Self-Assembled MXene@Fluorographene Hybrid for High Dielectric Constant and Low Loss Ferroelectric Polymer Composite Films

Modern electrical applications urgently need flexible polymer films with a high dielectric constant (εr) and low loss. Recently, the MXene-filled percolative composite has emerged as a potential material choice because of the promised high εr. Nevertheless, the typically accompanied high dielectric loss hinders its applications. Herein, a facile and effective surface modification strategy of cladding Ti3C2Tx MXene (T = F or O; FMX) with fluorographene (FG) via self-assembly is proposed. The obtained FMX@FG hybrid yields high εr (up to 108 @1 kHz) and low loss (loss tangent tan δ = 1.16 @ 1 kHz) in a ferroelectric polymer composite at a low loading level (the equivalent of 1.5 wt % FMX), which is superior to its counterparts in our work (e.g., FMX: εr = 104, tan δ = 10.71) and other studies. It is found that the FG layer outside FMX plays a critical role in both the high dielectric constant and low loss from experimental characterizations and finite element simulations. For one thing, FG with a high F/C ratio would induce a favorable structure of high β-phase crystallinity, extensive microcapacitor networks, and abundant interfacial dipoles in polymer composites that account for the high εr. For another, FG, as a highly insulating layer, can inhibit the formation of conductive networks and inter-FMX electron tunneling, which is responsible for conduction loss. The results demonstrate the potential of a self-assembled FMX@FG hybrid for high εr and low loss polymer composite films and offer a new strategy for designing advanced polymer composite dielectrics.