Inorganic/organic composite fluorinated interphase layers for stabilizing ether-based electrolyte in high-voltage lithium metal batteries
JOURNAL OF MATERIALS CHEMISTRY A(2024)
Abstract
Despite their superior reduction stability to Li metal compared with conventional carbonate electrolytes, ethers have been precluded from use in high-voltage batteries due to their limited oxidation stability (<4 V). Herein, this issue can be effectively addressed by the synergistic effect strategy based on dual salt and fluoroethylene carbonate (FEC) as a co-solvent, which forms a unique Li+ solvation structure with aggregated dual anions and induces more robust inorganic/organic composite fluorinated interphase layers. It is noted that this ether-based electrolyte presents an enlarged electrochemical window up to 4.6 V resulting from the enhanced oxidative stability by introducing FEC. Meanwhile, the interphase layers effectively improve the Li plating/stripping kinetics and interface stability. Besides, in situ FTIR, Raman spectra and theoretical calculations are used to confirm the solvation interactions. And the inorganic/organic composite fluorinated interphase layer component is verified by X-ray photoelectron spectroscopy (XPS) spectra. Using this ether-based electrolyte, the Li/Cu cells present colossal Li deposits with a high coulombic efficiency (approximate to 98.95%). More significantly, the 4.4 V Li/LiCoO2 battery exhibits excellent cycling stability with a capacity retention of 80% over 300 cycles. This work offers a promising approach to enable ether-based electrolytes for high-voltage Li metal batteries (LMBs).
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