High‐Throughput Phase‐Field Design of High‐Energy‐Density Polymer Nanocomposites

Abstract Understanding the dielectric breakdown behavior of polymer nanocomposites is crucial to the design of high‐energy‐density dielectric materials with reliable performances. It is however challenging to predict the breakdown behavior due to the complicated factors involved in this highly nonequilibrium process. In this work, a comprehensive phase‐field model is developed to investigate the breakdown behavior of polymer nanocomposites under electrostatic stimuli. It is found that the breakdown strength and path significantly depend on the microstructure of the nanocomposite. The predicted breakdown strengths for polymer nanocomposites with specific microstructures agree with existing experimental measurements. Using this phase‐field model, a high throughput calculation is performed to seek the optimal microstructure. Based on the high‐throughput calculation, a sandwich microstructure for PVDF–BaTiO 3 nanocomposite is designed, where the upper and lower layers are filled with parallel nanosheets and the middle layer is filled with vertical nanofibers. It has an enhanced energy density of 2.44 times that of the pure PVDF polymer. The present work provides a computational approach for understanding the electrostatic breakdown, and it is expected to stimulate future experimental efforts on synthesizing polymer nanocomposites with novel microstructures to achieve high performances.