Piezoelectric ultrasonic energy harvesters (PUEHs) have recently attracted increasing attention. For minimizing the energy losses during energy transfer, it is crucial for core piezoelectric materials to maintain high piezoelectric coefficient (d33), mechanical quality factor (Qm), and piezoelectric voltage coefficient (g33). Herein, a simple way of hardening strategy improves the piezoelectric properties of KNN-based ceramics, combined with optimizing grain growth. The enhanced d33 (∼340 pC/N), high Qm (∼211) and TC (∼305 °C) are obtained simultaneously in this system, accompanied by superior d33×g33=8770×10−15 m2/N. Through variable temperature resonance test, the polarization rotation diversity caused by phase structure difference is found to closely related to the temperature stability of Qm value. A prototype of PUEH device was further designed and fabricated, with adjustable ultrasound-induced output voltage up to 8.2 V. Our work exhibits an effective way to improve performance of PUEHs by optimizing piezoelectric materials, which is helpful for further developing PUEHs.
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