Enhanced discharge energy density of rGO/PVDF nanocomposites: The role of the heterointerface

Recent reports of conductive-filler/polymer composites with large dielectric permittivity (K) make them potential candidates for flexible capacitors. Hence, an interesting question is how these high K composites behave under a strong electric field strength. In this letter, we use in-situ-reduced graphite oxide (rGO)/poly(vinylidene fluoride) (PVDF) nanocomposites as an example to study the energy storage behaviour of high K materials. We show the dielectric behaviour contrasts between weak and strong fields. High K materials inevitably become more lossy with increasing field strength. Simultaneously, we reveal that the in-situ reduction temperature can affect the energy storage performance. Improved energy storage performance is achieved for a nanocomposite reduced at a moderate temperature. When reduced at 160 C, a device with an rGO volume fraction of 1.5 vol. % displayed a discharge energy density of 0.67 J/cm3 at 50 MV/m. This was 2.9 times greater than pure PVDF. We develop a model to explain this behaviour that proposes a reduced electrical contrast of the rGO/PVDF heterointerface minimising the recombination of localized charge carriers. Our results indicate, simultaneously, the potential and limitation of high K nanocomposites and shed light on the optimisation of the design and fabrication of high discharge energy density flexible capacitors for microelectronic devices.