Effects of heterovalent ions doping-induced oxygen octahedral distortion and defect chemical change on piezoelectric characteristics and thermal stability of PHT-PIN ceramics

•Li+ and W6+ Doping shortened the BO bond and enhanced the B-site ionic shift.•Microdomains caused by octahedral distortion of oxygen improved the properties.•Octahedral distortion and defect chemistry enhanced thermal stability. Electromechanical devices require functional materials possessing excellent piezoelectric properties, good thermal stability, and high electromechanical coupling coefficients. To modulate the piezoelectric, dielectric, and electromechanical characteristics of 0.89Pb(Hf0.47Ti0.53)O3-0.11Pb(In1/2Nb1/2)O3 (PHT-PIN) piezoelectric ceramics, heterovalent ions of lithium (Li) and tungsten (W) were doped through a traditional solid-phase reaction approach. On the one hand, large lattice distortions caused by the doped W6+ resulted in the shortening of BO bonds while an increase in the local displacement of B-site ions. Moreover, a mismatch occurred for the oxygen octahedral dimensions, and a subsequent disruption of the long-ranged ordered ferroelectric domains was observed, which resulted in the formation of microdomains. On the other hand, the changes in the concentration of oxygen vacancy defects induced by the Li and W doping inside the ceramic were comprehensively analyzed. The decrease in the concentration of oxygen vacancies was found to be accompanied by the enhancement of piezoelectric properties of the material. Excellent comprehensive performance (piezoelectric coefficient d33 = 655 pC N−1, Curie temperature Tc = 321.1 °C, dielectric constantεr = 3352.31, electromechanical coupling coefficient kp = 0.67, and residual polarization strength Pr = 55 μC cm−2) was obtained for 0.2 mol % doping amount of Li+ and W6+ ions. This work, therefore, proposes a novel strategy for the origin of piezoelectric properties and inspires doping of other heterovalent ions to improve the piezoelectric properties of ceramics. It further promotes the development of Pb-based piezoelectric ceramics for electromechanical devices that can efficiently operate under high-temperature environments.