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Defect engineering plays an important role in property modification for piezoelectric materials. In this work, we pay much attention to the effect of Nb nonstoichiometry on structure and properties of typical 0.95(K0.45Na0.55)Nb1+xO3–0.05Bi0.5Na0.5HfO3 ceramics. Large piezoelectric constant (d33 ~ 425 pC/N and d33∗ ~482 pm/V) together with high Curie temperature (TC ~ 315°C) have been achieved in the ceramics with excess Nb content (x = 0.01). However, the ceramics with deficient Nb element have seriously suppressed cryogenic εr‐T curves and deteriorated electrical properties. Multi‐scale characterizations including phase structure, microstructure, defect structure and domain structure have been adopted to explain the corresponding phenomenon. Defect complex VNb″″′-VO·· caused by deficient Nb induces clamped domain wall motion, leading to blocked polarization vector and poor electrical properties. On the contrary, the enhanced properties for the ceramics with excess Nb are attributed to easier domain switching due to the suppressed vacancies. We believe that defect engineering, for example nonstoichiometry, cannot only modulate electrical properties but also help us to understand some fundamental and critical problems about KNN‐based ceramics. [ABSTRACT FROM AUTHOR]

The strategy of modulating polarization rotation of potassium sodium-niobate ((K 0.5 Na 0.5)NbO 3 , KNN) lead-free piezoelectric materials was reported to boost piezoelectric properties and resultant piezocatalytic activities. The effectiveness of modulating polarization rotation was proved by degrading Rhodamine B (RhB) using three KNN-based samples with different phase structures (i.e., orthorhombic (O) phase, orthorhombic-tetragonal (O-T) coexistence phase, and rhombohedral-orthorhombic-tetragonal (R-O-T) coexistence phase). Poled samples with the R-O-T coexistence phase show a reaction rate constant of 0.091 min−1 owing to the easiest polarization rotation, 2.12 times more than that of poled O-phase featured samples with the most difficult polarization rotation. Enhanced piezocatalytic activities primarily originate from the easier polarization rotation and improved carrier concentration, accompanied by the trace of the mechano-charge generation. Therefore, modulating polarization rotation effectively boosts piezocatalysis of KNN-based materials, promising for harnessing natural energy and disease treatment. [Display omitted] • lead-free (K, Na)NbO 3 materials are eco-friendly piezocatalyst. • Proposing a new strategy to enhance there piezocatalysis. • Obtaining a high k value of 0.091 min−1, much superior to those of other materials. • Unveiling the physical mechanisms of the superior piezocatalytic activities. [ABSTRACT FROM AUTHOR]