<p>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.</p>

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

  • Tao Deng,
  • Jiyang Xie,
  • Zhen Liu,
  • Liqiang He,
  • Zhichao Hong,
  • Haonan Peng,
  • Dong Wang,
  • Cosme Milesi-Brault,
  • Teng Lu,
  • Yonghong Chen,
  • Zhisheng Lin,
  • Wanbiao Hu,
  • Brahim Dkhil,
  • Yun Liu,
  • Genshui Wang,
  • Junhao Chu

摘要

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-3 and high efficiency of 94.2% are obtained in our designed high-entropy Bi0.5Na0.5TiO3-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.