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–3 and 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.