KCS

Li metal batteries (LMBs) are attractive candidates for future high-energy-density battery systems. To date, high-voltage LMBs suffer from severe limitations because the electrolytes are unstable against Li anodes and high-voltage cathodes. Although ether-based electrolytes exhibit good stability with the Li metal anode, compared to carbonate-based electrolytes, they have been used only in LMBs at ≤4.0 V because of their limited oxidation stability. In our previous study (Small 2022, 18, 2107492), we report a high concentration electrolyte (HCE) comprising lithium bis(fluorosulfonyl)imide (LiFSI) and a weakly solvating solvent (1,2-diethoxyethane; DEE), which can generate associated complexes at a relatively lower concentration compared to the reported HCEs. This is a follow-up to our previous study, which involves the theoretical investigation of the solvation structures and the transport mechanisms that govern the aforementioned electrolyte. For this purpose, we employ the use of molecular dynamics methods that explicitly include polarizability, to investigate the aforementioned electrolyte. The results of this study report the changes in solvation structures and the Li⁺ transport mechanism as the salt concentration increases.