Publication date: 21st July 2025
A key step towards the development of Li-ion batteries with increased charging rates, durabilities and capacities is the development of suitable liquid (or solid) state battery electrolytes. However, designing battery electrolytes with the requisite solvation and electrochemical properties has remained extremely challenging due to an inability to build detailed relationships between the electrolyte performance and internal structure of the (liquid) electrolyte.
Here, we present preliminary experiments using single-beam 2D Raman spectroscopy to probe the internal structure of a prototypical LiTFSI-water electrolyte, that could be used in e.g., aqueous Zn-ion battery cells. Our approach, which allows measurement of the coupling between low energy vibrational modes, nullifies unwanted cascade signals that have previously hindered (time domain) 2D Raman spectroscopy approaches. Interestingly we observe strong intermolecular coupling between water libration modes and an SO stretch mode in LiTFSI, that varies with electrolyte concentration. Further work using molecular dynamics simulations and on more complex ternary electrolytes is ongoing, but our work points towards the power of 2D Raman for characterising the internal structure of battery electrolyte systems.
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