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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]

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]

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]

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]

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]

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]

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]

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]

• 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]

Abstract Bulk ceramics with high recoverable energy density (W re) and energy efficiency (η) play a critical role in the development of pulsed power systems for miniaturization and lightweight. The orthorhombic phase (Pb,La)(Zr,Ti)O 3 -based antiferroelectric (AFE) ceramics have been regarded as one of the most promising candidates for pulsed power system applications due to their relatively high energy storage density and efficiency. However, the main drawback of orthorhombic phase (Pb,La)(Zr,Ti)O 3 -based AFE ceramics is relatively low dielectric breakdown strengthen (DBS), which has always restricted the improvement of energy storage density. In this study, an effectively method to increase DBS by the introduction of Mn has been proposed. The relative density of orthorhombic phase (Pb 0.91 La 0.06)(Zr 0.96 Ti 0.04)O 3 (PLZT) ceramics was improved by Mn-doping. And the introduction of Mn can decrease the tolerance factor (t) of PLZT ceramics because the radius of Mn2+ is larger than that of B-site Zr4+/Ti4+, and thus enhancing antiferroelectricity. Meanwhile, the effects of Mn-doping on the phase structure, microstructure and dielectric properties of PLZT ceramics have been studied thoroughly in this study. It is found that the highest W re of 7.65 J/cm3 is obtained at 1.0 mol% Mn-doped PLZT ceramic, which is obviously larger than that of undoped PLZT ceramic (5.71 J/cm3). These results suggest that the Mn-doped PLZT ceramics are potential energy storage materials in pulsed power systems. Highlights • Enhanced the dielectric breakdown strengthen of pure antiferroelectric ceramics by Mn-doping. • Obtained a high recoverable energy density of 7.65 J/cm3 and relatively high η of 87% in Mn-doped antiferroelectric ceramics. • Better understanding of the mechanism on energy storage properties of Mn-doped antiferroelectric ceramics. [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]

PZT95/5 ferroelectric ceramics are widely utilized in pulsed power devices and the remanent polarization Pr of poled PZT95/5 can characterize the shock-driven energy density. However, this remanent polarization is difficult to be measured nondestructively. In this article, a series of pyroelectric tests of poled PZT95/5 ceramics were conducted near room temperature, from 25°C to 20°C. A linear relation between Pr and pyroelectric coefficient p was found, that is, Pr=1190.5( K)× p, which provides an effective way to nondestructively estimate the value of Pr of the poled PZT95/5 ceramics by measuring the pyroelectric coefficient p at room temperature. According to Devonshire's phenomenological theory, this result could be explained by a modified equation: [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]