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Electrocatalytic Reduction of CO2 with Palladium Bis-N-heterocyclic Carbene Pincer Complexes

TitleElectrocatalytic Reduction of CO2 with Palladium Bis-N-heterocyclic Carbene Pincer Complexes
Publication TypeJournal Article
Year of Publication2014
AuthorsTherrien, JA, Wolf, MO, Patrick, BO
JournalINORGANIC CHEMISTRY
Volume53
Pagination12962-12972
Date PublishedDEC 15
ISSN0020-1669
Abstract

A series of pyridine- and lutidine-linked bis-N-heterocyclic carbene (NHC) palladium pincer complexes were electrochemically characterized and screened for CO2 reduction capability with 2,2,2-trifluoroethanol, acetic acid, or 2,2,2-trifluoroacetic acid (TFA) as proton sources. The lutidine-linked pincer complexes electrocatalytically reduce CO2 to CO at potentials as low as -1.6 V versus Ag/AgNO3 in the presence of TFA. The one-electron reduction of these complexes is shown to be chemically reversible, yielding a monometallic species, with density functional theory studies indicating charge storage on the redox-active ligand, thus addressing a major source of deactivation in earlier triphosphine electrocatalysts.

DOI10.1021/ic502056w