The current global chip shortage and energy crisis has prompted research community to investigate alternative electronic and energy materials with improved performance. Here, we propose a versatile and easy to fabricate ceramic-free nanocomposite film, based on fluoropolymers and amine-functionalized graphene oxide (AGO) nanosheets with great application potentials in non-resonant energy harvesters, voltage-generating sensors, and ferroelectric random access memories. The electrical and electromechanical properties of pristine fluoropolymers are inferior due to their low polar crystalline phase content, leading to weak spontaneous and remanent polarization. By using intermolecular anchoring strategy as an interfacial coupling mechanism, we have achieved outstanding voltage coefficient, energy density, and energy-harvesting figure of merit values of 0.30 Vm/N, 4.75 J/cm3, and 14 pm3/J, respectively, making the work one of the best ceramic-free nanocomposites reported so far. Employing differential calorimetry, wide-angle and small-angle X-ray scattering analyses, we demonstrate that AGO incorporation leads to formation of bigger crystallites and higher β/α ratio, which translates into remarkably high remnant polarization of 11.3 µC/cm2. We believe this work can open up new insights towards structural and morphological tailoring of fluoropolymers to enhance their electrical and electromechanical performance and pave the way for their industrial deployment in next-generation wearable electronics and human-machine interfaces.

The electrical properties of pristine fluoropolymers are inferior due to their low polar crystalline phase content and rigid dipoles that tend to retain their fixed moment and orientation. Several strategies such as electrospinning, electrohydrodynamic pulling, and template-assisted growing have been proven to enhance the electrical properties of fluoropolymers, however, these techniques are mostly very hard to scale-up and expensive. Here, we propose a facile interfacial engineering approach based on amine-functionalized graphene oxide (AGO) to manipulate the intermolecular interactions in poly (vinylidenefluoride-trifluoroethylene) (PVDF-TrFE) to induce β-phase formation, enlarge the lamellae dimensions, and align the micro-dipoles. The coexistence of primary amine and hydroxyl groups on AGO nanosheets offers strong hydrogen bonding with fluorine atoms, which facilitates domain alignment, resulting in an exceptional remnant polarization of 11.3 µC cm-2. PVDF-TrFE films with 0.1 wt% AGO demonstrated voltage coefficient, energy density, and energy-harvesting figure of merit values of 0.30 Vm N-1, 4.75 J cm-3, and 14 pm3 J-1, respectively, making it outstanding compared with state-of-the-art ceramic-free ferroelectric films. We believe this work can open-up new insights towards structural and morphological tailoring of fluoropolymers to enhance their electrical and electromechanical performance and pave the way for their industrial deployment in next-generation wearables and human-machine interfaces.