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<p>Relaxor ferroelectric ceramics are promising energy-storage candidates for high-power electronic systems owing to their high energy density and fast charge-discharge speed. However, achieving ultrahigh energy density still poses challenges due to the inherently inverted coupling relationship between polarization (<i>P</i>) and breakdown electric field (<i>E</i><sub>b</sub>). Here, we propose a high-entropy strategy to decouple polarization from breakdown electric field. The high-entropy design exerts a triple effect, which involves flattening electronic band to restrict the transport of charge carriers, driving the formation of core-shell heterostructure to suppress electrical breakdown, and stabilizing polymorphic polar phases to promote polarization rotation. The triple synergy effect led to an ultrahigh <i>E</i><sub>b</sub> and a maximized polarization disparity (Δ<i>P</i> = <i>P</i><sub>m</sub> - <i>P</i><sub>r</sub>). As a result, the high-entropy ceramics exhibit an ultrahigh recoverable energy density (<i>W</i><sub>rec</sub>) of 10.23 ± 0.99 J/cm<sup>3</sup> and a satisfactory efficiency (<i>η</i>) of 85.44% ± 3.34%, alongside good cycling reliability and temperature stability. This work provides an innovative design paradigm for achieving excellent energy storage performance of dielectric capacitors.</p>

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Electronic band and core-shell structure engineering enables ultrahigh energy storage in high-entropy ceramics

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月12日

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  • Yunting Li,
  • Peng Li,
  • Haihua Huang,
  • Hairui Bai,
  • Fei Xu,
  • Jigong Hao,
  • Peng Fu,
  • Juan Du,
  • Zhongbin Pan,
  • Wangfeng Bai,
  • Wei Li,
  • Jiwei Zhai,
  • Zhenxiang Cheng

摘要

Relaxor ferroelectric ceramics are promising energy-storage candidates for high-power electronic systems owing to their high energy density and fast charge-discharge speed. However, achieving ultrahigh energy density still poses challenges due to the inherently inverted coupling relationship between polarization (P) and breakdown electric field (Eb). Here, we propose a high-entropy strategy to decouple polarization from breakdown electric field. The high-entropy design exerts a triple effect, which involves flattening electronic band to restrict the transport of charge carriers, driving the formation of core-shell heterostructure to suppress electrical breakdown, and stabilizing polymorphic polar phases to promote polarization rotation. The triple synergy effect led to an ultrahigh Eb and a maximized polarization disparity (ΔP = Pm - Pr). As a result, the high-entropy ceramics exhibit an ultrahigh recoverable energy density (Wrec) of 10.23 ± 0.99 J/cm3 and a satisfactory efficiency (η) of 85.44% ± 3.34%, alongside good cycling reliability and temperature stability. This work provides an innovative design paradigm for achieving excellent energy storage performance of dielectric capacitors.