We have prepared a new derivative of the popular [Re(bpy)(CO)3X] motif, featuring an internal electric field induced by distal quaternary ammonium groups. The dicationic charge and through space charge interaction significantly alter the mechanism of reduction by affecting the distribution of valence tautomers across the redox non-innocent system, and diminishing the propensity for the one electron reduced complex to dimerize. Spectroelectrochemical, electrochemical, and spectroscopic techniques, along with density functional theory, have been leveraged to elucidate the mechanistic deviations from known systems, and the effects on electrocatalytic CO2 reduction. Additionally, unique underpotential interactions with CO2 have been explored.

Coulombic effects on multi-electron reduction of a rhenium carbonyl complex with catalytic implications

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.