If the electron exchange reaction at the surface of an electrode is sufficiently fast, either due to the inherent kinetic properties of the reaction or due to large overpotentials, then the rate at which the overall reaction will proceed is determined by the rate of transport of reactant to, or products from, the electrode surface. At low overpotentials, or for intrinsically slow electrode processes, it is necessary to take into account the kinetics of the electrode reaction at the surface when solving the diffusion equation for the system. In other instances, chemical reactions may precede or follow the charge transfer reaction, and in these cases it is necessary to modify the diffusion equations to recognize the contributions from these “kinetic” processes to the overall transient response of the system. Since the theoretical description of the transient responses of systems of this type requires the time dependences of surface concentrations and fluxes, it is necessary to consider in detail various methods for solving Fick’s laws of diffusion.

The Mathematics of Diffusion

Polarography is still the best known classical measuring method in electroanalytical chemistry. However, in recent years its position has been challenged by cyclic voltammetry (CV). Simple diagnostic criteria and relatively easily acquired measuring techniques have hastened this development. Cyclic voltammetry has the further attraction of providing information not only on the thermodynamics of redox processes but also on the kinetics of heterogeneous electron-transfer reactions and coupled chemical reactions. The characteristic shapes of the voltammetric waves and their unequivocal position on the potential scale virtually fingerprint the individual electrochemical properties of redox systems. For this reason the method has been labeled “electrochemical spectroscopy”.

Cyclic Voltammetry—“Electrochemical Spectroscopy”. New Analytical Methods (25)

Pyridinium and its substituted derivatives are effective and stable homogeneous electrocatalysts for the aqueous multiple-electron, multiple-proton reduction of carbon dioxide to products such as formic acid, formaldehyde, and methanol. Importantly, high faradaic yields for methanol have been observed in both electrochemical and photoelectrochemical systems at low reaction overpotentials. Herein, we report the detailed mechanism of pyridinium-catalyzed CO2 reduction to methanol. At metal electrodes, formic acid and formaldehyde were observed to be intermediate products along the pathway to the 6e−-reduced product of methanol, with the pyridinium radical playing a role in the reduction of both intermediate products. It has previously been thought that metal-derived multielectron transfer was necessary to achieve highly reduced products such as methanol. Surprisingly, this simple organic molecule is found to be capable of reducing many different chemical species en route to methanol through six sequential e...

Using a one-electron shuttle for the multielectron reduction of CO2 to methanol: kinetic, mechanistic, and structural insights.

Standard potential and kinetic parameters of the electrochemical reduction of carbon dioxide in dimethylformamide

Electrodimerization: I. One-electron irreversible dimerization. Diagnostic criteria and rate determination procedures for voltammetric studies

Theory of cyclic voltammetry for a dimerization reaction initiated electrochemically

Cyclic voltammetry theory for the disproportionation reaction and spherical diffusion

Influence of double-layer charging in chronopotentiometry

A method based on polynomial approximations for numerical solution of volterra integral equations

Double potential step method for measuring rate constants of dimerization reactions

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