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Electrocatalytic reduction of CO2 with palladium bis-N-heterocyclic carbene pincer complexes.

Authors
  • Therrien, Jeffrey A
  • Wolf, Michael O
  • Patrick, Brian O
Type
Published Article
Journal
Inorganic Chemistry
Publisher
American Chemical Society
Publication Date
Dec 15, 2014
Volume
53
Issue
24
Pages
12962–12972
Identifiers
DOI: 10.1021/ic502056w
PMID: 25337973
Source
Medline
License
Unknown

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.

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