Effect of Various Nanofillers on Piezoelectric Nanogenerator Performance of P(VDF-TrFE) Nanocomposite Thin Film

Flexible polymer-based piezoelectric nanogenerators (PENGs) have gained significant interest due to their ability to deliver clean and sustainable energy for self-powered electronics and wearable devices. Recently, the incorporation of fillers into the ferroelectric polymer matrix has been used to improve the relatively low piezoelectric properties of polymer-based PENGs. In this study, we investigated the effect of various nanofillers such as titania (TiO₂), zinc oxide (ZnO), reduced graphene oxide (rGO), and lead zirconate titanate (PZT) on the PENG performance of the nanocomposite thin films containing the nanofillers in poly(vinylidene fluoride-co-trifluoro ethylene) (P(VDF-TrFE)) matrix. The nanocomposite films were prepared by depositing molecularly thin films of P(VDF-TrFE) and nanofiller nanoparticles (NPs) spread at the air/water interface onto the indium tin oxide-coated polyethylene terephthalate (ITO-PET) substrate, and they were characterized by measuring their microstructures, crystallinity, β-phase contents, and piezoelectric coefficients (<i>d</i>₃₃) using SEM, FT-IR, XRD, and quasi-static meter, respectively. Multiple PENGs incorporating various nanofillers within the polymer matrix were developed by assembling thin film-coated substrates into a sandwich-like structure. Their piezoelectric properties, such as open-circuit output voltage (<i>V_OC</i>) and short-circuit current (<i>I_SC</i>), were analyzed. As a result, the PENG containing 4 wt% PZT, which was named P-PZT-4, showed the best performance of <i>V_OC</i> of 68.5 V with the <i>d</i>₃₃ value of 78.2 pC/N and β-phase content of 97%. The order of the maximum <i>V_OC</i> values for the PENGs of nanocomposite thin films containing various nanofillers was PZT (68.5 V) > rGO (64.0 V) > ZnO (50.9 V) > TiO₂ (48.1 V). When the best optimum PENG was integrated into a simple circuit comprising rectifiers and a capacitor, it demonstrated an excellent two-dimensional power density of 20.6 μW/cm² and an energy storage capacity of 531.4 μJ within 3 min. This piezoelectric performance of PENG with the optimized nanofiller type and content was found to be superior when it was compared with those in the literature. This PENG comprising nanocomposite thin film with optimized nanofiller type and content shows a potential application for a power source for low-powered electronics such as wearable devices.