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Antiferroelectric thin films have attracted blooming interest due to their potential application in energy storage areas. Pb(1−3x/2)LaxHfO3 (PLHO-x, x = 0–0.05) thin films were fabricated on Pt(111)/TiO2/SiO2/Si substrates via the chemical solution deposition method. The x-ray diffraction and high-resolution transmission electron microscopy results show that the doping of La3+, which has a smaller ion radius, leads to a slight decrease in the lattice constant and unit cell volume, which can induce the lattice distortion. In addition, the dielectric and polarization properties indicate that with an increase in the temperature or La3+ content, the antiferroelectric (AFE) I phase can transform into an AFE II phase, exhibiting a slimmer P–E loop with enhanced switching field and more pronounced polarization dispersion. Notably, PLHO-0.04 showcases excellent energy storage performance (55 J/cm3, at 2.8 MV/cm). This material also exhibits good thermal, frequency, and fatigue stability. These results suggest that the energy storage performance of PbHfO3-based films can be enhanced through the phase structure design, presenting a valuable approach to fulfill the growing demand for advanced energy storage devices. [ABSTRACT FROM AUTHOR]

Dielectric ceramic capacitors with ultrahigh power densities are fundamental to modern electrical devices. Nonetheless, the poor energy density confined to the low breakdown strength is a long-standing bottleneck in developing desirable dielectric materials for practical applications. In this instance, we present a high-entropy tungsten bronze-type relaxor ferroelectric achieved through an equimolar-ratio element design, which realizes a giant recoverable energy density of 11.0 J·cm−3 and a high efficiency of 81.9%. Moreover, the atomic-scale microstructural study confirms that the excellent comprehensive energy storage performance is attributed to the increased atomic-scale compositional heterogeneity from high configuration entropy, which modulates the relaxor features as well as induces lattice distortion, resulting in reduced polarization hysteresis and enhanced breakdown endurance. This study provides evidence that developing high-entropy relaxor ferroelectric material via equimolar-ratio element design is an effective strategy for achieving ultrahigh energy storage characteristics. Our results also uncover the immense potential of tetragonal tungsten bronze-type materials for advanced energy storage applications. The authors present an equimolar-ratio element high-entropy strategy for designing high-performance dielectric ceramics and uncover the immense potential of tetragonal tungsten bronze-type materials for advanced energy storage applications. [ABSTRACT FROM AUTHOR]

PbZrO3 has been broadly considered as a prototypical antiferroelectric material for high-power energy storage. A recent theoretical study suggests that the ground state of PbZrO3 is threefold-modulated ferrielectric, which challenges the generally accepted antiferroelectric configuration. However, such a novel ferrielectric phase was predicted only to be accessible at low temperatures. Here, we successfully achieve the room-temperature construction of the strongly competing ferrielectric and antiferroelectric state by strain-mediated phase separation in PbZrO3/SrTiO3 thin film. We demonstrate that the phase separation occurs spontaneously in quasi-periodic stripe-like patterns under a compressive misfit strain and can be tailored by varying the film thickness. The ferrielectric phase strikingly exhibitsa threefold modulation period with a nearly up-up-down configuration, which could be stabilized and manipulated by the formation and evolution of interfacial defects under applied strain. The present results construct a fertile ground for further exploring the physical properties and applications based on the novel ferrielectric phase. There is a desire to know how the threefold ferrielectric coexists with the antiferroelectric phase. Here, the authors realize a threefold-modulated ferrielectric phase regulated by strain-mediated phase separation in PbZrO3 thin film. [ABSTRACT FROM AUTHOR]

