Flexible dielectric materials with high dielectric constant and low loss have attracted significant attention. In this work, we fabricated novel polymer-based nanocomposites with both homogeneously dispersed conductive nanofillers and ion-conductive nanodomains within a polymer matrix. An unsaturated ionic liquid (IL), 1-vinyl-3-ethylimidazolium tetrafluoroborate ([VEIM][BF₄]), was first coated on the surface of multi-walled carbon nanotubes (CNTs) by the mechanical grinding. The ILs coated CNTs were then well dispersed in poly(vinylidene fluoride) (PVDF) matrix by melt-blending. The ILs on the surface of CNTs were subsequently grafted onto the PVDF chains by electron beam irradiation (EBI). The formed ILs grafted PVDF (PVDF-g-IL) finally aggregated into ionic nanodomains with the size of 20⁻30 nm in the melt state. Therefore, novel PVDF nanocomposites with both homogenously dispersed CNTs and ionic nanodomains were achieved. Both carbon nanotubes and ionic nanodomains contributed to the enhancement of the dielectric constant of PVDF significantly. At the same time, such homogeneously dispersed CNTs along with the confined ions in the nandomains decreased current leakage effectively and thus led to the low dielectric loss. The final PVDF nanocomposites exhibited high dielectric constant, low dielectric loss and good flexibility, which may be promising for applications in soft/flexible devices.
Keywords: carbon nanotube; dielectric performance; flexibility; ionic liquid; ionic nanoclusters; poly(vinylidene fluoride) (PVDF).