Strategically Designed Multifunctional Nanocomposite Solid Polymer Electrolytes for Futuristic Opto‐Mechanic Regulated Hybrid Energy Harvester/Storage Devices

Towards advances in multifunctional energy materials, herein, we considered the blends of electroactive P(VDF‐HFP) with plexiglass PMMA and also solid solvent PEO as efficient host polymer matrices, anhydrous LiTFSI salt as ions dopant, and piezoelectric BaTiO 3 as nanofiller, for strategic design of flexible‐type wide bandgap ionic semiconductor nanocomposite electrolytes. Four samples based on P(VDF‐HFP)/PMMA binary blend (50/50 wt%) matrix and P(VDF‐HFP)/PMMA/PEO ternary blend (50/25/25 wt%) matrix having a fixed 35 wt% concentration of LiTFSI salt, and also dispersion of 5 wt% amount of BaTiO 3 nanoparticles, are prepared through a state‐of‐the‐art solution cast route. The DSC thermograms established that all these electrolyte materials are amorphous owing to the formation of ion‐dipole complexes in the heterogeneous chains hydrogen bonded polymer network as revealed from their FTIR structural characteristics. The photosensitive and UV detection effectiveness of these electrolytes are examined from the UV–Vis absorbance spectra, which also explained dual bandgaps of about 5 eV and 3 eV establish them as wide bandgap semiconductors. The 20 Hz—1 MHz range dielectric spectroscopic study exhibited high dielectric permittivity (~10 3 ) of these electrolytes at lower frequencies having ionic conductivity of the order up to 10 −5 S/cm at 25°C. The observed correlation between chain segmental relaxation and conductivity demonstrated that the cooperative polymer chain dynamics in these complexes regulate the ions mobility that occurs through the hopping barrier transport mechanism. The electrochemical characterization reveals that these electrolytes have a total ion transference number close to unity with a considerable electrochemical stability window and charge–discharge performance. The promising optical, dielectric, electrical, and electrochemical performance of these strategically engineered electrolytes establish them as multifunctional ionic dielectric materials. Extensive photon sensing and well‐established dielectric constant dependent stress sensing characteristics of the P(VDF‐HFP) and BaTiO 3 explain that these flexible type nanocomposite materials could be potential candidates for sustainable development of next‐generation wearable‐type hybrid energy harvester/storage devices.