Functionality Tuning in Hierarchically Engineered Magnetoelectric Nanocomposites for Energy-Harvesting Applications

The β-phase of the copolymer poly(vinylidene fluoride-trifluoroethylene) P(VDF-TrFE) possesses the highest dipole moment among all the functional polymers. It remains a key component of flexible energy-harvesting devices based on piezoelectricity and triboelectricity in the last decade. However, the quest for P(VDF-TrFE)-based magnetoelectric (ME) nanocomposites with enhanced ferroelectric, piezoelectric, and triboelectric properties remains elusive. The magnetostrictive inclusion in the copolymer matrix forms electrically conducting pathways and degrades β-phase crystallinity significantly, deteriorating the functional properties of the nanocomposite films. To address this issue, we report the synthesis of magnetite (Fe₃O₄) nanoparticles on micron-scale magnesium hydroxide [Mg(OH)₂] templates. These hierarchical structures were incorporated within the P(VDF-TrFE) matrix rendering composites with enhanced energy-harvesting capability. The Mg(OH)₂ template prevents the formation of a continuous network of magnetic fillers, leading to lower electrical leakage in the composite. The addition of dual-phase fillers with 5 wt % only increases remanent polarization (P_r) values by ∼44%, owing to the presence of the β-phase with significant crystallinity and increased interfacial polarization. The composite film exhibits a quasi-superparamagnetic nature and a significant magnetoelectric coupling coefficient (α_ME) of 30 mV/cm Oe. The film was also employed for triboelectric nanogenerator applications, exhibiting five times higher power density than the pristine film. We finally explored the integration of our ME devices with an internet of things platform to monitor the operational status of electrical appliances remotely. In light of these findings, the present work opens the path for future self-powered, multifunctional, and flexible ME devices with new application domains.