<p>Tetragonal tungsten bronze (TTB) ceramics have emerged as promising candidates for dielectric energy storage due to their intrinsic multi-site architectures. However, the limited energy storage performance achieved so far remains insufficient for advanced electronic and pulsed power applications. Here, we propose a targeted polar-entropy regulation strategy via minor multi-element substitution at the polar-active B-sites, enabling precise modulation of polar displacements and weakened coupling among polar nanoregions. Atomic-scale characterization reveals site-dependent structural responses, which collectively reshape local polarization configurations and dipolar correlations. As a result, we demonstrate the feasibility of TTB ceramics for state-of-the-art multilayer energy-storage device applications, achieving an outstanding recoverable energy density (<i>W</i><sub>rec</sub>) of 17.6 J·cm<sup>−3</sup> with a high efficiency of 96.8%, corresponding to a high figure of merit (<i>W</i><sub>F</sub>) of 550. Moreover, excellent thermal stability (Δ<i>W</i><sub>rec</sub> ≤ 2.0%) is achieved, and a highest <i>W</i><sub>rec</sub> of 15.0 J·cm<sup>−3</sup> is maintained over a wide temperature range (−40 to 125 °C). This work offers new insights into polarization regulation and provides an effective pathway for developing high-performance energy storage dielectric capacitors.</p>

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Targeted polar entropy regulation enables superior energy-storage in tungsten bronze multilayer capacitors

  • Haonan Peng,
  • Jiyang Xie,
  • Jiaqi Li,
  • Teng Lu,
  • Lingling Wei,
  • Wanbiao Hu,
  • Yun Liu,
  • Zhen Liu,
  • Genshui Wang

摘要

Tetragonal tungsten bronze (TTB) ceramics have emerged as promising candidates for dielectric energy storage due to their intrinsic multi-site architectures. However, the limited energy storage performance achieved so far remains insufficient for advanced electronic and pulsed power applications. Here, we propose a targeted polar-entropy regulation strategy via minor multi-element substitution at the polar-active B-sites, enabling precise modulation of polar displacements and weakened coupling among polar nanoregions. Atomic-scale characterization reveals site-dependent structural responses, which collectively reshape local polarization configurations and dipolar correlations. As a result, we demonstrate the feasibility of TTB ceramics for state-of-the-art multilayer energy-storage device applications, achieving an outstanding recoverable energy density (Wrec) of 17.6 J·cm−3 with a high efficiency of 96.8%, corresponding to a high figure of merit (WF) of 550. Moreover, excellent thermal stability (ΔWrec ≤ 2.0%) is achieved, and a highest Wrec of 15.0 J·cm−3 is maintained over a wide temperature range (−40 to 125 °C). This work offers new insights into polarization regulation and provides an effective pathway for developing high-performance energy storage dielectric capacitors.