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<p>Recent electrolyte solvent design based on ether-based has shown promise in enhancing cycling performance of Li-metal batteries. However, they inherently low oxidation potential (&lt;4.0 V) limits their application to high-voltage batteries. Here, we report an approach employing stepwise anion utilization from three Li salts in 1,2-dimethoxyethane (DME) solvent to enhance high-voltage stability. Through synergistic modulation with strongly coordinating lithium nitrate (LiNO<sub>3</sub>) and lithium difluorophosphate (LiPO<sub>2</sub>F<sub>2</sub>), the electrolyte forms a weakly solvating structure characterized by a low coordination number (CN) at a conventional Li salt concentration. Anion participation in the solvation sheath initiates a stepwise decomposition process (LiNO<sub>3</sub>→LiPO<sub>2</sub>F<sub>2</sub>→lithium bis(fluorosulfonyl)imide (LiFSI)) within the 4.0.4.5 V range, leading to the formation of an inorganic dual-layer CEI. This CEI suppresses DME decomposition at the interface and improves the high-voltage resistance of the electrolyte. This electrolyte exhibited superior performance compared to state-of-the-art electrolytes, enabling Li∥LiNi<sub>0.8</sub>-Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> cells to cycle stably for over 500 cycles with 80.35% capacity retention at 1 C at 2.8–4.3 V. Moreover, it enabled, for the first time, the operation of Li-rich cathode in Li∥Li<sub>1.14</sub>(Ni<sub>0.136</sub>Co<sub>0.136</sub>Mn<sub>0.542</sub>)O<sub>2</sub> cells cycling at 2.8–4.7 V using a single DME solvent electrolyte. This anion cooperative strategy effectively enhances the oxidation stability window of ether-based electrolytes while demonstrating practical application potential.</p>

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Anion engineering in a single ether solvent electrolyte enables a 4.7 V high-voltage lithium metal battery

  • 期刊论文

  • 发表日期：

    2025年7月14日

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  • Yifan Li,
  • Lipu Sun,
  • Nan Chen,
  • Mai Feng,
  • Boyao Li,
  • Feng Wu,
  • Yuejiao Li,
  • Renjie Chen

摘要

Recent electrolyte solvent design based on ether-based has shown promise in enhancing cycling performance of Li-metal batteries. However, they inherently low oxidation potential (<4.0 V) limits their application to high-voltage batteries. Here, we report an approach employing stepwise anion utilization from three Li salts in 1,2-dimethoxyethane (DME) solvent to enhance high-voltage stability. Through synergistic modulation with strongly coordinating lithium nitrate (LiNO3) and lithium difluorophosphate (LiPO2F2), the electrolyte forms a weakly solvating structure characterized by a low coordination number (CN) at a conventional Li salt concentration. Anion participation in the solvation sheath initiates a stepwise decomposition process (LiNO3→LiPO2F2→lithium bis(fluorosulfonyl)imide (LiFSI)) within the 4.0.4.5 V range, leading to the formation of an inorganic dual-layer CEI. This CEI suppresses DME decomposition at the interface and improves the high-voltage resistance of the electrolyte. This electrolyte exhibited superior performance compared to state-of-the-art electrolytes, enabling Li∥LiNi0.8-Co0.1Mn0.1O2 cells to cycle stably for over 500 cycles with 80.35% capacity retention at 1 C at 2.8–4.3 V. Moreover, it enabled, for the first time, the operation of Li-rich cathode in Li∥Li1.14(Ni0.136Co0.136Mn0.542)O2 cells cycling at 2.8–4.7 V using a single DME solvent electrolyte. This anion cooperative strategy effectively enhances the oxidation stability window of ether-based electrolytes while demonstrating practical application potential.