The development of advanced liquid electrolytes for high-voltage/high-energy rechargeable Li metal batteries is an important strategy to attain an effective protective surface film on both the Li metal anode and the high-voltage composite cathode. Herein, we report a study of two CF-substituted ethylene carbonates as components of the electrolyte solutions for Li metal|NCM811 cells. We evaluated trifluoromethyl ethylene carbonate (CF-EC) and trans-ditrifluoromethylethylene carbonate Di-(CF)-EC as cosolvents and additives to the electrolyte solutions. Using CF-substituted ethylene carbonates as additives to a fluoroethylene carbonate (FEC)-based electrolyte solution enables improved capacity retention of high-power Li metal|NCM811 cells. The composition of the products from the transformations of CF-EC and Di-(CF)-EC in Li|NCM811 cells was studied by FTIR, XPS, and F NMR spectroscopy. We concluded that fluorinated Li alkyl carbonates are the main reaction products formed from these cyclic carbonates during the cycling of Li|NCM 811 cells, and fragmentation of the ring with the formation of CO, CO, or olefins is not characteristic of CF-substituted ethylene carbonates. The NCM 811 cathodes and Li metal anodes were characterized by X-ray diffraction, SEM, XPS, and FTIR spectroscopy. The role of CF-substituted ethylene carbonate additives in stabilizing high energy density secondary batteries based on Li metal anodes was discussed. A bright horizon for developing sustainable rechargeable batteries with the highest possible energy density is demonstrated.

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http://dx.doi.org/10.1021/acsami.4c08870DOI Listing

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