High-Performance Energy Storage in Ba(Al0.5Nb0.5)O3-Modified (Bi0.5Na0.5)TiO3-Based Lead-Free Ceramics via High-Entropy Strategy

Lead-free dielectric capacitors are widely utilized in high-power pulse devices due to their outstanding power density, rapid charging-discharging speed, and environmental friendliness. However, there are still challenges in further improving their energy storage performance. Recently, a high-entropy strategy has received widespread attention to obtain high-performance dielectric capacitors. In this work, Ba(Al0.5Nb0.5)O3 (BAN) was introduced into lead-free (Bi0.5Na0.5)TiO3-based ceramics to increase configuration entropy and chemical disorder, exploiting a synergistic high-entropy strategy to optimize the energy storage characteristics. Remarkably, superior energy storage density (Wrec ∼7.40 J/cm3) and efficiency (η ∼85.5%) at a great electric breakdown strength (Eb ∼547 kV/cm) are achieved in 0.85(0.6(Bi0.5Na0.5)TiO3-0.4(Sr0.7Bi0.2)TiO3)-0.15BAN high-entropy ceramic. The integration of BAN boosts the increase of entropy and induces grain refinement, strengthened relaxation behavior, formation of polar nanoregions, and a widened band gap, leading to reduced Pr and improved Eb as well as excellent energy storage performance. Moreover, good thermal stability, frequency stability, and charge-discharge performance are also realized. This study confirms that high-entropy engineering is a feasible route to realize high-performance energy storage, providing prospective lead-free dielectric materials for practical applications.