Structure and temperature-dependent phase transitions of lead-free Bi1/2Na1/2TiO3-Bi1/2K1/2TiO3-K0.5Na0.5NbO3 piezoceramics

Abstract

Structure and phase transitions of (1 - y)((1 - x)Bi1/2Na1/2TiO3-xBi(1/2)K(1/2)TiO(3))-yK(0.5)Na(0.5)NbO(3) (x; y) piezoceramics (0.1 <= x <= 0.4; 0 <= y <= 0.05) were investigated by transmission electron microscopy, neutron diffraction, temperature-dependent x-ray diffraction, and Raman spectroscopy. The local crystallographic structure at room temperature (RT) does not change by adding K0.5Na0.5NbO3 to Bi1/2Na1/2TiO3-xBi(1/2)K(1/2)TiO(3) for x = 0.2 and 0.4. The average crystal structure and microstructure on the other hand develop from mainly long-range polar order with ferroelectric domains to short-range order with polar nanoregions displaying a more pronounced relaxor character. The (0.1; 0) and (0.1; 0.02) compositions exhibit monoclinic Cc space group symmetry, which transform into Cc + P4bm at 185 and 130 degrees C, respectively. This high temperature phase is stable at RT for the morphotropic phase boundary compositions of (0.1; 0.05) and all compositions with x = 0.2. For the compositions of (0.1; 0) and (0.1; 0.02), local structural changes on heating are evidenced by Raman; for all other compositions, changes in the long-range average crystal structure were observed.