Graphene sheets segregated by barium titanate for polyvinylidene fluoride composites with high dielectric constant and ultralow loss tangent

In this paper, we report a unique method to develop polyvinylidene fluoride (PVDF) composites with high dielectric constant and low loss tangent by loading relatively low content of graphene-encapsulated barium titanate (BT) hybrid fillers. BT particles encapsulated with graphene oxide (BT-GO) were prepared via electrostatic self-assembly and subsequent chemical reduction resulted in BT-RGO particles. SEM morphology revealed that RGO sheets were segregated by BT particles. The hybrid fillers have two advantages for tuning dielectric properties: loading extremely low content of RGO can be exactly controlled and individual RGO sheets segregated by BT particles would prevent leakage current. As a result, PVDF composites filled with BT-RGO displayed improved dielectric properties before percolative behavior occurred. Composites filled with 30 vol% BT-RGO have a dielectric constant and loss tangent (tan δ) value of 67.5 and 0.060 (1 kHz), respectively. By contrast, dielectric constant and tan δ of composites filled with 30 vol% BT-GO and BT were 57.7 and 38.3, 0.076 and 0.042 (1 kHz), respectively. The improvement of dielectric constant is attributable to the formation of microcapacitors by highly conductive RGO sheets segregated by BT particles. Meanwhile, the distance between adjacent RGO sheets is large enough to prevent leakage current from tunneling conductance, by which tan δ is remarkably constrained. The composites could achieve excellent dielectric properties by loading relatively low amount of ceramic fillers, which indicates that this method can be used as guideline for reduce the usage amount of ceramic fillers.