Abstract
Due to growing environmental concerns on the toxicity of lead-based piezoelectric materials, lead-free alternatives are urgently required but so far have not been able to reach competitive performance. Here we employ a novel phase-boundary engineering strategy utilizing the multiphase convergence, which induces a broad structural flexibility in a wide phase-boundary zone with contiguous polymorphic phase transitions. We achieve an ultrahigh piezoelectric constant ( d33) of 700 ± 30 pC/N in BaTiO3-based ceramics, maintaining >600 pC/N over a wide composition range. Atomic resolution polarization mapping by Z-contrast imaging reveals the coexistence of three ferroelectric phases (T + O + R) at the nanoscale with nanoscale polarization rotation between them. Theoretical simulations confirm greatly reduced energy barriers facilitating polarization rotation. Our lead-free material exceeds the performance of the majority of lead-based systems (including the benchmark PZT-5H) in the temperature range of 10-40 °C, making it suitable as a lead-free replacement in practical applications. This work offers a new paradigm for designing lead-free functional materials with superior electromechanical properties.
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