Abstract

Antiferroelectric (AFE) ceramics with near-zero remanent polarization originating from unique electric field-induced antiferroelectric-ferroelectric phase transition are of great importance for the application in the energy-storage devices. However, achieving the most widely optimized switching electric field and energy-storage performance of antiferroelectric ceramics has predominantly relied on A/B-site ion doping strategies, often accomplished through a series of experimental and analytical works. In this context, we propose a novel strategy of heterogeneous laminated engineering as a substitute for A/B-site ion doping. This approach allows for a more intuitive regulation of the switching electric field and energy-storage performance in antiferroelectric ceramics without the need for complicated workload. Namely, the ferroelectric Pb0.99(Nb0.9Ta0.1)0.2(Zr0.9Sn0.1)0.8O3 (PNTZS) and antiferroelectric (Pb0.875La0.05Sr0.05) (Zr0.7Sn0.3)O3 (PLSZS) were layer-by-layer laminated using a tape-casting technique. All heterogeneous laminated ceramics exhibit antiferroelectric characteristics, and the magnitude of the switching electric field can be controlled by regulating the ratio between PNTZS and PLSZS. Furthermore, the finite element simulation revealed differences in the local electric fields between PNTZS and PLSZS in heterogeneous laminated ceramics, resulting in a win-win situation for both polarization and the breakdown strength. A large recoverable energy density of 11.2 J cm−3 with ultrahigh energy efficiency of 94.2 % can be obtained under 56 kV mm−1. Moreover, the energy storage performance shows no obvious deterioration in a broad frequency range (1–100 Hz) and temperature range (25–120 °C). Particularly, the outstanding discharge properties with a large discharge energy density of 7.1 J cm−3 and a high power density of 263.7 MW cm−3 show great potential for energy-storage applications. To conclude, a new strategy is opened up herein for designing antiferroelectric energy storage materials, showing the great application potential in the pulse power devices.

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