Dielectric energy storage has gained considerable significance owing to the high energy requirements of human society. Lead zirconate-based (PZ) antiferroelectric materials have received much attention due to their fast discharge rate, high power density, and low cost. Nevertheless, their low energy storage density seriously limits their practical applications. To overcome this limitation, the phase modulation strategy via chemical modification was adopted to optimize the breakdown strength and phase switching field. Specifically, the antiferroelectric ceramics of (Pb0.97−xGd0.02Srx)(Zr0.87Sn0.12Ti0.01)O3 were prepared by the tape-casting method. An apparent multistage phase transition behavior revealed for x ≥ 0.05 is rarely discussed in reported Sr2+ modified PZ system. This is attributed to the coexistence of the main orthorhombic phase and the tetragonal phase. Although the transition near the lower field reduces the energy storage slightly, the disruption of the long-range order stabilizes the antiferroelectricity of the orthorhombic phase, hence elevating its transition field. In addition, the tetragonal phase with lower polarization suppresses the electrostrain thus improving the breakdown strength. Consequently, an ultrahigh recoverable energy storage density of 14.5 J/cm3 with a high energy efficiency of 81 % is achieved at a high electric field of 717 kV/cm for (Pb0.92Gd0.02Sr0.05)(Zr0.87Sn0.12Ti0.01)O3. Moreover, the fatigue resistance of this composition is excellent within 26,000 fatigue cycles. Besides, it exhibits a high discharge energy density of 9.4 J/cm3 and a great power density of 387 MW/cm3. These results confirm that the energy storage properties of PZ-based antiferroelectric materials can be effectively optimized via a phase modulation strategy.
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