Multielectron, multisubstrate molecular catalysis of electrochemical reactions: Formal kinetic analysis in the total catalysis regime

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Abstract
Significance: Small-molecule conversions important to contemporary energy science often involve the reaction of two substrates in a multielectron redox process. The design of catalysts to effect such reactions requires knowledge of the reaction mechanism. It was shown over 30 y ago that quantitative kinetics information may be extracted from the cyclic voltammograms of catalysts that promote reactions involving a single electron and a single substrate. Attempts to extend this model to multielectron, multisubstrate reactions have permitted only qualitative kinetics insights to be extracted. The models developed herein allow quantitative kinetics rate constants to be obtained from peak currents and peak potentials of electrocatalytic reactions beyond a single electron and substrate, and accordingly they should be useful for guiding rational catalyst design.

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