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Chelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry

TitleChelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry
Publication TypeJournal Article
Year of Publication2018
AuthorsCao, Z, Derrick, JS, Xu, J, Gao, R, Gong, M, Nichols, EM, Smith, PT, Liu, X, Wen, X, Copéret, C, Chang, CJ
JournalAngewandte Chemie International Edition
Volume57
Pagination4981-4985
KeywordsCO2 reduction, electrocatalysis, N-heterocyclic carbenes, palladium, surface chemistry
Abstract

Abstract Reported here is the chelate effect as a design principle for tuning heterogeneous catalysts for electrochemical CO2 reduction. Palladium functionalized with a chelating tris-N-heterocyclic carbene (NHC) ligand (Pd-timtmbMe) exhibits a 32-fold increase in activity for electrochemical reduction of CO2 to C1 products with high Faradaic efficiency (FEC1=86 %) compared to the parent unfunctionalized Pd foil (FE=23 %), and with sustained activity relative to a monodentate NHC-ligated Pd electrode (Pd-mimtmbMe). The results highlight the contributions of the chelate effect for tailoring and maintaining reactivity at molecular-materials interfaces enabled by surface organometallic chemistry.

URLhttps://onlinelibrary.wiley.com/doi/abs/10.1002/anie.201800367
DOI10.1002/anie.201800367