Effect of BaTiO3 Additives on β-Phase Formation and Enhanced Piezoelectric Behavior of PVDF
摘要
Piezoelectric composites of poly(vinylidene fluoride) (PVDF) and barium titanate (BaTiO3) are promising candidates for flexible energy harvesting and sensing devices. Here, PVDF/BaTiO3 composite films with different BaTiO3 concentrations (50–80 wt.%) were prepared on indium tin oxide (ITO) and silver (Ag) substrates, and their structural, morphological, and piezoelectric characteristics were thoroughly explored. X-ray diffraction (XRD) results verified the retention of the BaTiO3 tetragonal perovskite structure without formation of other phases and a strong substrate-dependent diffraction effect. Fourier transform infrared (FTIR) spectroscopy revealed an increase in the electroactive β-phase of PVDF up to 60 wt.% BaTiO3, suggesting improved interfacial interactions and dipole orientation. Scanning electron microscopy (SEM) showed an evolution from dispersed particles (low filler content) to interconnected ceramic networks (medium filler content) and finally agglomerates (high filler content). This transition had a profound impact on the piezoelectric properties, with the piezoelectric coefficient (d33) peaking at 60 wt.% BaTiO3 due to a balance between the increase in β-phase, favorable dispersion, and interfacial polarization. Furthermore, Ag substrates produced composites with superior piezoelectric properties compared to ITO due to enhanced charge mobility and electric field enhancement. These findings reveal a shift from polymer-dominated effects at intermediate filler concentrations to ceramic connectivity at high concentrations. This study provides a comprehensive understanding of the structure–property relationship in PVDF/BaTiO3 composites and identifies an optimal composition for high-performance flexible piezoelectric devices.