2D Raman correlation analysis of formation mechanism of passivating film on overcharged LiCoO2 electrode with additive system

•Effect of vinylene carbonate (VC) on the electrochemical performance of the LiCoO2 cathode.•Solid electrolyte interface (SEI) film formation on the LiCoO2 cathode under overcharge conditions.•Reduced capacity fading in VC-containing electrolyte.•Electrochemical reaction kinetics in cathode/electrolyte interface with and without VC.

The effect of vinylene carbonate (VC) as solid electrolyte interface (SEI)-forming additive on the electrochemical performance of the LiCoO2 cathode was investigated by galvanostatic charge–discharge testing as well as Raman and 2D correlation spectroscopy. It was found that VC-containing electrolyte has a positive effect on capacity fading. An analysis of the 2D Raman correlation spectra suggested that even though the same SEI components (i.e., Co3O4 and Li2O) are produced on the cathode surface, the electrochemical reaction kinetics in the cathode/electrolyte interface differ according to the non-use or use of VC: in the latter case, formation of the SEI components is delayed.

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