In this report, a simple solution-cast method was employed to prepare poly(dopamine) (PDA) encapsulated BaTiO (BT) nanoparticle (PDA@BT) filled composites using PVDF matrix cross-linked by the free radical initiator. The effects of both the particle encapsulation and matrix cross-linking on the mechanical and dielectric properties of the composites were carefully investigated. The results suggested that the introduction of BT particles improved permittivity of the composites to ∼30 at 100 Hz when particle contents of only 7 wt % were utilized. This was attributed to the enhanced polarization, which was induced by high permittivity ceramic particles. Compared to bare BT, PDA@BT particles could be dispersed more homogeneously in the matrix, and the catechol groups of PDA layer might form chelation with free ions present in the matrix. The latter might depress the ion conduction loss in the composites. Other results revealed that the formation of hydrogen-bonding between the PDA layer and the polymer, especially the chemical cross-linking across the matrix, resulted in increased Young' modulus by ∼25%, improved breakdown strength by ∼40%, and declined conductivity by nearly 1 order of magnitude when compared to BT filled composites. The composite films filled with PDA@BTs indicated greater energy storage capacities by nearly 190% when compared to the pristine matrix. More importantly, the excellent mechanical performance allowed the composite films to adopt uni- or biaxially stretching, a crucial feature required for the realization of high breakdown strength. This work provided a facile strategy for fabrication of flexible and stretchable dielectric composites with depressed dielectric loss and enhanced energy storage capacity at low filler loadings (<10 wt %).

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Remarkably improved dielectric properties including high-k, low loss, and high breakdown strength combined with promising mechanical performance such as high flexibility, good heat, and chemical resistivity are hard to be achieved in high-k dielectric composites based on the current composite fabrication strategy. In this work, a family of high-k polymer nanocomposites has been fabricated from a facile suspension cast process followed by chemical cross-linking at elevated temperature. Internal double bonds bearing poly(vinylidene fluoride-chlorotrifluoroethylene) (P(VDF-CTFE-DB)) in total amorphous phase are employed as cross-linkable polymer matrix. α-SiC particles with a diameter of 500 nm are surface modified with 3-aminpropyltriethoxysilane (KH-550) as fillers for their comparable dielectric performance with PVDF polymer matrix, low conductivity, and high breakdown strength. The interface between SiC particles and PVDF matrix has been finely tailored, which leads to the significantly elevated dielectric constant from 10 to over 120 in SiC particles due to the strong induced polarization. As a result, a remarkably improved dielectric constant (ca. 70) has been observed in c-PVDF/m-SiC composites bearing 36 vol % SiC, which could be perfectly predicted by the effective medium approximation (EMA) model. The optimized interface and enhanced compatibility between two components are also responsible for the depressed conductivity and dielectric loss in the resultant composites. Chemical cross-linking constructed in the composites results in promising mechanical flexibility, good heat and chemical stability, and elevated tensile performance of the composites. Therefore, excellent dielectric and mechanical properties are finely balanced in the PVDF/α-SiC composites. This work might provide a facile and effective strategy to fabricate high-k dielectric composites with promising comprehensive performance.

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Simultaneously improved permittivity and breakdown strength, accompanied with reduced dielectric loss and conductivity, are difficult to achieve in polymer nanocomposites with conductive fillers by blending to construct a homogeneous structure.