Effect of antimony substitution for niobium on the crystal structure, piezoelectric and dielectric properties of (K0.5Na0.5)NbO3 ceramics

The effect of antimony (Sb) substitution for niobium (Nb) on potassium sodium niobate (KNN) ceramic was investigated with respect to the densification behaviour at different sintering temperatures, microstructure and electrical properties. A small amount of Sb5+ was added while simultaneously lowering the amount of Nb5+ and in this study of the (K0.5Na0.5)(Nb1-xSbx)O3 system, x content was varied from 0 to 14 mol%.

Our results show that Sb5+ slightly increased the optimum sintering temperature for KNN but above 8 mol%, its resistivity and piezoelectric properties decreased. As the amount of Sb5+ substituted is increased, the structure of the ceramic transformed from orthorhombic to pseudo-cubic which led to slight shrinkage in the unit cell volume.

Microstructural examination revealed that above 10 mol%, a second phase (K2NaSb3O9) was formed which segregated mainly to the grain boundary while the quantitative EDX analysis showed that there was A-site vacancy due to loss of the alkali elements. The two phase transitions points, Curie temperature (TC) and the tetragonal to orthorhombic (TT-O) shifted to lower temperature with increasing Sb5+ content and above 10 mol%, the TT-O shifted to below room temperature.

The dielectric loss slightly increases with increasing Sb5+ content up to 200°C. There was an improvement in the piezoelectric properties with ≤ 6 mol% Sb content while optimum properties were obtained with 4 mol% (KP = 0.46, Qm = 6.2, NP = 2296).