Significantly Enhanced Energy Density by Tailoring the Interface in Hierarchically Structured TiO₂-BaTiO₃-TiO₂...

Dielectric polymer nanocomposites with a high breakdown field and high dielectric constant have drawn significant attention in modern electrical and electronic industries due to their potential applications in dielectric and energy storage systems. The interfaces of the nanomaterials play a significant role in improving the dielectric performance of polymer nanocomposites. In this work, polydopamine (dopa)-functionalized TiO₂-BaTiO₃-TiO₂ (TiO₂-BT-TiO₂@dopa) core@double-shell nanoparticles have been developed as novel nanofillers for high-energy-density capacitor applications. The hierarchically designed nanofillers help in tailoring the interfaces surrounding the polymer matrix as well as act as individual capacitors in which the core and outer TiO₂ shell function as a capacitor plate because of their high electrical conductivity while the middle BT layer functions as a dielectric medium due to high dielectric constant. Detailed electrical characterizations have revealed that TiO₂-BT-TiO₂@dopa/poly(vinylidene fluoride) (PVDF) possesses a higher relative dielectric permittivity (ε_r), breakdown strength ( E_b), and energy density as compared to those of PVDF, TiO₂/PVDF, TiO₂@dopa/PVDF, and TiO₂-BT@dopa/PVDF polymer nanocomposites. The ε_r and energy density of TiO₂-BT-TiO₂@dopa/PVDF were 12.6 at 1 kHz and 4.4 J cm^-3 at 3128 kV cm^-1, respectively, which were comparatively much higher than those of commercially available biaxially oriented polypropylene having ε_r of 2.2 and the energy density of 1.2 J cm^-3 at a much higher electric field of 6400 kV cm^-1. It is expected that these results will further open new avenues for the design of novel architecture for high-performance polymer nanocomposite-based capacitors having core@multishell nanofillers with tailored interfaces.