This paper investigates 0.69BiFeO3-0.31BaTiO3+x(0.8Bi0.5Na0.5TiO3-0.2Bi0.5K0.5TiO3) (abbreviated as 0.69BF-0.31BT+x(0.8BNT-0.2BKT) (0≤x≤0.025) quaternary high-temperature lead-free piezoelectric ceramics. X-ray diffraction(XRD) analysis reveals that these ceramics exhibit morphotropic phase boundaries (MPB) with coexistence of rhombohedral (R) and pseudo-cubic (Pc) phases. The in-situ d33 measurements indicate that 0.69BF-0.31BT+x(0.8BNT-0.2BKT) possesses excellent thermal stability, achieving an in-situ d33 of 687 pC/N at Tdr = 382℃, and a high Curie temperature (Tc = 474℃). Transmission electron microscopy (TEM) results show that the high depolarization temperature (Tdr) and excellent piezoelectric properties are attributed to compositional inhomogeneity introduced by the incorporation of double relaxation ferroelectrics (0.8BNT-0.2BKT), resulting in the formation of polar nanoregions (PNRs). This design demonstrates that the quaternary system of BF-BT+(BNT-BKT)-based ceramics serves as a promising example for optimizing high-temperature lead-free piezoelectric ceramics.
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