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Synthesis and comparison of nickel, palladium, and platinum bis(N-heterocyclic carbene) pincer complexes for electrocatalytic CO2 reduction

TitleSynthesis and comparison of nickel, palladium, and platinum bis(N-heterocyclic carbene) pincer complexes for electrocatalytic CO2 reduction
Publication TypeJournal Article
Year of Publication2018
AuthorsTherrien, JA, Wolf, MO, Patrick, BO
JournalDALTON TRANSACTIONS
Volume47
Pagination1827-1840
Date PublishedFEB 14
ISSN1477-9226
Abstract

A valence isoelectronic and isostructural series of charged bis(N-heterocyclic carbene) pincer complexes {[}M(bC(boolean AND)N(boolean AND)bC)X]OTf and {[}M(bC(boolean AND)N(boolean AND)bC)CH3CN](OTf)(2) (where M = Ni, Pd, and Pt, bC(boolean AND)N(boolean AND)bC = 1,1'-(pyridine- 2,6-diylbis(methylene)) bis(3-butylbenzo{[}d]imidazol-2-ylidene)) were synthesized, characterized, modelled by density functional theory calculations, and compared for their electrochemical properties and reactivity with CO2. Although the electrochemical response of each complex is altered by the presence of CO2, controlled potential electrolysis experiments demonstrated the superior ability of {[}Pd] to reduce CO2 to CO in faradaic efficiencies up to 58% in the presence of trifluoroacetic acid, compared to {[}Pt] and {[}Ni] which showed only marginal production of CO, giving the trend {[}Pd] >> {[}Pt] > {[}Ni] for this series.

DOI10.1039/c7dt04089j