<p>Post-treatment annealing is a critical strategy for modulating the defect structure and electrical performance of dielectric capacitors; however, the competitive mechanisms between stress relief and defect evolution during low-temperature annealing remain unclear. In this study, dense (Pb, La) (Zr, Ti) O<sub>3</sub> (PLZT) antiferroelectric ceramics were fabricated via a sol–gel route combined with a two-step sintering regime, followed by systematic post-annealing at 280&#xa0;°C for varying durations (30&#xa0;min–2&#xa0;h). Complex impedance spectroscopy revealed that the conduction activation energy remained stable at approximately 0.36–0.38&#xa0;eV regardless of the annealing time, indicating that the dominant conduction mechanism and migration barrier are governed primarily by the thermal history rather than the low-temperature treatment. Despite the constant defect concentration, the ferroelectric polarization exhibited a strong dependence on the annealing duration. Short-term annealing (30&#xa0;min) effectively relieved residual internal stresses, yielding a high maximum polarization of 26.18 μC/cm<sup>2</sup>. Conversely, prolonged annealing (2&#xa0;h) induces surface morphological degradation and severe domain wall clamping, which drastically suppressed the switchable polarization. Consequently, the optimized ceramic achieved a recoverable energy storage density of 1.65&#xa0;J/cm<sup>3</sup> at elevated temperatures, accompanied by exceptional frequency stability. These findings explicitly clarify that performance variations during low-temperature annealing are driven by microstructural-induced domain pinning rather than bulk defect fluctuations, providing distinct guidance for processing high-performance energy storage ceramics.</p>

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Optimizing energy storage in PLZT antiferroelectric ceramics via low-temperature post-annealing: stress relief vs. domain clamping

  • Shubao Yang,
  • Jianghai Wang,
  • Zhongxiang Zheng,
  • Yulin Zhang,
  • Weihao Wu,
  • Rongli Gao,
  • Xiaoling Deng,
  • Wei Cai,
  • Chunlin Fu,
  • Junming Li

摘要

Post-treatment annealing is a critical strategy for modulating the defect structure and electrical performance of dielectric capacitors; however, the competitive mechanisms between stress relief and defect evolution during low-temperature annealing remain unclear. In this study, dense (Pb, La) (Zr, Ti) O3 (PLZT) antiferroelectric ceramics were fabricated via a sol–gel route combined with a two-step sintering regime, followed by systematic post-annealing at 280 °C for varying durations (30 min–2 h). Complex impedance spectroscopy revealed that the conduction activation energy remained stable at approximately 0.36–0.38 eV regardless of the annealing time, indicating that the dominant conduction mechanism and migration barrier are governed primarily by the thermal history rather than the low-temperature treatment. Despite the constant defect concentration, the ferroelectric polarization exhibited a strong dependence on the annealing duration. Short-term annealing (30 min) effectively relieved residual internal stresses, yielding a high maximum polarization of 26.18 μC/cm2. Conversely, prolonged annealing (2 h) induces surface morphological degradation and severe domain wall clamping, which drastically suppressed the switchable polarization. Consequently, the optimized ceramic achieved a recoverable energy storage density of 1.65 J/cm3 at elevated temperatures, accompanied by exceptional frequency stability. These findings explicitly clarify that performance variations during low-temperature annealing are driven by microstructural-induced domain pinning rather than bulk defect fluctuations, providing distinct guidance for processing high-performance energy storage ceramics.