期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 26, 页码 8120-8125出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b02878
关键词
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资金
- U.S. Department of Energy/Lawrence Berkeley National Laboratory [101528-002]
- Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, U.S. Department of Energy [DE-AC02-05CH11231]
- Samsung
- National Science Foundation
- Grants-in-Aid for Scientific Research [15J04635] Funding Source: KAKEN
Conversion of the greenhouse gas carbon dioxide (CO2) to value-added products is an important challenge for sustainable energy research, and nanomaterials offer a broad class of heterogeneous catalysts for such transformations. Here we report a molecular surface functionalization approach to tuning gold nanoparticle (Au NP) electrocatalysts for reduction of CO2 to CO. The N-heterocyclic (NHC) carbene-functionalized Au NP catalyst exhibits improved faradaic efficiency (FE = 83%) for reduction of CO2 to CO in water at neutral pH at an overpotential of 0.46 V with a 7.6-fold increase in current density compared to that of the parent Au NP (FE = 53%). Tafel plots of the NHC carbene-functionalized Au NP (72 mV/decade) vs parent Au NP (138 mV/decade) systems further show that the molecular ligand influences mechanistic pathways for CO2 reduction. The results establish molecular surface functionalization as a complementary approach to size, shape, composition, and defect control for nanoparticle catalyst design.
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