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

Junyeob Moon, Dong Ok Kim, Lieven Bekaert, Munsoo Song, Jinkyu Chung, Danwon Lee, Annick Hubin () and Jongwoo Lim ()
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Junyeob Moon: Seoul National University
Dong Ok Kim: Seoul National University
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

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-32192-5

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