Optimizing Output Power Density in Lead-Free Energy-Harvesting Piezoceramics with an Entropy-Increasing Polymorphic Phase Transition Structure.

It is an urgent need to develop lead-free piezoelectric energy harvesters (PEHs) to address the energy dilemma and meet environmental protection requirements. However, the low output power densities limit further promotion of lead-free PEHs for use in daily life. Here, an entropy-increasing strategy is proposed to achieve an increased output power density of 819 μW/cm in lead-free potassium sodium niobate (KNN)-based piezoceramics by increasing the configuration entropy and realizing nearly two times the growth compared with low-entropy counterparts. Evolution of the energy-harvesting performance with increasing configuration entropy is demonstrated systematically, and the excellent energy-harvesting properties achieved are attributed to the enhanced lattice distortion, the flexible polarization configuration, and the high-density randomly distributed nanodomains with the entropy-increasing effect. Moreover, excellent vibration fatigue resistance and variable temperature output power characteristics were also realized in the PEH prepared by the proposed entropy-increasing material. The significant enhancement of the comprehensive energy-harvesting performance demonstrates that the construction of KNN-based ceramics with high configuration entropy represents an effective and convenient strategy to enable design of high-performance piezoceramics and thus promotes the development of advanced PEHs.