Enhanced Energy Storage Performance of Polymer/Ceramic/Metal Composites by Increase of Thermal Conductivity and Coulomb-Blockade Effect

Polymer-based dielectrics have attracted considerable attention for a wide range of applications as energy storage devices with high power. However, high loss from low thermal conductivity (K) and leaky current may limit their practical utilization greatly. To overcome these issues, two-dimensional hexagonal boron nitride (h-BN) modified with polydopamine (PDA) and metal palladium nanoparticles (h-BN@PDA@Pd NPs) are introduced into a poly­(vinylidene fluoride-hexafluoropropylene) P­(VDF-HFP) copolymer matrix. The PDA coating improves the compatibility between the ceramic h-BN filler and the polymer matrix. Contrary to the general idea, the metallic Pd NPs enhance the breakdown strength of the polymer nanocomposites through the Coulomb-blockade effect. The nanocomposite film filled with 6 vol % h-BN@PDA@Pd NPs exhibits significantly improved recoverable energy density (U_rec) of 58.6 J cm^–3, which is increasedby 496% compared to pure P­(VDF-HFP) film, maintaining an efficiency of 65%, even under a high voltage of 500 MV m^–1. The in-plane thermal conductivity of the nanocomposites was improved from 0.21 to 1.02 W m^–1 K^–1 with increasing ceramic h-BN content. This study suggests that a dielectric polymer with surface-engineered ceramic h-BN fillers through a Coulomb-blockade effect of metal Pd NPs might be a promising strategy for high energy storage devices.