Superb energy density of PbHfO3-based antiferroelectric ceramics via regulating the antiferroelectric–ferroelectric transition energy barrier

Abstract

Antiferroelectric (AFE) ceramics are excellent candidates for developing capacitors with enhanced energy storage capabilities due to their unique field-induced phase transitions. Research showed that AFE materials with large energy barriers typically exhibit better AFE stability. However, the higher intrinsic potential barriers make it difficult for the polar phase to cross the barrier after the electric field is removed, significantly reducing the maximum polarization (P_max). Herein, we propose a universal approach to introducing mutually exclusive interaction ions at both the A-site and B-site to regulate the AFE-FE transition energy barrier in PbHfO₃-based ceramics to markedly enhance capacitive performance. By precisely tuning the position of the AFE and FE states in the energy paths, we achieve a large phase-switching field (∼509 kV cm⁻¹) and a high P_max (∼47.07 μC cm⁻²), accompanied by an ultrahigh recoverable energy storage density (∼16.05 J cm⁻³). In terms of practical applications, the ceramics display commendable frequency and cycling stability, as well as a rapid discharge time of 106 ns and a high-power density of 193.5 MW cm⁻³. This work presents an innovative strategy for synergistically enhancing the energy storage performance of AFE ceramics, potentially advancing the development of advanced dielectric capacitors.