Constructing nanocomposites with robust covalent connection between nanoparticles and polymer for high discharged energy density and excellent tensile properties

High discharged energy density and excellent flexible properties in dielectric materials are significantly sought to meet the rapid advancements in the electronics industry. In this study, covalent bonds are constructed between poly(vinylidene fluoride-chlorotrifluoroethylene), which contains olefinic bonds, and thiol-modified BaTiO3 at the interface before the nanocomposite films are fabricated. The presence of the covalent bonds is proved to promote the dispersibility of the modified BaTiO3 and enhance the interfacial adhesion between the modified BaTiO3 and the polymer, followed by a remarkably positive effect in suppressing the dielectric loss (tanδ) and increasing the breakdown strength (Eb) of the nanocomposite films. In addition, the cross-linking treatment in the preparation process is found to be favourable for improving the mechanical properties of the nanocomposite films, which benefits the enhancement of Eb. Furthermore, at 400% elongation, the stretched nanocomposite film doped with 5 vol% modified BaTiO3 exhibits an Eb 15.6% greater than that of the unstretched film, and the discharged energy density reaches 11.4 J/cm3 with a high discharge energy efficiency of 84.5%. This study provides a novel strategy for preparing flexible nanocomposites with powerful interfacial adhesion at high filler content to achieve high discharged energy density.