The rational design of electrochemical devices depends on the molecular understanding of the reaction processes under realistic working conditions. To gain insights into molecular adsorption/desorption on solid-liquid interfaces, highly sensitive in-situ molecular detection methods and the ability of controlling the Fermi level are required. In-operando surface-enhanced Raman scattering (EC-SERS) entails both requisites, but is diffraction limited. In contrast, electrochemical tip-enhanced Raman scattering (EC-TERS) offers unprecedented nanoscale chemical resolution of electrified solid-liquid interfaces. Here, we employ both tools, EC-SERS and EC-TERS, to study the Au oxidation/reduction, which represents a fundamental reaction for a wealth of electrochemical/electrocatalytic processes.
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