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<p>Proton conduction in hydrogen-bond-rich protic electrolytes enables fast mass and charge transport, crucial for electrochemical energy storage and power conversion. Such transport can give proton-based batteries exceptional rate capability and low-temperature operation beyond other working ions. Here we show that in phosphoric acid (H<sub>3</sub>PO<sub>4</sub>) electrolytes, vehicular and structural proton transport coexist, and their contributions to conductivity can be quantitatively distinguished. We link structural diffusion directly to hydrogen-bond strength, enabling the precise tuning of proton migration. Guided by this, we reveal a double conductivity peak from regulated structural diffusion. The optimal electrolyte (5.8-M H<sub>3</sub>PO<sub>4</sub>) achieves high overall (232.9 mS cm<sup>−1</sup>) and structural (164.9 mS cm<sup>−1</sup>) conductivity. A MoO<sub>3</sub>‖CuFe-TBA battery with this electrolyte outperforms a deep-eutectic benchmark (8.3-M H<sub>3</sub>PO<sub>4</sub>), delivering &gt;17,474 W kg<sup>−1</sup> at room temperature and retaining 15.1 Wh kg<sup>−1</sup> at −75 °C. These findings provide a framework for designing advanced protic electrolytes across electrochemical systems.</p>

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Quantitative and mechanistic insights into proton dynamics for fast energy storage

  • 期刊论文

  • 发表日期：

    2025年10月3日

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  • Ziyue Li,
  • Yuxiao Lin,
  • Mounesha N. Garaga,
  • Steven G. Greenbaum,
  • Mochou Liao,
  • Jiafeng Ruan,
  • Qin Li,
  • Yunsong Li,
  • Dalin Sun,
  • Kang Xu,
  • Fang Fang,
  • Fei Wang

摘要

Proton conduction in hydrogen-bond-rich protic electrolytes enables fast mass and charge transport, crucial for electrochemical energy storage and power conversion. Such transport can give proton-based batteries exceptional rate capability and low-temperature operation beyond other working ions. Here we show that in phosphoric acid (H3PO4) electrolytes, vehicular and structural proton transport coexist, and their contributions to conductivity can be quantitatively distinguished. We link structural diffusion directly to hydrogen-bond strength, enabling the precise tuning of proton migration. Guided by this, we reveal a double conductivity peak from regulated structural diffusion. The optimal electrolyte (5.8-M H3PO4) achieves high overall (232.9 mS cm−1) and structural (164.9 mS cm−1) conductivity. A MoO3‖CuFe-TBA battery with this electrolyte outperforms a deep-eutectic benchmark (8.3-M H3PO4), delivering >17,474 W kg−1 at room temperature and retaining 15.1 Wh kg−1 at −75 °C. These findings provide a framework for designing advanced protic electrolytes across electrochemical systems.