The oxygen reduction reaction (ORR) continues to be a reaction of interest because of its importance to biologically relevant reactions and as a pathway for meeting increasing energy demands through fuel cell applications. Developing earth-abundant molecular mimics of metalloprotein active sites can offer insight into fundamental biological processes, as well as, offer a green alternative to the anthraquinone process for the synthesis of H2O2 if selectivity can be achieved. We have conducted a series of mechanistic investigations on the electrocatalytic reduction of dioxygen (O2) to hydrogen peroxide (H2O2) by a molecular manganese (III) complex with a tetradentate dianionic bipyridine-based ligand that, upon electrochemical reduction, is competent for the reduction of dioxygen to H2O2 with 81±4% Faradaic efficiency. Spectrochemical stopped-flow analyses utilizing decamethylferrocene as a reductant uncovered a divergence in mechanism based of the nature of the reductant, although H2O2 is still generated when a homogeneous reductant is used. Additionally, studies utilizing p-benzoquinone as an electron-proton transfer mediator quantitative selectivities for the four electron/four proton reduction product H2O are observed.

Electrocatalytic reduction of dioxygen by a molecular manganese complex with a bipyridine-containing Schiff base ligand

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.