With the gradual promotion of new energy technologies, there is a growing demand for capacitors with high energy storage density, high operating temperature, high operating voltage, and good temperature stability. In recent years, researchers have been devoted to improving the energy storage properties of lead‐based, titanium‐based, and iron‐based multilayer ceramic capacitors (MLCCs). However, limited research has been conducted into MLCC development using NaNbO3 (NN)‐based materials. In this paper, the successful achievement of excellent overall energy storage performance in a novel NaNbO3–(Bi0.5Na0.5)TiO3–Bi(Mg0.5Hf0.5)O3 lead‐free MLCCs is presented. The disordered tilting around the cp axis, disrupts Na and Bi ions' long‐range displacements and induces PNRs and strong relaxor behavior, which ensures a superior energy storage performance, together with the multilayer ceramic design strategy. As a result, the NN‐based MLCC device presents an ultra‐high Wrec = 12.65 J cm−3 and η = 88.5%, simultaneously showing superior temperature stability (Wrec varies <±1% and η varies <±6% from −50 to 125 °C) and fatigue resistance (Wrec and η vary <±1% over 107 cycles). This study highlights the advanced energy storage potential of NaNbO3‐based MLCCs for various applications, and ushers in a new era for designing high‐performance lead‐free capacitors that can operate in harsh environments. [ABSTRACT FROM AUTHOR]

High polarization of ferroelectric materials has profound research significance and is the decisive factor in the application of energy storage, pyroelectricity, and explosive energy conversion. Herein, in force-electric conversion field, an ultrahigh remanent polarization (51.43 μC/cm2) and record-breaking energy density (4.59 J/cm3) after poling were achieved with a lead-free (1 − x)Bi0.5Na0.5TiO3 − xAgNbO3 [(1 − x)BNT – xAN] relaxor ceramics. The enhancement effect of AgNbO3 on polarization is attributed to the increase in lattice distortion and orientation after poling. Additionally, a significant force-electric conversion effect under hydrostatic pressure (depolarization rate ∼44.8%, 400 MPa) and shock pressure (depolarization rate ∼54.4%, 6.3 GPa) in (1 − x)BNT – xAN was attributed to the pressure-driven ferroelectric/relaxor (FE/RE) phase transition. This work is expected to enlighten the further design of ferroelectric materials with high polarization for pulse power energy conversion application. [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]

This correction notice is for an article titled "High-entropy relaxor ferroelectric ceramics for ultrahigh energy storage" published in Nature Communications. The notice addresses two errors in the original article. The first error is in the first paragraph of page 4, where 'Tm,1MHz-Tm,10Hz' was incorrectly written. The correct version should state 'Tm,1MHz-Tm,10Hz'. The second error is in the first paragraph of page 7, where '(S1, S1)' was incorrectly written. The correct version should state '(Fig. S15)'. The correction has been made in both the PDF and HTML versions of the article. The authors of the article are Haonan Peng, Tiantian Wu, Zhen Liu, Zhengqian Fu, Dong Wang, Yanshuang Hao, Fangfang Xu, Genshui Wang, and Junhao Chu. [Extracted from the article]

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]

The phase boundaries of dielectric materials have constantly been valuable for instructing the design of phase structures, revealing correlations between compositions and structures, and attaining the desired functional properties for piezoelectric, pyroelectric, electrostriction, electrocaloric, energy storage and energy harvesting applications. We here observe a new type of phase boundary in a solid solution of xPbTiO3·(1 − x)Pb(Yb1/2Nb1/2)O3 (x = 0.00–0.20), which is between an antiferroelectric (AFE) phase and a relaxor ferroelectric (RFE) phase. x = 0.10 is confirmed as the phase boundary. XRD, TEM, PFM and Raman spectroscopy analysis reveal two fundamental traits of the phase structure: (1) the polar state changes from AFE to FE order; and (2) the domain range evolves from micrometer-sized to nanometer-sized, both of which are normally separated but coexist around the phase boundary. The intriguing phase structure contributes to the distinctive dielectric properties: (1) a broad compositional zone (x < 0.10 and x ≥ 0.14) features low remnant polarization, low hysteresis and highly reversible domain wall motion, and is expected to be utilized for dielectric energy storage and electrostriction applications; and (2) a narrow nonergodic RFE zone (0.10 ≤ x < 0.14) demonstrates remnant and maximum polarization, co-dominated by composition and temperature, and has potential for pyroelectric and electrocaloric applications. [ABSTRACT FROM AUTHOR]

