Superior energy storage performance via engineering crossover region with competing orders in high-entropy multilayer capacitors.

Deng, Tao; Xie, Jiyang; Liu, Zhen; He, Liqiang; Hong, Zhichao; Peng, Haonan; Wang, Dong; Milesi-Brault, Cosme et al. · Nat Commun · 2026

basic_science · Level V

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Abstract

As promising candidates for next-generation energy storage devices in electrical and electronic systems, lead-free multilayer ceramic capacitors face increasingly high performance requirements. To counteract the usual trade-off between energy storage density and efficiency, we here propose a high-entropy design that directly harnesses diverse oxide symmetries to targetedly engineer competing orders and tune the composition into the crossover region between relaxor ferroelectric and superparaelectric states. Atomic-scale structural analysis reveals high-entropy ceramic develops pronounced local polarization fluctuation and dispersed oxygen octahedral rotations, which enhance relaxor behavior and reduce switching barrier. Consequently, superior recoverable energy density of 20.64 J cm<sup>-3</sup> and high efficiency of 94.2% are obtained in our designed high-entropy Bi<sub>0.5</sub>Na<sub>0.5</sub>TiO<sub>3</sub>-based multilayer ceramic capacitors, along with excellent thermal/anti-fatigue stability and charge-discharge capabilities. This work provides a transferable strategy to engineer competing orders in lead-free dielectric materials and successfully achieves high-entropy multilayer ceramic capacitors with superior energy storage performance.