An A-Site Equimolar High-Entropy Strategy Induced a High Weakly Coupled Relaxor Phase and Enhancement of Energy Storage Properties in Perovskite Ceramics Based on Nd3+
摘要
High configurational entropy (ΔS) in dielectric ceramics is promising for high-power pulse applications. However, their low recoverable energy storage density (Wrec) and low breakdown strength (Eb) remain major challenges for achieving superior energy storage performance. Herein, three different systems were investigated on the basis of low-entropy (Na0.5Bi0.5)TiO3 (NBT, ΔS = 0.69R), medium-entropy (Na0.3Bi0.3Sr0.3Ba0.1)TiO3 (NBBST, ΔS = 1.31R), and high-entropy (Bi0.2Na0.2Nd0.2K0.2Ba0.2)TiO3 (NNBBKT, ΔS = 1.61R) ceramics, derived from the NBT system, to disrupt their long-range ferroelectric order via A-site cation disorder. The results revealed that the high-entropy ceramic significantly induced a weakly coupled relaxor phase along with suppression of remnant polarization, leading to a remarkable increase in breakdown strength. The elevation of grain resistance (Rg) at high entropy caused a mismatch between grain and grain boundary resistance (Rgb), resulting in the pinching of interfacial polarization. These cascade effects achieved a high Wrec of 6.2 J/cm3 with a large conversion efficiency (ƞ) of 92.8% at an ultra-high Eb of ~500 kV/cm in the high-entropy NNBBKT ceramic. The present work demonstrates that high entropy and the suppression of interfacial polarization are promising strategies for enhancing the energy storage performance of dielectric ceramics.