceramic of pyrochlore phase Sm 2 Ti 2 O 7 modified perovskite phase Bi 0.5 Na 0.5 TiO 3 is successfully prepared and systematically studied. As the concentration of Sm 2 Ti 2 O 7 increases, the dielectric breakdown strength is greatly strengthened because of expanded band gap and shrunk grain size, and the relaxor behavior is enhanced due to the effect of linear character pyrochlore. As a result, the optimized composition demonstrates excellent energy storage properties including high recoverable energy storage density (W rec) of 6.387 J/cm3 at 402 kV/cm, superior stability of temperature (<6% variation in − 120 ∼ 120 °C), frequency (∼4% variation in 5 ∼ 500 Hz) and cycling (∼2% variation within 106 cycles). Besides, fast discharge behavior of t 0.9 ∼ 29.4 ns and high power density of 80.49 MW/cm3 at 200 kV/cm are also achieved. This study presents a novel strategy to enhance the performance of BNT-based materials through forming composite ceramic, which is anticipated to be a general method for other material systems as regards the design of advanced energy storage ceramics. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The composition dependent dielectric, ferroelectric and energy storage properties of tetragonal lead lanthanum zirconate stannate titanate (PLZST) antiferroelectric ceramics were systematically studied in this paper. Two sets of simple linear scaling relations were established for the forward switching field E AFE-FE , the backward switching field E FE-AFE and recoverable energy density W re . As Zr content increases (Ti fixed), E AFE-FE , E FE-AFE , W re decreases linearly, while the stored energy density W st declines first and then increases. In addition, decreasing Ti content (Zr fixed) leads to linear increments in all of E AFE-FE , E FE-AFE , W re and W st . These results not only reveal the superiority of PLZST with lower Zr and lower Ti contents for energy storage capacitors, but also provide a fast way to design PLZST ceramics with specific energy storage properties. Our work may also be very helpful for better understanding the mechanism of phase transition behaviors of antiferroelectric materials. [ABSTRACT FROM AUTHOR]

• The comprehensive optimization strategy of discharge curve can serve as the paradigm of conceptual materials. • A balance between W re = 5.92 J/cm3 and η = 81.7% is gotten in the BSZT-BMN-0.06 ceramic. • The mechanism of core–shell structure enhancing breakdown strength is clarified. • BSZT-BMN-0.06 ceramics owns a fast charge–discharge speed (44 ns) and a high P D of 144 MW/cm3. The conventional dielectric ceramics are extensively studied for applications in electronics and pulsed power systems owing to the advantages of high voltage and high power density. However, the inferior energy storage performance is difficult to satisfy the development requirements of integration and lightweight of power electronic devices. The main research efforts have been done to improve the energy storage density by enhancing the electric breakdown strength (BDS) or effective dielectric constant (ΔP/ΔE) due to the contradiction between ΔP/ΔE and BDS. Here, it is proposed to use composition design and microstructural core–shell engineering to surmount this contradiction and thus enhance the energy storage density. The heterogeneous microstructures are introduced through a two-step calcination, and the appearance of this microstructure is related to the destruction of the cooperative diffusion effect of multiple ions. Consequently, 0.93Ba 0.55 Sr 0.45- x Zn x TiO 3 -0.07BiMg 2/3 Nb 1/3 O 3 (BSZT-BMN- x) ceramics with core–shell microstructure prepared by traditional solid-state reaction method exhibits an ultrahigh recoverable energy density of 5.92 J/cm3, a superior energy storage efficiency of 81.7% and an outstanding charge–discharge performance (P D = 144 MW/cm3, t 0.9 = 44 ns). The experimental results and numerical simulations reveal that the doping of Zn2+ enhances the potential for off-centering of anions and cations, the core–shell microstructure makes the distribution of electric field to be regulated and the effective path of electric trees is extended to improve the BDS. The present research not only offers a novel paradigm for other material systems to further improve energy storage performance, but also should be generalizable for other functional materials for which a high BDS is required. [ABSTRACT FROM AUTHOR]