Enhanced Energy Density at a Low Electric Field in PVDF-Based Heterojunctions Sandwiched with High Ion-Polarized BTO Films

Inorganic/organic dielectric composites with outstanding energy storage properties at a low electric field possess the advantages of low operating voltage and small probability of failure. Composites filled with two-dimensional inorganic nanosheets have attracted much attention owing to their fewer interfacial defects caused by the agglomeration of fillers. Continuous oxide films with a preferred orientation can play a significant role in enhancing energy storage. The challenge is to prepare large-sized, freestanding, single-crystal, ferroelectric oxide films and to combine them with polymers. In this work, a well-developed water-dissolvent process was used to transfer millimeter-sized (100)-oriented BaTiO₃(BTO) films. Poly(vinylidene fluoride) (PVDF)-based heterojunctions sandwiched with the single-crystal films were synthesized via the transferring process and an optimized hot-pressing technique. By virtue of high ion displacement polarization and inhibited conductive path formation of single-crystal BTO films, the energy storage density and efficiency of BTO/PVDF heterojunctions reach 1.56 J cm^-3and 71.2% at a low electric field of 120 MV m^-1, which are much higher than those of pure PVDF and BTO nanoparticles/PVDF composite films, respectively. A finite-element simulation was employed to further confirm the experimental results. This work provides an effective approach to enhance energy storage properties in various polymer-based composites and opens the door to advanced dielectric capacitors.