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<p>The reliability of lithium metal anodes (LMAs) has long been challenged by dendrite-induced short circuits and an unstable solid electrolyte interphase (SEI). Herein, an organic–inorganic hybrid dual-layer artificial SEI (ASEI) is strategically engineered based on a facile and scalable roll-pressing technique, significantly enhancing the long-term performance of lithium metal batteries (LMBs) under high current densities. Internally, the <i>in-situ</i> formed LiF-rich layer facilitates lithium-ion transport by lowering diffusion barriers and provides robust mechanical integrity to suppress dendrite penetration. Complementarity, the outer organic PFOE layer plays a critical role in chemically stabilizing the interface by resisting electrolyte oxidation and minimizing electrolyte depletion. As a result, symmetric cells with PFOE-LiF@Li anodes exhibit exceptional cycling stability in Li plating/stripping cycles for over 1400 h under harsh conditions of 30 mA cm<sup>−2</sup> and 5 mAh cm<sup>−2</sup>, outperforming most previously reported ASEI systems. Furthermore, full cells assembled with the LiFePO<sub>4</sub> cathodes demonstrate excellent capacity retention and Coulombic efficiency, sustaining 350 cycles at 1 C and over 550 cycles at 2 C. This work establishes a broadly applicable design principle for interfacial engineering by uniting the mechanical rigidity of inorganic components with the chemical functionality of organic layers, offering a promising pathway toward the practical commercialization of LMBs.</p>

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Dual-layered organo-fluorinated hetero-interphase: a robust shield for ultra-stable lithium metal batteries

  • 期刊论文

  • 发表日期：

    2026年5月26日

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  • Dachao Du,
  • Junhao Chen,
  • Hengfeng Hong,
  • Xipin Zhang,
  • Haijiang Qiu,
  • Yuewen Dai,
  • Yuhang Liang,
  • Yuanhui Zheng

摘要

The reliability of lithium metal anodes (LMAs) has long been challenged by dendrite-induced short circuits and an unstable solid electrolyte interphase (SEI). Herein, an organic–inorganic hybrid dual-layer artificial SEI (ASEI) is strategically engineered based on a facile and scalable roll-pressing technique, significantly enhancing the long-term performance of lithium metal batteries (LMBs) under high current densities. Internally, the in-situ formed LiF-rich layer facilitates lithium-ion transport by lowering diffusion barriers and provides robust mechanical integrity to suppress dendrite penetration. Complementarity, the outer organic PFOE layer plays a critical role in chemically stabilizing the interface by resisting electrolyte oxidation and minimizing electrolyte depletion. As a result, symmetric cells with PFOE-LiF@Li anodes exhibit exceptional cycling stability in Li plating/stripping cycles for over 1400 h under harsh conditions of 30 mA cm−2 and 5 mAh cm−2, outperforming most previously reported ASEI systems. Furthermore, full cells assembled with the LiFePO4 cathodes demonstrate excellent capacity retention and Coulombic efficiency, sustaining 350 cycles at 1 C and over 550 cycles at 2 C. This work establishes a broadly applicable design principle for interfacial engineering by uniting the mechanical rigidity of inorganic components with the chemical functionality of organic layers, offering a promising pathway toward the practical commercialization of LMBs.