Giant piezoelectricity, rhombohedral-orthorhombic-tetragonal phase coexistence and domain configurations of (K,Na)(Nb,Sb)O3–BiFeO3–(Bi, Na)ZrO3 ceramics

Abstract Research on lead-free piezoelectric ceramics has been an important subject in recent years due to increasingly strong environmental concerns. In this paper, we report the piezoelectric performance, phase transitions and domain structure for a series of dense (0.994-x)(K0.40Na0.60)(Nb0.955Sb0.045)O3–0.006BiFeO3–x(Bi0.50Na0.50)ZrO3 ceramics prepared by two step-sintering through solid-state reaction. Among these ceramics, the one with x = 0.03 shows a giant piezoelectricity with remarkably high piezoelectric coefficient d33 of 550 pC/N at room temperature. Concurrent measurements of e′ and e′′ vs. temperature dependences and X-ray diffraction analysis showed that ceramics with x ≤ 0.04 are in rhombohedral-orthorhombic-tetragonal (R-O-T) phase coexistence at room temperature. More intriguingly, the rhombohedral-orthorhombic phase transition temperature, TR-O, is almost independent of the (Bi0.50Na0.50)ZrO3 content, while orthorhombic-tetragonal phase transition temperature, T O-T, decreases largely with increasing the (Bi0.50Na0.50)ZrO3 content. Domain configurations of the ceramic with x = 0.03 were investigated by acid-etching. Complicated domain patterns consisting of watermark-shaped domains of long parallel stripes separated by irregularly shaped boundaries are seen before poling. In contrast, relatively simple domain patterns of long parallel stripes with some nanodomains appearing in a part of broad stripes are observed after poling. The obtained excellent piezoelectric properties are ascribed to the R-O-T phase coexistence and the corresponding characteristic domain structure.