Recently, dielectrics for energy storage have been attracting increasing attention due to their ultrahigh power density. However, the widespread application of dielectrics remains limited by their low energy density. In this work, lead-free single-phase relaxor (1 − x)Ba0.55Sr0.45TiO3-xBiMg2/3Nb1/3O3 [(1 − x)BST-xBMN] (x = 0, 0.05, 0.07, and 0.10) bulk ceramics were prepared by a conventional solid-state reaction process. The dielectric properties, the relaxor behavior, and the energy storage properties were explored in detail. With increasing BMN content, the observed increase in activation energy (Ea) and the decrease in freezing temperature (Tf) indicate that the coupling between polar nano-regions (PNRs) gradually weakened, leading to the decrease in remanent polarization (Pr) and the increase in energy storage efficiency (η). For the composition x = 0.07, the breakdown strength (BDS) significantly increased from 240 kV cm of pure BST to 450 kV cm. Finally, large Wrec (4.55 J cm3) and high η (81.8%) were achieved in 0.93BST-0.07BMN ceramics. The results demonstrate that the (1 − x)BST-xBMN ceramics have superior potential for use in advanced pulsed power capacitors. [ABSTRACT FROM AUTHOR]

Abstract: Energy storage materials and their applications have long been areas of intense research interest for both the academic and industry communities. Dielectric capacitors using antiferroelectric materials are capable of displaying higher energy densities as well as higher power/charge release densities by comparison with their ferroelectric and linear dielectric counterparts and therefore have greater potential for practical energy storage applications. Over the past decade, extensive efforts have been devoted to the development of high performance, antiferroelectric, energy storage ceramics and much progress has been achieved. In this review, the current state‐of‐the‐art as regards antiferroelectric ceramic systems, including PbZrO3‐based, AgNbO3‐based, and (Bi,Na)TiO3‐based systems, are comprehensively summarized with regards to their energy storage performance. Strategies are then discussed for the further improvement of the energy storage properties of these antiferroelectric ceramic systems. This is followed by a review of the low temperature sintering techniques and the charge–discharge performance of antiferroelectric ceramics from a practical point of view. The review will be of benefit for researchers in the area as it offers a quick overview of recent progress in the development of various kinds of antiferroelectric ceramics and their properties. It should also stimulate the development of novel antiferroelectric ceramics with high energy storage performance. [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]

Polarization switching and energy storage properties of highly (100) oriented antiferroelectric (AFE) (Pb,La)(Zr,Ti)O3 thin films (≤250 nm) deposited via a sol-gel process with both LaNiO3 and Pt top electrodes were investigated. By using LaNiO3 top electrodes, the energy density as well as energy efficiency can be enhanced by 4.6 J/cm3 and 11%, respectively. Furthermore, the films with LaNiO3 top electrodes are more capable of providing high energy density over a wide temperature regime above room temperature compared to Pt. This work clearly highlights that oxide top electrodes can greatly improve the energy storage performance of antiferroelectric thin film capacitors. [ABSTRACT FROM AUTHOR]

Energy-storage properties of 0.89 Bi0.5Na0.5TiO3-0.06 BaTiO3-0.05 K0.5Na0.5NbO3 (0.89 BNT-0.06 BT-0.05 KNN) lead-free ceramics were first investigated. Measurements of dielectric properties together with switching current curves indicate a rather diffuse ferroelectric ( FE) to anti-ferroelectric ( AFE) phase transition when heating from 20°C to 90°C. The energy density ( W), which was calculated from P-E hysteresis loops, increases linearly with the external electric field when E exceeds AFE- FE transition field. W is independent of temperature and frequency, and maintains around 0.59 J/cm3 under 5.6 kV/mm in the stable AFE phase region. These properties indicate that 0.89 BNT-0.06 BT-0.05 KNN ceramics might be a promising lead-free AFE material for energy-storage capacitor application. [ABSTRACT FROM AUTHOR]

