Piezoelectric Enhancement in P(VDF-TrFE) Copolymer Films via Controlled and Template-Induced Epitaxy

The surge in wearable electronics and Internet of Things technologies necessitates the development of both flexible sensors and a sustainable, efficient, and compact power source. The latter further challenges conventional batteries due to environmental pollution and compatibility issues. Addressing this gap, piezoelectric energy harvesters emerge as one kind of promising alternative to convert mechanical energy from ambient sources to electrical energy to charge those low-energy-consumption electronic devices. Despite slightly lower piezoelectric performance compared with those inorganic materials, piezoelectric polymers, notably poly(vinylidene fluoride-co-trifluoroethylene) P(VDF-TrFE), offer compelling properties for both flexible mechanical energy harvesting and self-powered strain/stress sensing, though their piezoelectric performance is expected to be further enhanced via varieties of modulation strategies of microstructures. Herein, we reported the controlled epitaxy process of micrometer-thick copolymer films with the cooperation of friction-transferred poly(tetrafluoroethylene) templates and precise modulation of the annealing conditions. Epitaxial P(VDF-TrFE) films present averaged d₃₃ piezoelectric coefficient of -58.2 pC/N between 50 Hz and 1 kHz with good electromechanical and thermal stability. Owing to the nature of anisotropic crystallization, the epitaxial films exhibit an anisotropic transverse piezoelectric property. Epitaxial films were further utilized for mechanical energy harvesting and monitoring of human pulsation and respiration. This study provided a feasible route for the development of high-performance flexible piezoelectric devices to meet the requirement of flexible electronics.