Probing the electrode-solution interfaces in rechargeable batteries by sum-frequency generation spectroscopy.

An in-depth understanding of the electrode-electrolyte interaction and electrochemical reactions at the electrode-solution interfaces in rechargeable batteries is essential to develop novel electrolytes and electrode materials with high performance. In this perspective, we highlight the advantages of the interface-specific sum-frequency generation (SFG) spectroscopy on the studies of the electrode-solution interface for the Li-ion and Li-O batteries. The SFG studies in probing solvent adsorption structures and solid-electrolyte interphase formation for the Li-ion battery are briefly reviewed. Recent progress on the SFG study of the oxygen reaction mechanisms and stability of the electrolyte in the Li-O battery is also discussed. Finally, we present the current perspective and future directions in the SFG studies on the electrode-electrolyte interfaces toward providing deeper insight into the mechanisms of discharging/charging and parasitic reactions in novel rechargeable battery systems.