Breakdown strength and energy density enhancement in polymer-ceramic nanocomposites: Role of particle size distribution

Polymer-ceramic nanocomposites play a very promising role for energy-storage in high power electronics and advanced pulsed power systems, due to their extremely fast charge-discharge capability. The low energy density is the key factor hindering their application, for which large endeavors have been made in the modulation of the fraction, morphology, size, and dispersion of the particle fillers but small in that of the size distribution, which is critical for energy-storage performance. We first investigated the role of this based on simulated nanocomposites with controlled lognormal distributions via a generation algorithm devised in this work. Dielectric response, breakdown behavior and energy-storage performance were explored for distributions with different standard deviations (SD) and mean values (MV), which were solved with the energy equivalence basis and a phase-field dielectric breakdown model. With the decrease of SD and MV, the effective permittivity declines slightly with enhanced permittivity change, which was related with the enhanced local electric field with intensified fluctuation and should be originated from the major contribution of the polymer matrix from the local energy perspective; whereas improved nominal breakdown strength was achieved owing to the weakened local maximum electric field, which leads to distinctly increased nominal energy density despite the slight decline of the permittivity. Keeping the fillers within a narrow disperse outperforms employing super fine particles. This work demonstrates that enhancement in breakdown strength and energy density can be attained via particle size distribution modulation, paving a new way for the further improvement of the energy-storage performance of polymer-ceramic nanocomposites.