Relaxor behavior and energy storage density induced by B-sites substitutions in (Ca0.28Ba0.72)2.1Na0.8Nb5O15 Tungsten bronze ceramics

Lead-free relaxor ferroelectrics (Ca0.28Ba0.72)2.1Na0.8Nb5-xSbxO15 (CBNNS) and (Ca0.28Ba0.72)2.1Na0.8Nb5-yTayO15 (CBNNT) with tungsten bronze structure were fabricated via solid-state reactions. The obtained CBNNS and CBNNT ceramics showed different dielectric behaviors. Only the CBNNS ceramics revealed an intensified diffusion and relaxor-like characteristics, which could be verified by the modified Curie-Weiss law. The relaxor behaviors in CBNNS were attributed to the radii difference between Sb5+ and Nb5+ ions co-occupying in B-sites. For the substitution of Nb5+ by Sb5+ in CBNNS ceramics, the change from macroscopic polarization to local polarization could also give rise to the obvious relaxor behavior. The Raman spectra verified a larger off-centering of the cation and a higher distortion degree for BO6 octahedron in the ab plane for CBNNS ceramics when compared with those of CBNNT. In addition, the ferroelectric properties of CBNNS ceramics further indicated the relaxor ferroelectric nature, and also confirmed that the relaxor behavior helped to improve the energy-storage performance.