Carbon electrodes are widely used in a broad range of technologies including energy conversion, metals production, and analytical sensors. This research project, supported by the Analytical and Surface Chemistry Program, uses various Raman spectroscopic probes to obtain information about the structure of carbon electrode surfaces in various electrochemical environments. Resonance Raman spectroscopy of adsorbed probe molecules is used to examine specific surface sites. Unenhanced surface Raman spectroscopy is applied to the study of adsorbate overlayers on the carbon surface. This structural information is correlated with the activity and stability of these electrodes in various applications, including microanalytical methods applications. In order to understand the reactivity and stability of carbon electrodes widely used in electrochemical technologies, surface structural information is essential. Raman spectroscopic probing of the carbon electrode surface is the subject of this research project. The structural information obtained from these studies helps to design and modify electrodes for energy conversion and electrocatalytic and sensor applications.