|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|
|Keywords||CO2 reduction, electrocatalysis, N-heterocyclic carbenes, palladium, surface chemistry|
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.