Significantly Enhanced Dielectric Performances and High Thermal Conductivity in Poly(vinylidene fluoride)-Based Composites Enabled by SiC@SiO Core-Shell Whiskers Alignment.

Design of composites with ordered fillers arrangement results in anisotropic performances with greatly enhanced properties along a specific direction, which is a powerful tool to optimize physical properties of composites. Well-aligned core-shell SiC@SiO whiskers in poly(vinylidene fluoride) (PVDF) matrix has been achieved via a modified spinning approach. Because of the high aspect ratio of SiC whiskers, strong anisotropy and significant enhancement in dielectric constant were observed with permittivity 854 along the parallel direction versus 71 along the perpendicular direction at 20 vol % SiC@SiO loading, while little increase in dielectric loss was found due to the highly insulating SiO shell. The anisotropic dielectric behavior of the composite is perfectly understood macroscopically to have originated from anisotropic intensity of interfacial polarization based on an equivalent circuit model of two parallel RC circuits connected in series. Furthermore, finite element simulations on the three-dimensional distribution of local electric field, polarization, and leakage current density in oriented SiC@SiO/PVDF composites under different applied electrical field directions unambiguously revealed that aligned core-shell SiC@SiO whiskers with a high aspect ratio significantly improved dielectric performances. Importantly, the thermal conductivity of the composite was synchronously enhanced over 7 times as compared to that of PVDF matrix along the parallel direction at 20 vol % SiC@SiO whiskers loading. This study highlights an effective strategy to achieve excellent comprehensive properties for high-k dielectrics.