Achieving Excellent Energy Storage and Discharge Performance in PbHfO₃-Based Antiferroelectric Ceramics via Optimization of Parameters

Antiferroelectric (AFE) materials demonstrate potential application in pulse power systems and energy-storage devices due to outstanding power density (<i>P</i>_D) and rapid charge-discharge capability. Simultaneously achieving a high discharge energy density (<i>W</i>_dis) and large energy-storage density in AFE ceramics remains a key research focus. In this work, a method for optimizing parameters is proposed for ameliorating the grain size of the ceramic and enhancing antiferroelectricity, ultimately enhancing the energy-storage density and breakdown strength (<i>E</i>_b). Therefore, an excellent recoverable energy density (<i>W</i>_rec) of 13.6 J/cm³ and a large energy efficiency (η) of 82% along with outstanding thermal and frequency stabilities are simultaneously achieved in (Pb_0.96La_0.02Ca_0.02)(Hf_0.9Sn_0.1)O₃ (C1) AFE ceramics at a maximum electric field. The multistage field-induced phase transition phenomenon is detected at the polarization-electric field (<i>P</i>-<i>E</i>) hysteresis loop of the C1 ceramic. Meanwhile, a superior <i>P</i>_D of 314.6 MW/cm³ and an excellent <i>W</i>_dis of 9.05 J/cm³ as well as a rapid discharge time (84 ns) are also obtained in the C1 ceramic at 380 kV/cm. The results highlight the potential of (Pb_{0.98-<i>x</i>}La_0.02Ca_<i>x</i>)(Hf_0.9Sn_0.1)O₃ AFE ceramics for pulsed power systems and energy-storage applications.