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This paper synthesizes lead-free tetragonal BaTiO3 nanoparticles with controlled distortion via a ligand-assisted sol-gel method, achieving enhanced piezoelectric performance by engineering Ti-O covalency and dipole coherence through size and annealing optimization. The resulting hybrid piezoelectric nanogenerators (PENGs) exhibit significantly improved voltage generation and energy storage (BTO-900) or higher power density and current (BTO-1200) by synergistically combining intrinsic piezoelectricity with triboelectric effects. These findings demonstrate a promising pathway for high-performance, lead-free energy harvesting devices through nanoparticle material and interface engineering.
Nanoparticle size and bonding engineering unlock lead-free BaTiO3 piezoelectric nanogenerators with over 100 V output and microjoule-level energy storage.
Lead-free ferroelectric BaTiO3 (BTO) nanoparticles with stabilized tetragonal distortion were synthesized via a ligand-assisted sol-gel method to serve as the active piezoelectric phase in high-performance hybrid piezoelectric nanogenerators (PENGs) operating with triboelectric synergy. XRD, Raman spectroscopy, and Pair Distribution Function (PDF) analysis confirmed pseudo-cubic tetragonal BTO nanoparticle, annealed at 900{\deg}C (BTO-900, ~54nm) and well-defined tetragonal BTO annealed at 1200{\deg}C (BTO-1200, ~104nm). Density Functional Theory (DFT) calculations confirmed enhanced Ti-O covalency, stronger Ti 3d-O 2p hybridization, narrower HOMO-LUMO gap, and improved dipole coherence in BTO-900, indicating superior ferroelectric polarization, piezoelectric activity, and charge retention. BTO-900-PDMS PENG device generated a high open-circuit voltage of ~100 V and stored ~29 {\mu}J energy, and superior capacitor-charging performance of BTO-900, while the optimized BTO-1200 based device showed a higher power density of ~649 {\mu}W cm-2 and short-circuit current of ~181 {\mu}A. The superior performance of BTO-900 was attributed to enhanced defect-assisted charge trapping, interfacial polarization, and impedance-controlled charge retention. By coupling the intrinsic piezoelectric response of covalency-engineered tetragonal BTO with triboelectric charge generation at the BTO-PDMS interface, this work establishes nanoparticle size and bonding engineering as an effective route to high-output, lead-free piezoelectric nanogenerators for self-powered electronics.