Enhanced energy storage performance and relaxor behavior in CaZrO3-modified 0.76Bi0.5Na0.5TiO3-0.24Sr0.7La0.2TiO3 lead-free ceramics
摘要
In pursuit of lead-free dielectric materials possessing superior energy density and outstanding reliability under intermediate electric field conditions, this study fabricated (1-x)(0.76Bi0.5Na0.5TiO3-0.24Sr0.7La0.2TiO3)-xCaZrO3 (BNSLT-xCZ; x = 0.00, 0.05, 0.10, 0.15) relaxor ferroelectrics via the classic solid-state ceramic processing. This study systematically explores how CaZrO3 (CZ) incorporation modulates the phase development, microstructural features, dielectric response, and energy storage capabilities. XRD patterns verify the formation of a single-phase perovskite structure, indicating that CZ has been successfully integrated into the BNSLT host lattice without any visible impurities. The evolution of a tripartite phase system—comprising cubic, rhombohedral, and tetragonal symmetries—is facilitated by optimal substitution (x = 0.10–0.15). With the suppression of macro-domain ferroelectric order, the formation of polar nanoregions (PNRs) is effectively facilitated, which subsequently enhances the dielectric relaxation response. Noticeably, the x = 0.10 composition achieves a high recoverable energy storage density (Wrec) of 2.91 J/cm3 at a modest electric field of 220 kV/cm, with an efficiency (η) of 64.3% and a maximum polarization (Pmax) of 37.8 μC/cm2. Furthermore, the ceramic demonstrates excellent thermal stability (with Wrec variation < ± 10% from 30 to 150 °C) and robust frequency stability (from 5 to 100 Hz) under a fixed field of 180 kV/cm, surpassing many reported lead-free systems operating at similar field levels. These results demonstrate that CZ doping enables the synergistic optimization of phase composition and microstructure, providing a promising strategy for emerging micro-scale energy storage devices.