Energy storage capacitors for advanced pulse power systems and high-power electric devices is a kind of important electronic components, the demand continues to grow, specifications are constantly being upgraded, and performance boundaries are continuously being pushed. Multilayer ceramic capacitors (MLCCs) for energy storage applications have received increasing attention due to the advantages of ultralow equivalent series inductance, equivalent series resistance, good frequency characteristics, strong voltage overload ability, and stable operability at high temperatures. However, the relatively low energy storage density significantly limits its broader applications. Here, 0.4Ba 0.55 Sr 0.45 TiO 3 -0.4Bi 0.5 Na 0.5 TiO 3 -0.2SrZrO 3 (0.4BST-0.4BNT-0.2SZ) relaxor ferroelectric MLCCs are prepared at different heating rates. Excellent recoverable energy storage density of 10.3 J cm−3 and high energy efficiency of 93 % are achieved in fast-fired MLCCs under the electric field of 106.3 V μm−1. The impedance spectroscopy and thermally stimulated depolarization current technologies are employed to investigate the conductance mechanism of MLCCs, and the results can explain the effect of heating rate on the performance of MLCCs. In addition, the charge-discharge performances of fast-fired MLCCs are also thoroughly investigated, exhibiting great thermal and fatigue stability. [ABSTRACT FROM AUTHOR]

The (0.9−x) Bi0.5Na0.5TiO3-xBaTiO3-0.1K0.5Na0.5NbO3 [ BNBKN(x), x = 0.060, 0.063, 0.066, and 0.069] ceramics were fabricated by the conventional sintering technique. The P- E hysteresis loops measured under 5 kV/mm at room temperature show that the BNBKN(0.063) ceramics obtain the maximum ( Ps− Pr) value of 20.6 μC/cm2 and the largest energy-storage density W of 0.424 J/cm3. In addition, calculation from the X-ray diffraction results shows that the BNBKN(0.063) ceramics are featured with the largest c/ a ratio of 0.70887. The W is observed to increase with the increase of the c/ a ratio in the BNBKN( x) ceramics. The c/ a ratio can be regarded as a significant factor for W in the BNBKN( x) ceramics. [ABSTRACT FROM AUTHOR]

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 effect of residual stress on energy storage property was investigated for a series of PbZrO3 thin films on SrTiO3 and Si substrates. Compressive or tensile residual stress influences the critical electric field EA for the ferroelectric-to-antiferroelectric phase transition, thus for films with (110)/(101) orientation, energy density W of films on SrTiO3 is 38% larger than films on Si; in contrast, (001)-oriented PbZrO3 films on SrTiO3 show slightly smaller W compared to films on Si. We conclude that the different responses of W to stress are related to the different constrain states in films with different orientations. [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]

Pulse ceramic capacitors that request particularly high reliability and long lifetime forbid over-applied electric field, hence demanding high energy density (W re) and energy storage efficiency (η) at low electric field. In this work, we investigated a lead lanthanum zirconate titanate (PLZT) ceramic featuring both of tetragonal antiferroelectric phase (AFE T) and relaxor characteristic, which emerge in converged area of PLZT phase diagram (mole ratio of La reaches ~10%). Temperature dependent permittivity and XRD analysis proves the crossover trait in this structure. In this special relaxor-like AFE T structure, decent W re (1.2–1.3 J cm−3) and η (86–90%) are achieved at 12 V μ m−1. Equivalent dielectric constant (ε eq) is also introduced to illustrate nonlinear energy storage performance at different electric field. Compared to common dielectric materials, tunable ε eq in relaxor-like AFE T structure shows advantages of excellent low-field energy density and wide working span, leading to the convenience in size design of capacitors. Finally, good energy storage stability under various external field was verified: ~1.00 J cm−3 in W re and ~92% in η were stabilized under varied frequency (< ± 8.9%, 0.01–2000 Hz), temperature (< ± 9.8%, −60 to 120 ℃) and fatigue loading (< ± 9.8%, >108 times) at ~10 V μ m−1. [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]

(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]

In this work, Pb 1−3 x /2 La x ZrO 3 (x = 0–0.12) (PLZ- x) antiferroelectric thin films were fabricated on Pt(111)/TiO 2 /SiO 2 /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 (W re) 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 W re (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 PbZrO 3 films with high energy storage density, high efficiency and excellent cycling stability can be considered as potential candidates for energy storage applications. [ABSTRACT FROM AUTHOR]

