High
dielectric constant and breakdown strength are crucial for
high-energy-density polymer/ceramic composites. Anatase-TiO2 with low dielectric constant and V2C MXene with high
work function are not satisfactory fillers. In the present work, V2C–TiO2 hybrid filler was in situ synthesized,
followed by fabricating poly(vinylidene fluoride) (PVDF)/V2C–TiO2 composites via solution cast. Compared with
PVDF/TiO2 and PVDF/V2C composites, PVDF/V2C–TiO2 composites have an improved high
dielectric constant, depressed low dielectric loss, and maintained
high breakdown strength. High overall electric traits are ascribed
to the synergy of conductive V2C and semiconductive TiO2. Outer and inner surfaces of V2C were ornament-combined
by anatase-TiO2 particles having surface point defects
as electron traps, contributing to low interface leakage conduction.
Through density functional theory (DFT) calculations, nontypical V–F–Ti-bonding-induced
dipole enhancement and Fermi-level (E
F) overlapping-induced high electron localization mechanisms improve
the dielectric response. Ternary composite with 10 wt % hybrid filler
exhibits a dielectric constant of ∼99, a dielectric loss of
∼0.24 at 1 kHz, and a breakdown strength of ∼189 MV/m.
This work might enable large-scale preparation of promising polymer/MXene
composite dielectrics.
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