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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]

(Pb,La)(Zr,Ti)O3 antiferroelectric (AFE) ceramics have attracted considerable interest due to their high‐energy storage density and numerous field‐induced phase transitions. However, the positional equilibrium of the A‐site and B‐site is typically maintained without considering that heterovalent doping of La3+ can induce defects within the material, leading to high‐temperature leakage conduction. In this work, we introduced the acceptor ion Na+ at the A‐site simultaneously and designed Pb0.9175–0.5xLa0.055NaxZr0.975Ti0.025O3 (x = 0.01, 0.03, 0.055, 0.07, 0.10) AFE ceramics. The dielectric properties of these ceramics exhibited a consistent pattern of improvement followed by deterioration as the content of Na+ increased. Notably, when x = 0.055 (Na5.5), the AFE ceramic demonstrated superior high‐temperature frequency stability with negligible leakage conduction. Impedance spectroscopy analysis suggested that Na5.5 displays the greatest resistance and highest Edc. Concurrently, the thermally stimulated depolarization current indicates that Na5.5 possesses the lowest defect concentration and the largest Ea. This can be attributed to the internal generation of defect dipole clusters (VPb′′−VO••−NaPb′−LaPb•$V_{{\mathrm{Pb}}}^{{\prime\prime}} - V_{\mathrm{O}}^{ \bullet \bullet } - {\mathrm{Na}}_{{\mathrm{Pb}}}^{\prime} - {\mathrm{La}}_{{\mathrm{Pb}}}^ \bullet $), which effectively restrict the movement of charged defects. These findings suggest that Na5.5 holds significant potential for application and offer insights into the understanding of internal defects in lead‐based AFE materials. [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]

• 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]