<p>In high-power pulse electronic devices and advanced energy-storage systems, antiferroelectric ceramics have attracted attention owing to their rapid charge–discharge capability and excellent cycling stability. However, their energy-storage performance is still limited by defect concentration and microstructural inhomogeneity, necessitating process optimization. In this work, Pb<sub>1−1.5x</sub>La<sub>x</sub> (Zr<sub>0.95</sub>Ti<sub>0.05</sub>) O<sub>3</sub> (x = 0.02) antiferroelectric ceramics were prepared via a sol–gel method, and the effects of post-annealing temperature (280–750&#xa0;°C) on their phase composition, microstructure, dielectric properties, and energy-storage characteristics were systematically investigated. XRD and SEM revealed that all samples retained a pure perovskite structure, while both grain size and crystallinity increased with annealing temperature. Dielectric and ferroelectric measurements demonstrated that moderate annealing (280&#xa0;°C) enhanced the dielectric constant, frequency stability, and reversibility of the electric-field-induced antiferroelectric–ferroelectric phase transition. The sample annealed at 280&#xa0;°C exhibited the highest recoverable energy density (<i>W</i><sub><i>rec</i></sub>) of 1.83&#xa0;J/cm<sup>3</sup> and efficiency (<i>η</i>) of 67.8% under an electric field of 165&#xa0;kV/cm, significantly outperforming samples processed at higher temperatures. Comprehensive impedance spectroscopy and activation energy analysis reveal that low-temperature annealing (280&#xa0;°C) effectively suppresses mobile oxygen vacancies while preserving beneficial defect-dipole complexes (e.g.,&#xa0;<i>V</i><sub><i>Pb</i></sub><i>’’-Vӧ</i>). This unique defect chemistry minimizes leakage current and promotes a slim, highly reversible polarization loop. This work provides a low-cost post-processing defect engineering strategy for high-performance PLZT antiferroelectric capacitors.</p>

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Enhanced energy-storage performance of PLZT antiferroelectric ceramics via optimizing the annealing temperature

  • Shubao Yang,
  • Jianghai Wang,
  • Weihao Wu,
  • Yulin Zhang,
  • Haowen Mu,
  • Rongli Gao,
  • Xiaoling Deng,
  • Wei Cai,
  • Chunlin Fu

摘要

In high-power pulse electronic devices and advanced energy-storage systems, antiferroelectric ceramics have attracted attention owing to their rapid charge–discharge capability and excellent cycling stability. However, their energy-storage performance is still limited by defect concentration and microstructural inhomogeneity, necessitating process optimization. In this work, Pb1−1.5xLax (Zr0.95Ti0.05) O3 (x = 0.02) antiferroelectric ceramics were prepared via a sol–gel method, and the effects of post-annealing temperature (280–750 °C) on their phase composition, microstructure, dielectric properties, and energy-storage characteristics were systematically investigated. XRD and SEM revealed that all samples retained a pure perovskite structure, while both grain size and crystallinity increased with annealing temperature. Dielectric and ferroelectric measurements demonstrated that moderate annealing (280 °C) enhanced the dielectric constant, frequency stability, and reversibility of the electric-field-induced antiferroelectric–ferroelectric phase transition. The sample annealed at 280 °C exhibited the highest recoverable energy density (Wrec) of 1.83 J/cm3 and efficiency (η) of 67.8% under an electric field of 165 kV/cm, significantly outperforming samples processed at higher temperatures. Comprehensive impedance spectroscopy and activation energy analysis reveal that low-temperature annealing (280 °C) effectively suppresses mobile oxygen vacancies while preserving beneficial defect-dipole complexes (e.g., VPb’’-Vӧ). This unique defect chemistry minimizes leakage current and promotes a slim, highly reversible polarization loop. This work provides a low-cost post-processing defect engineering strategy for high-performance PLZT antiferroelectric capacitors.