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Non-fluorinated non-solvating cosolvent enabling superior performance of lithium metal negative electrode battery

Author

Listed:
  • Junyeob Moon

    (Seoul National University)

  • Dong Ok Kim

    (Seoul National University
    Swarthmore College)

  • Lieven Bekaert

    (Vrije Universiteit Brussel, Research Group Electrochemical and Surface Engineering)

  • Munsoo Song

    (Seoul National University)

  • Jinkyu Chung

    (Seoul National University)

  • Danwon Lee

    (Seoul National University)

  • Annick Hubin

    (Vrije Universiteit Brussel, Research Group Electrochemical and Surface Engineering)

  • Jongwoo Lim

    (Seoul National University
    Seoul National University)

Abstract

The growth of dendrites on lithium metal electrodes is problematic because it causes irreversible capacity loss and safety hazards. Localised high-concentration electrolytes (LHCEs) can form a mechanically stable solid-electrolyte interphase and prevent uneven growth of lithium metal. However, the optimal physicochemical properties of LHCEs have not been clearly determined which limits the choice to fluorinated non-solvating cosolvents (FNSCs). Also, FNSCs in LHCEs raise environmental concerns, are costly, and may cause low cathodic stability owing to their low lowest unoccupied molecular orbital level, leading to unsatisfactory cycle life. Here, we spectroscopically measured the Li+ solvation ability and miscibility of candidate non-fluorinated non-solvating cosolvents (NFNSCs) and identified the suitable physicochemical properties for non-solvating cosolvents. Using our design principle, we proposed NFNSCs that deliver a coulombic efficiency up to 99.0% over 1400 cycles. NMR spectra revealed that the designed NFNSCs were highly stable in electrolytes during extended cycles. In addition, solvation structure analysis by Raman spectroscopy and theoretical calculation of Li+ binding energy suggested that the low ability of these NFNSCs to solvate Li+ originates from the aromatic ring that allows delocalisation of electron pairs on the oxygen atom.

Suggested Citation

  • Junyeob Moon & Dong Ok Kim & Lieven Bekaert & Munsoo Song & Jinkyu Chung & Danwon Lee & Annick Hubin & Jongwoo Lim, 2022. "Non-fluorinated non-solvating cosolvent enabling superior performance of lithium metal negative electrode battery," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32192-5
    DOI: 10.1038/s41467-022-32192-5
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