Surface Ligand Promotion of Carbon Dioxide Reduction through Stabilizing Chemisorbed Reactive Intermediates

• DOI: 10.1021/acs.jpclett.8b00959
• Publication Date: 2018-05-22T15:04:34Z
• Authors: Zhijiang Wang; Lina Wu; Kun Sun; Ting Chen; Zhaohua Jiang; Tao Cheng; William A. Goddard
• Keywords: Promotion (chess)

We have explored functionalizing metal catalysts with surface ligands as an approach to facilitate electrochemical carbon dioxide reduction reaction (CO2RR). To provide a molecular level understanding of the mechanism by which this enhancement occurs, we combine in situ spectroscopy analysis interpretation based on quantum mechanics (QM) calculations. find that ligand can play critical role stabilizing chemisorbed CO2, facilitates CO2 activation and leads 0.3 V decrease overpotential for monoxide (CO) formation. Moreover, presence nearly exclusive CO production. At −0.6 (versus reversible hydrogen electrode, RHE), is only significant product faradic efficiency 93% current density 1.9 mA cm–2. This improvement corresponds 53-fold turnover frequency compared Ag nanoparticles (NPs) without ligands.