Establishing a Relationship between the Piezoelectric Response and Oxygen Vacancies in Lead-Free Piezoelectrics

BiFeO₃-BaTiO₃ (BF-BT)-based lead-free piezoceramics are desired materials for high-temperature applications of piezoelectric sensors with a high Curie temperature and good piezoelectric properties. Recent studies have shown that oxygen vacancies have a significant effect on electrostrain and piezoelectric properties. Interestingly, two different phenomena exist, i.e., the increase in piezoelectric properties is often associated with a decrease in the concentration of oxygen vacancies, while the increase in electrostrain is often associated with an increase in the concentration of oxygen vacancies. Especially, for BF-based ceramics, the physical mechanisms related to property differences caused by oxygen vacancies are rarely reported, which needs further exploration. Here, two ceramics with differences in their oxygen vacancy concentrations are designed. Based on Rayleigh analysis, thermal/electric field-induced domain response (ferroelectric scaling), and macro-microstructural characterization, we can conclude that the transient piezoelectric response and the aging process are significantly affected by the oxygen vacancy concentration. In other words, the increasing concentration of oxygen vacancies in BF-BT ceramics enhances the reversible piezoelectric response contributed by lattice distortion and strengthens the response of domain switching and domain wall motion to electric and thermal fields but deteriorates their aging behavior, which leads to the degradation of piezoelectric performance. Besides, polarization saturation and defect pegging significantly improve the temperature stability of the strain.