Structural phase coexistence enhances the energy storage density of (Bi0.5Na0.5)0.8Ba0.2Ti1-ySnyO3 lead-free ceramics

Abstract

In the present study, BaSnO3 was introduced into polycrystalline NBT-BT ferroelectric ceramics and conducted a comprehensive investigation into the structural, dielectric, ferroelectric, and energy storage characteristics of the (Bi0.5Na0.5)0.8Ba0.2Ti1-ySnyO3 (BNBTS) ceramics. The coexistence of structural phases P4mm and Amm2 was observed through Rietveld refinement and also confirmed by Raman analysis. The formation energy decreases with an increase in substitution concentration favouring the formation of the orthorhombic phase. The SEM analysis revealed a denser microstructure characterised by smaller grain sizes, which favourably enhances energy storage density. Furthermore, Raman spectroscopic analysis unveiled a softening of Ti–O bonds, indicating the emergence of macroscopic relaxor behaviour. Dielectric studies provided evidence of a transition from ferroelectric to relaxor behaviour, an observation further confirmed by P-E loop measurements. This transition can be linked to the partial substitution of Sn4+ ions for Ti4+ ions, disrupting the ferroelectric long-range order within the matrix phase. Notably, the polarization-electric field (P-E) loop of BNBTS2 ceramics exhibited a substantial value of polarization (Ps) 30 μC/cm2 with a reduced value of remnant polarization (Pr) 2.29 μC/cm2. These characteristics contributed to the achievement of higher energy recovery (Wrec) and lower energy loss (Wloss) values, measuring 1.184 J/cm3 and 0.142 J/cm3, respectively, with a notable efficiency of 88.8%. Consequently, the system of ternary ceramics demonstrates promise as a potential option for energy storage ceramics among NBT-BT-based materials.