The senior author and his collaborators have long been concerned with the use of analytical chemical techniques – more specifically, experimental approaches and methodologies primarily based on polarography – to study problems of general chemical interest. Currently, electroanalytical approaches are being used in a systematic investigation of chemical phenomena involving biologically significant compounds, where such approaches seem to offer distinct advantages. Attention has been focused on the behavior of nucleic acid components, pyridine coenzymes, and relevant model compounds in solution as well as the electron-transfer interface. Behavior at the interface involves (a) adsorption of original, intermediate, and product species, (b) association in the adsorbed state, (c) mechanisms and kinetics of electron-transfer (redox) processes, and (d) chemical reactions (kinetics and mechanisms) involving reactant, intermediate (free radical, carbanion), and product species preceding, accompanying and following electron-transfer. Solution behavior includes (a) the "shape" of the compounds as reflected in structure, conformation, and association including stacking, (b) intra-and intermolecular association, and (c) orientation of the compound as it approaches the interface.