期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 9, 期 11, 页码 3057-3061出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b00959
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资金
- Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub through the Office of Science of the U.S. Department of Energy [DE-SC0004993]
- National Science Foundation [ACI-1053575]
- State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology [HC201813]
- National Natural Science Foundation of China [81771903]
- Wuliande Foundation of Harbin Medical University [WLD-QN1404]
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 with an interpretation based on quantum mechanics (QM) calculations. We find that a surface ligand can play a critical role in stabilizing the chemisorbed CO2, which facilitates CO2 activation and leads to a 0.3 V decrease in the overpotential for carbon monoxide (CO) formation. Moreover, the presence of the surface ligand leads to nearly exclusive CO production. At -0.6 V (versus reversible hydrogen electrode, RHE), CO is the only significant product with a faradic efficiency of 93% and a current density of 1.9 mA cm(-2). This improvement corresponds to 53-fold enhancement in turnover frequency compared with the Ag nanoparticles (NPs) without surface ligands.
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