Operando Spectroscopy-Inspired Design of Electrochemical Interface

The quest to design active and stable electrochemical interface hinges on unequivocally identifying the active site(s) and reaction mechanism under realistic operating conditions. This comprehensive paper summarizes the most recent understanding of the electrochemical interface during energy conversion and storage reactions probed by operando surface-enhanced infrared spectroscopy (SEIRAS), operando attenuated total reflection infrared spectroscopy (ATR-IR), and operando synchrotron surface X-ray scattering, coupled with density functional theory (DFT) calculations. The paper also demonstrates that the holistic information about the complex interaction in the electrochemical interface can alter the reaction energetics/kinetics in a way incapable of electrode-centered design strategy. This work shed light on the significance of advanced operando techniques to accelerate the design of electrochemical interfaces by providing additional knobs to tune the reaction energetics/kinetics, leading further improvements in electrocatalytic activity for energy conversion and storage reactions.