Enhanced dielectric response of ternary polymeric composite films via interfacial bonding between V2C MXene and wide-bandgap ZnS

Abstract Increasing the dielectric constant of polymer/sulfide ceramic composites by using wide-bandgap semiconducting sulfide ceramic fillers like ZnS is difficult because of their low interface polarization. To increase the dielectric constant, in this study, ternary polymer-based composite films were designed and fabricated using a hybrid filler consisting of shell-like ZnS particles and core-like V2C MXene particles. First, V2C MXene with a multi-layered structure was synthesized from the simplest raw materials followed by the in-situ hydrothermal growth of ZnS particles around the V2C particles. Then, binary polymer/ZnS and ternary polymer/V2C–ZnS composites were fabricated, and their dielectric, conductive, and electrical breakdown properties were investigated. Finally, the effect of interfacial bonding between the V2C and ZnS phases was investigated by density functional theory calculations, and the contribution of V2C/ZnS interfacial bonding to the higher dielectric constant of the ternary composites than that of the binary composites was explained. The ternary composites exhibited balanced electrical properties suitable for energy storage applications. The ternary composite with 10 wt% hybrid filler loading exhibited a high dielectric constant of ~52, a low dielectric loss of ~0.11 at 100 Hz, and a high electrical breakdown strength of ~202 MV m−1. This study paves the way for the facile fabrication of high-performance composite dielectrics for application in advanced capacitors.