Title | Chelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry |
Publication Type | Journal Article |
Year of Publication | 2018 |
Authors | Cao, Z, Derrick, JS, Xu, J, Gao, R, Gong, M, Nichols, EM, Smith, PT, Liu, X, Wen, X, Copéret, C, Chang, CJ |
Journal | Angewandte Chemie International Edition |
Volume | 57 |
Pagination | 4981-4985 |
Keywords | CO2 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. |
URL | https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.201800367 |
DOI | 10.1002/anie.201800367 |