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Electrostatic energy storage technology based on dielectrics is the basis of advanced electronics and high-power electrical systems. High polarization (P) and high electric breakdown strength (Eb) are the key parameters for dielectric materials to achieve superior energy storage performance. In this work, a composite strategy based on antiferroelectric dielectrics (AFEs) has been proposed to improve the energy storage performance. Here, AlN is selected as the second phase for the (Pb0.915Ba0.04La0.03)(Zr0.65Sn0.3Ti0.05)O3 (PBLZST) AFEs, which is embedded in the grain boundaries to construct insulating networks and regulate the local electric field, improving the Eb. Meanwhile, it is emphasized that AFEs have the AFE–FE and FE–AFE phase transitions, and the increase of the phase transition electric fields can further improve the recoverable energy density (Wrec). As a result, the Eb increases from 180 to 290 kV·cm−1 with a simultaneous increase of the phase transition electric fields, magnifying the Wrec to ~144% of the pristine PBLZST. The mechanism for enhanced Eb and the phase transition electric fields is revealed by the finite element simulation method. Moreover, the PBLZST:1.0 wt% AlN composite ceramics exhibit favorable temperature stability, frequency stability, and charge–discharge ability, making the composite ceramics a promising candidate for energy storage applications.
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