Antiferroelectrics (AFE) are considered a promising energy storage material for components that require nanosecond-level discharge. Pb(Yb 1/2 Nb 1/2)O 3 (PYN) is an AFE material with potential energy storage applications. However, the unmatched critical phase transition field (E F) and breakdown electric field (E B) conceal most of energy storage capacitance. This work is aimed to settle imbalanced E F / E B via a compositional design strategy. E F and E B were tuned in order to obtain 5.18 J cm−3 in recoverable energy density, 65% energy efficiency, and thermal and frequency stability varying within 15%, producing excellent comprehensive energy storage properties. A modified kinetic model of energetic path was used to understand the mechanism governing the variation of E F. We expect our work to contribute to further development of novel AFE materials for energy storage. [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]

• a way of external pressure to enhance energy storage properties of AgNbO 3 ceramics. • An η of 56% and W rec of 1.3 J/cm3 has been achieved in AgNbO 3 ceramics under 400 MPa. • Hydrostatic pressure results in an enhancement in η and W rec by 47% and 23%, respectively. Despite its low energy storage efficiency (∼46%), silver niobate (AgNbO 3) is considered as a promising lead-free antiferroelectric material due to its environmental advantages. Herein, we demonstrate that the energy storage efficiency of AgNbO 3 ceramics can be enhanced by applying hydrostatic pressure. The results reveal that the hydrostatic pressure contributed to the decline of remanent polarization (P r) and the switching hysteresis Δ E. In addition, the externally applied pressure improved the reverse switching field (E A). This indicates an enhanced antiferroelectricity, benefiting the enhancement of energy storage properties of AgNbO 3 ceramics. Under the pressure of 400 MPa, the as-prepared AgNbO 3 ceramics exhibited an energy storage efficiency (η) of 56% and a recoverable energy storage density (W rec) of 1.3 J/cm3 under the electric field of 13 kV/mm, corresponding to an enhancement of 47% and 30%, respectively. [ABSTRACT FROM AUTHOR]

In this work, high performance (Pb 0.97 La 0.02 )(Zr 0.66 Sn 0.23 Ti 0.11 )O 3 polycrystalline antiferroelectric thin-film was successfully fabricated on (La 0.7 Sr 0.3 )MnO 3 /Al 2 O 3 (0001) substrate via a cost-effectively chemical solution method. A large recoverable energy storage density ( W re ) of 46.3 J/cm 3 and high efficiency ( η ) of 84% were realized simultaneously under an electric field of 4 MV/cm by taking full advantage of the linear dielectric response after the electric field induced antiferroelectric-ferroelectric transition. Moreover, the PLZST thin-film displayed high temperature stability. With increasing temperature from 300 K to 380 K, the W re decreased only 1.3%. The film also exhibited good fatigue endurance up to 1 × 10 5 cycling under an electric field of 2.2 MV/cm. Our work underlines the importance of the interface quality between the film and the substrate and the important role of linear dielectric answer after saturation in the improvement of the energy storage density and efficiency of antiferroelectric materials. [ABSTRACT FROM AUTHOR]

Antiferroelectric Pb 0.97 La 0.02 (Zr 0.33 Sn 0.55 Ti 0.12 )O 3 @SiO 2 (with 5% mole of SiO 2 ) particles were synthesized by a citric acid sol-gel method. Transmission electron microscopy(TEM) results illustrated the formation of core–shell nanostructures with controllable shell thicknesses about 3–5 nm. X-ray diffraction(XRD) patterns displayed that a stable perovskite phase was preserved and no other crystallization peaks were discovered from the shell component. Scanning electron microscopy(SEM) and Energy Dispersive Spectrometer(EDS) investigations confirmed that core-shell structures were inherited from particles to ceramics after sintering. As a result, through the coating process, the breakdown strength of the ceramic increases by 95% from 12.2 kV/mm to 23.8 kV/mm and the recoverable energy density was greatly enhanced from 1.76 J/cm 3 to 2.68 J/cm 3 . These results demonstrate a promising reaction method to enhance breakdown strength in antiferroelectrics for energy storage capacitor applications. [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]

