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<p>Recent electrolyte solvent design based on weakening lithium-ion solvation have shown promise in enhancing cycling performance of Li-metal batteries. However, they often face slow redox kinetics and poor cycling reversibility at high rate. Here we report using asymmetric solvent molecules substantially accelerates Li redox kinetics. Asymmetric ethers (1-ethoxy-2-methoxyethane, 1-methoxy-2-propoxyethane) showed higher exchange current densities and enhanced high-rate Li<sup>0</sup> plating/stripping reversibility compared to symmetric ethers. Adjusting fluorination levels further improved oxidative stability and Li<sup>0</sup> reversibility. The asymmetric 1-(2,2,2-trifluoro)-ethoxy-2-methoxyethane, with 2 M lithium bis(fluorosulfonyl)imide, exhibited high exchange current density, oxidative stability, compact solid–electrolyte interphase (~10 nm). This electrolyte exhibited superior performance among state-of-the-art electrolytes, enabling over 220 cycles in high-rate Li (50 μm)||LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811, 4.9 mAh cm<sup>−2</sup>) cells and for the first time over 600 cycles in anode-free Cu | |Ni95 pouch cells (200 mAh) under electric vertical take-off and landing cycling protocols. Our findings on asymmetric molecular design strategy points to a new pathway towards achieving fast redox kinetics for high-power Li-metal batteries.</p>

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Asymmetric ether solvents for high-rate lithium metal batteries

  • 期刊论文

  • 发表日期：

    2025年2月14日

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  • Il Rok Choi,
  • Yuelang Chen,
  • Aditya Shah,
  • Jacob Florian,
  • Chad Serrao,
  • John Holoubek,
  • Hao Lyu,
  • Elizabeth Zhang,
  • Jun Ho Lee,
  • Yangju Lin,
  • Sang Cheol Kim,
  • Hyunchang Park,
  • Pu Zhang,
  • Junyoung Lee,
  • Jian Qin,
  • Yi Cui,
  • Zhenan Bao

摘要

Recent electrolyte solvent design based on weakening lithium-ion solvation have shown promise in enhancing cycling performance of Li-metal batteries. However, they often face slow redox kinetics and poor cycling reversibility at high rate. Here we report using asymmetric solvent molecules substantially accelerates Li redox kinetics. Asymmetric ethers (1-ethoxy-2-methoxyethane, 1-methoxy-2-propoxyethane) showed higher exchange current densities and enhanced high-rate Li0 plating/stripping reversibility compared to symmetric ethers. Adjusting fluorination levels further improved oxidative stability and Li0 reversibility. The asymmetric 1-(2,2,2-trifluoro)-ethoxy-2-methoxyethane, with 2 M lithium bis(fluorosulfonyl)imide, exhibited high exchange current density, oxidative stability, compact solid–electrolyte interphase (~10 nm). This electrolyte exhibited superior performance among state-of-the-art electrolytes, enabling over 220 cycles in high-rate Li (50 μm)||LiNi0.8Mn0.1Co0.1O2 (NMC811, 4.9 mAh cm−2) cells and for the first time over 600 cycles in anode-free Cu | |Ni95 pouch cells (200 mAh) under electric vertical take-off and landing cycling protocols. Our findings on asymmetric molecular design strategy points to a new pathway towards achieving fast redox kinetics for high-power Li-metal batteries.