K0.5Na0.5NbO3 (KNN)-based ceramics with large polarization (Pmax) and submicron grain size are considered as promising candidates for dielectric capacitors. However, the existence of significant remnant polarization (Pr) imposes constraints on achieving high recoverable energy storage density (Wrec) and efficiency (η). In this study, we developed and produced ceramic materials by utilizing the composition of (1-x)K0.5Na0.5NbO3-xBi(Mg0.5Hf0.5)O3 ((1-x)KNN-xBMH, x = 0–0.22), employing a viscous polymer rolling technique. We utilized a combined strategy to improve the energy storage capabilities of these materials by manipulating their crystal structures, inducing relaxor behavior, and minimizing microdefects. As a result, we obtained an optimum Wrec of 3.32 J/cm3 and η of 85.37 % at an electric field strength of 350 kV/cm in the x = 0.18 ceramic. Furthermore, excellent temperature stability was observed within the temperature range 20–120 °C, along with frequency stability across frequencies between 5 and 500 Hz. Moreover, at 200 kV/cm in the same composition (i.e., 0.82KNN-0.18BMH), we obtained a power density value as high as 103.13 MW/cm3, accompanied by a fast discharge speed reaching 30.6 ns. Overall, our results demonstrate that the comprehensive energy storage performances exhibited by the 0.82KNN-0.18BMH ceramic make it highly promising for applications in pulsed-power supply.
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