Lead-free antiferroelectric materials can be used in environmental-friendly energy applications and are receiving tremendous attention owing to their high energy-storage density, which is achieved through a phase transition between antiferroelectric and ferroelectric state. Here, by slowing down the antiferroelectric-ferroelectric transition via controllable beam irradiation in a transmission electron microscope, we demonstrate that such a transition in NaNbO 3 undergoes by means of forming a buffer-area (about 40–150 nm wide) at the on-going transition front. The spatial buffer-area approximately maintains its shape during moving and are characterized to be the antiferroelectric phase but exhibits a gradual variation of lattice spacing along the [010] proceeding direction of phase transition. With help of such buffer-area, the overall stress or barrier between the two phases could be considerably reduced compared to the direct change between the two structures. Therefore, our findings provide new insights for understanding the dynamical energy-storage process in antiferroelectric materials. [Display omitted] [ABSTRACT FROM AUTHOR]

Highly (001)-oriented pure PbZrO 3 (PZO) films and Sn-substituted PZO films are deposited on (001)-LaNiO 3 buffered SiO 2 /Si substrates by RF magnetron sputtering. Different Sn-substituted PbZrO 3 films (PbZr 1-x Sn x O 3 , x = 0%, 3%, 5%, 10%) with orthorhombic anti-ferroelectric phase are fabricated. The effects of Sn substitution on structure and energy performance have been investigated in detail. The switching electric fields are enlarged and energy loss is lowered by Sn substitution. Recoverable energy density (Wr) of 14.8 ± 0.2 J/cm 3 and energy efficiency (η) of 71.2 ± 0.5% at 900 kV/cm are obtained in 5% Sn-substituted PZO film (~ 360 nm). Furthermore, with thicker thickness of ~ 650 nm, Wr and η can be further improved. The Sn-substituted PZO film is believed to be an improved material for applications in energy storage systems and 5% Sn-substituted PZO film exhibits the highest Wr and η in this work. [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]

[Display omitted] • The superior energy storage properties of Pb 0.925 La 0.05 Zr 1- x Ti x O 3 antiferroelectric thin films in Zr rich were obtained. • In Zr-rich region, the saturation polarization strengthens of PLZT with increasing Ti content due to change of ion-radius, and the switching field decreased which means the enhancement of ferroelectricity. • The co-doped PLZT films possessed higher breakdown strength, which greatly optimized the energy storage properties. • The high recoverable energy density of 49.7 J/cm3 and efficiency of 54% were obtained in the Pb 0.925 La 0.05 Zr 0.985 Ti 0.015 O 3 film. Pb 0.925 La 0.05 Zr 1- x Ti x O 3 (PLZT, x = 0.5%∼5.5%) thin film were fabricated on Pt(1 1 1)/TiO 2 /SiO 2 /Si substrates by sol–gel method. In the Zr-rich region, the saturation polarization strengthens with increasing Ti content due to the change of ion-radius. On the other hand, the switching field decreases, which means the enhancement of ferroelectricity. The phase structure and polarization of the films can be tuned by a small amount of Ti doping, and then the energy storage characteristics of the thin films can be modulated. The results showed that a large energy storage density (W rec) of 49.7 J/cm3 and efficiency (η) of 54% were achieved in the x = 1.5%. Moreover, the x = 1.5% sample displayed excellent cycling stability up to 1 × 106 cyclings, which demonstrated that La and Ti co-doped films can be considered as potential candidates for future energy storage devices. [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]

• Obtained the PLZST ceramics with "slanted" shape of P-E loops by modifying Sn content. • Obtained a high recoverable energy density of 1.42 J/cm3 and high η of 90% in PLZST30/60/10. • Better understanding of the mechanism on energy storage properties of PLZST ceramics. Both high energy density and high energy efficiency are indispensable as considering antiferroelectric materials for pulse power capacitor applications. However, the electrical hysteresis will inevitably limit the energy efficiency reported in previous literatures. In this work, lead lanthanum zirconate stannate titanate (PLZST) antiferroelectrics with both high energy density and high energy efficiency was presented. It is found that PLZST antiferroelectric ceramics with high Sn content not only exhibit enhanced antiferroelectricity, but also demonstrate higher energy efficiency. As Sn content increases, grain size decreases and the electric hysteresis values reduces. The high energy density of 1.28 J/cm3 and ultrahigh energy efficiency of 91% was obtained for PLZST30/60/10. The results will not only enrich our understanding of PLZST antiferroelectric materials but also offers new approach to developing high performance antiferroelectric for energy storage based applications. [ABSTRACT FROM AUTHOR]