Significantly Enhanced Energy-Harvesting Performance and Superior Fatigue-Resistant Behavior in [001]_c-Textured BaTiO₃-Based Lead-Free Piezoceramics

Energy-harvesting utilizing piezoelectric materials has recently attracted extensive attention due to the strong demand of self-powered electronics. Unfortunately, low power density and poor long-term stability seriously hinder the implementation of lead-free piezoelectrics as high-efficiency energy harvesters. For the first time, we demonstrate that tailoring grain orientations of lead-free ceramics via templated grain growth can effectively produce ultrahigh power generation performance and excellent endurance against electrical/mechanical fatigues. Significantly improved fatigue resistance was observed in (Ba_0.94Ca_0.06)(Ti_0.95Zr_0.05)O₃ grain-oriented piezoceramics (with ~99% [001]_c texture) up to 10⁶ bipolar cycles, attributed to the enhanced domain mobility, less defect accumulation, and thus suppressed crack generation/propagation. Interestingly, the novel energy harvesters, which were developed based on the textured ceramics with high electromechanical properties, possessed 9.8 times enhancement in output power density compared to the nontextured counterpart while maintaining stable output features up to 10⁶ vibration cycles. The power densities, which increased from 6.4 to 93.6 μW/mm³ with increasing acceleration excitation from 10 to 50 m/s², are much higher than those reported previously on lead-free energy harvesters. This work represents a significant advancement in piezoelectric energy-harvesting field and can provide guidelines for future efforts in this direction.