Abstract
A mathematical model was developed for the impedance response associated with coupled homogeneous chemical and heterogeneous electrochemical reactions. The model includes a homogeneous reaction in the electrolyte in which species AB reacts reversibly to form A− and B+ and B+ reacts electrochemically on a rotating disk electrode to produce B. The resulting diffusion impedance has two asymmetric capacitive loops, one associated with convective diffusion and the other with the homogeneous reaction. For an infinitely fast homogeneous reaction, the system is shown to behave as though AB is the electroactive species. A modified Gerischer impedance was found to provide a good fit to the simulated data.
Highlights
To cite this version: Morgan S Harding, Bernard Tribollet, Vincent Vivier, Mark E Orazem
Bossche et al.[4] describe finite-difference calculations under assumption of a steady state for an electrochemical system controlled by diffusion, migration, convection, and nonlinear homogeneous reaction kinetics
Concentrations were scaled by the mass balance of the species involved in the homogeneous reaction, co = cA− +cB+ +cAB, to emphasize the relative changes in values as well as the overall concentration in the electrolyte
Summary
To cite this version: Morgan S Harding, Bernard Tribollet, Vincent Vivier, Mark E Orazem. Koutecky and Levich[1,2,3] developed a steady-state model for a homogeneous reaction coupled with an electrochemical reaction on a rotating disk electrode. Bossche et al.[4] describe finite-difference calculations under assumption of a steady state for an electrochemical system controlled by diffusion, migration, convection, and nonlinear homogeneous reaction kinetics. Their convection term used a three-term expansion appropriate for positions close to the electrode surface.[5] Deslouis et al.[6] used a submerged impinging jet cell to measure interfacial pH during the reduction of dissolved oxygen in the presence of carbonate
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