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<p>Charge transfer across interfaces constitutes the rate-determining step in electrochemical systems. Sluggish kinetics triggers side reactions and hazardous surface morphologies, as represented by dendritic/dead lithium (Li<sup>0</sup>) in Li-metal batteries (LMBs), especially under ultrafast charging (UFC). Here we report an approach to accelerate interfacial charge transfer by redesigning the solvent molecular structure into a distinctive planar coordination of lone-pair electrons (LPEs) with alkaline cations (Li<sup>+</sup> or Na<sup>+</sup>). This planar-aligned electron channel (PAEC) greatly strengthens the coupling between LPEs and Li<sup>+</sup>, promoting Li<sup>+</sup>/Li<sup>0</sup> redox reaction kinetics and reversibility. The designed electrolyte dramatically enables stable cycling of industrial 2 Ah Li||LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> pouch cells at an ultrahigh rate of 4 C, achieving 100% full charge within 15 min at a charging power density of 1,747.6 W kg<sup>−1</sup>. We establish a link between the solvation electronic structure and charge-transfer dynamics, highlighting a potential strategy for electrolyte design under extreme electrochemical conditions.</p>

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Molecularly aligned electron channels for ultrafast-charging practical lithium-metal batteries

  • 期刊论文

  • 发表日期：

    2026年1月23日

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  • Digen Ruan,
  • Shunqiang Chen,
  • Jiasen Guo,
  • Dazhuang Wang,
  • Weiduo Zhu,
  • Bing Huang,
  • Yuan Li,
  • Jun Ma,
  • Zhihao Ma,
  • Zihong Wang,
  • Zhongliang Zhu,
  • Ruiguo Cao,
  • Shuhong Jiao,
  • Yiying Wu,
  • Kang Xu,
  • Xiaodi Ren

摘要

Charge transfer across interfaces constitutes the rate-determining step in electrochemical systems. Sluggish kinetics triggers side reactions and hazardous surface morphologies, as represented by dendritic/dead lithium (Li0) in Li-metal batteries (LMBs), especially under ultrafast charging (UFC). Here we report an approach to accelerate interfacial charge transfer by redesigning the solvent molecular structure into a distinctive planar coordination of lone-pair electrons (LPEs) with alkaline cations (Li+ or Na+). This planar-aligned electron channel (PAEC) greatly strengthens the coupling between LPEs and Li+, promoting Li+/Li0 redox reaction kinetics and reversibility. The designed electrolyte dramatically enables stable cycling of industrial 2 Ah Li||LiNi0.8Mn0.1Co0.1O2 pouch cells at an ultrahigh rate of 4 C, achieving 100% full charge within 15 min at a charging power density of 1,747.6 W kg−1. We establish a link between the solvation electronic structure and charge-transfer dynamics, highlighting a potential strategy for electrolyte design under extreme electrochemical conditions.