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<p>Lead-free 0.95Bi<sub>0.5</sub>Na<sub>0.5</sub>TiO<sub>3</sub>–0.05BaTiO<sub>3</sub> (BNT–5BT) ceramics were Cu/Zr co-doped to improve the electromechanical properties relevant to low-power energy harvesting. Based on the optimized single-dopant contents (1&#xa0;mol% CuO and 2&#xa0;mol% Zr), the co-doped composition 0.95(Bi<sub>0.5</sub>Na<sub>0.5</sub>)(Ti<sub>0.98</sub>Zr<sub>0.02</sub>)O<sub>3</sub>–0.05Ba(Ti<sub>0.98</sub>Zr<sub>0.02</sub>)O<sub>3</sub>–0.01CuO (BNT–5BT–2Zr–1Cu) was synthesized by solid-state reaction with mechanochemical activation. X-ray diffraction and Raman spectroscopy confirmed the formation of a single perovskite phase and an increased tetragonal contribution compared to the single-doped counterparts, consistent with morphotropic phase boundary (MPB) stabilization. Co-doping increased the ferroelectric–relaxor crossover temperature (T<sub>F–R</sub> = 195&#xa0;°C) while reducing the room-temperature permittivity, thereby enhancing the piezoelectric voltage response. The co-doped ceramic exhibited <i>ρ</i> = 5.74&#xa0;g·cm<sup>−3</sup>, d<sub>33</sub> = 130 pC·N<sup>−1</sup>, and g<sub>33</sub> = 10.71 × 10<sup>–3</sup>&#xa0;V·m·N<sup>−1</sup>, outperforming the undoped and single-doped reference compositions. These results indicate that Cu/Zr co-doping, combining Cu-assisted densification and defect equilibration with Zr-induced structural tuning, is an effective strategy to enhance the voltage response of lead-free BNT–BT ceramics for low-power energy harvesting applications.</p>

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Optimization of piezoelectric performance in lead-free BNT–5BT ceramics by Cu/Zr Co-doping: structure–property correlations

  • 期刊论文

  • 发表日期：

    2026年7月23日

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  • Mauro Difeo,
  • Javier Camargo,
  • Miriam Castro,
  • Leandro Ramajo

摘要

Lead-free 0.95Bi0.5Na0.5TiO3–0.05BaTiO3 (BNT–5BT) ceramics were Cu/Zr co-doped to improve the electromechanical properties relevant to low-power energy harvesting. Based on the optimized single-dopant contents (1 mol% CuO and 2 mol% Zr), the co-doped composition 0.95(Bi0.5Na0.5)(Ti0.98Zr0.02)O3–0.05Ba(Ti0.98Zr0.02)O3–0.01CuO (BNT–5BT–2Zr–1Cu) was synthesized by solid-state reaction with mechanochemical activation. X-ray diffraction and Raman spectroscopy confirmed the formation of a single perovskite phase and an increased tetragonal contribution compared to the single-doped counterparts, consistent with morphotropic phase boundary (MPB) stabilization. Co-doping increased the ferroelectric–relaxor crossover temperature (TF–R = 195 °C) while reducing the room-temperature permittivity, thereby enhancing the piezoelectric voltage response. The co-doped ceramic exhibited ρ = 5.74 g·cm−3, d33 = 130 pC·N−1, and g33 = 10.71 × 10–3 V·m·N−1, outperforming the undoped and single-doped reference compositions. These results indicate that Cu/Zr co-doping, combining Cu-assisted densification and defect equilibration with Zr-induced structural tuning, is an effective strategy to enhance the voltage response of lead-free BNT–BT ceramics for low-power energy harvesting applications.