Fabrication of a lead-free ternary ceramic system for high energy storage applications in dielectric capacitors

The importance of electroceramics is well-recognized in applications of high energy storage density of dielectric ceramic capacitors. Despite the excellent properties, lead-free alternatives are highly desirous owing to their environmental friendliness for energy storage applications. Herein, we provide a facile synthesis of lead-free ferroelectric ceramic perovskite material demonstrating enhanced energy storage density. The ceramic material with a series of composition (1-z) (0.94Na_0.5Bi_0.5TiO₃-0.06BaTiO₃)-zNd_0.33NbO_3, denoted as NBT-BT-zNN, where, z = 0.00, 0.02, 0.04, 0.06, and 0.08 are synthesized by the conventional solid-state mix oxide route. Microphases, microstructures, and energy storage characteristics of the as-synthesized ceramic compositions were determined by advanced ceramic techniques. Powder X-ray diffraction analysis reveals pure single perovskite phases for z = 0 and 0.02, and secondary phases of Bi₂Ti₂O₇ appeared for z = 0.04 and 0.08. Furthermore, scanning electron microscopy analysis demonstrates packed-shaped microstructures with a reduced grain size for these ceramic compositions. The coercive field (E_c) and remnant polarization (P_r) deduced from polarization vs. electric field hysteresis loops determined using an LCR meter demonstrate decreasing trends with the increasing z content for each composition. Consequently, the maximum energy storage density of 3.2 J/cm³, the recoverable stored energy of 2.01 J/cm³, and the efficiency of 62.5% were obtained for the z content of 2 mol% at an applied electric field of 250 kV/cm. This work demonstrates important development in ceramic perovskite for high power energy storage density and efficiency in dielectric capacitors in high-temperature environments. The aforementioned method makes it feasible to modify a binary ceramic composition into a ternary system with highly enhanced energy storage characteristics by incorporating rare earth metals with transition metal oxides in appropriate proportions.