Concurrently Achieving High Discharged Energy Density and Efficiency in Composites by Introducing Ultralow Loadings of Core–Shell Structured Graphene@TiO₂ Nanoboxes

Polymer dielectrics have drawn tremendous attention worldwide due to their huge potential for pulsed power capacitors. Recent studies have demonstrated that linear/nonlinear layered composites, which can effectively balance energy density and efficiency, have huge potential for capacitive energy storage applications. However, further enhanced energy densities are strongly desired to meet the everincreasing demand for the miniaturization of electronic devices. Herein, a novel class of core–shell structured graphene@titanium dioxide nanoboxes is successfully synthesized and introduced into poly(vinylidene fluoride-hexafluoropropylene)-poly(ether imide) double-layer films. It is exciting to find that the introduction of merely 0.5 wt % nanoboxes results in a substantially enhanced energy density of 19.39 J/cm3, which is over 2.6 times that of the film without nanoboxes (7.44 J/cm3). Meanwhile, a high breakdown strength of 655 kV/mm and a high efficiency of 83% are achieved. Furthermore, the nanocomposites also show excellent power densities and cycling stabilities. These composites with excellent comprehensive energy storage performances have huge potential for advanced pulsed power capacitors.