(1-x)(0.9Ba1.003Ti0.97Ca0.03O3–0.1(Bi0.51Na0.47)0.94Ba0.06TiO3)-xNa(Nb0.85Ta0.15)O3 (x = 0.03–0.15) ceramics were designed and fabricated through a bidirectional optimization strategy using traditional solid reaction method. The results revealed that the introduction of Na(Nb0.85Ta0.15)O3 increased the vacancy concentration at the A site, conducing to improved polarization and reduced grain size. The substitution at the B site disrupted the long-range ordered ferroelectric domains and generated polar nanodomains, leading to enhanced relaxation behavior. The optimum energy storage density of 3.57 J/cm3 and efficiency of 87.5% were simultaneously achieved under the electric field of 220 kV/cm in the sample with x = 0.09. Moreover, it also exhibits extremely high-power density (∼57 MW/cm3), ultrafast discharge time (∼103 ns), high discharge density (1.35 J/cm3), along with excellent temperature (30‒120 °C) and frequency stability (1‒100 Hz) under the equivalent electric field of 120 kV/cm. This novel design strategy provides theoretical guidance for the development of advanced electrical energy storage devices.
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