PDA-Decorated MXene Nanosheets Lead to Elevated Dielectric Performances in PVDF Nanocomposites

As a prospective two-dimensional conductive filler, titanium carbide (MXene) can remarkably boost the dielectric constant (ε) of polymer composites at low loadings. Nevertheless, the accompanied large dielectric loss (tan δ) and leakage current greatly limit their practical applications in dielectric-related fields. To tackle this dilemma, an organic polydopamine (PDA) shell was coated on an MXene surface via a self-polymerization method, and the dielectric properties of PDA-modified MXene/poly(vinylidene fluoride) (PVDF) were explored. The findings show that, in comparison to unmodified MXene/PVDF, MXene@PDA/PVDF retains a high ε and improved breakdown strength (Eb). It further realizes a notable decrease in both tan δ and electrical conductivity. The introduced PDA interlayer serves to effectively separate adjacent MXene nanosheets, which inhibits the development of conductive paths and introduces charge traps to restrict carrier migration, thus reducing tan δ. Further, the interlayer not only improves the interfacial compatibility, but also mitigates strong dielectric mismatch between MXene and PVDF, which facilitates the homogeneous redistribution of the local electric field, contributing to enhanced Eb. Theoretical fitting and simulation studies unlock the profound polarization mechanisms and charge migration modulated by the PDA interlayer. The resulting Mxene@PDA/PVDF exhibits concurrently elevated ε (35.68) and enhanced Eb (12.94 kV/mm), as well as low tan δ (0.34) at 103 Hz and 7 wt% filler loading, which is not achievable in neat MXene/PVDF. This work demonstrates that core–shell interfacial engineering offers an effective strategy for designing flexible polymer dielectrics with superior dielectric performances, showcasing potential applications in energy storage, advanced power systems and flexible electronics.