Ordering‐Structured Antiferroelectric Composite Ceramics for Energy Storage Applications

Abstract Dielectric capacitors possessing high power density and ultrashort discharge time are valuable for high‐power energy storage applications. However, achieving high energy storage density remains challenging due to the limited breakdown strength of dielectric ceramics. In this study, inspired by the layered architecture of natural nacre and with the guidance of phase‐field simulations, a strategy of constructing a nacre‐like layered structure is proposed to improve the breakdown strength and energy storage density of the ceramics. This unique structure is formed by controlling the morphology and ordering of high‐voltage‐resistant fillers in a ceramic matrix. The (Pb 0.98 La 0.02 )(Zr 0.7 Sn 0.3 ) 0.995 O 3 ‐Al 2 O 3 antiferroelectric composite ceramics, containing 5vol% parallel‐aligned Al 2 O 3 plates, demonstrate a remarkable enhancement in breakdown strength from 390 to 570 kV cm −1 . Of particular importance is that an ultrahigh recoverable energy storage density of up to 13.2 J cm −3 is achieved, representing a 50% enhancement compared to the pure ceramic (8.7 J cm −3 ). The parallel‐aligned Al 2 O 3 plates are strongly bound together with the ceramic matrix, effectively blocking charge migration and controlling the breakdown path, thus greatly enhancing the voltage endurance of the composite ceramics. This work provides an innovative approach to designing high‐performance composite ceramics for next‐generation energy storage applications.