期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 136, 期 19, 页码 6978-6986出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja500328k
关键词
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资金
- U.S. Department of Energy DOE-BES [DE-FG02-08ER15995]
- cluster of excellence RESOLV (DFG) at the Ruhr University Bochum [EXC-1069]
- German Research Foundation (DFG) [STR 596/3-1, 1613]
- U.S. Department of Energy (DOE) [DE-FG02-08ER15995] Funding Source: U.S. Department of Energy (DOE)
A study of particle size effects during the catalytic CO2 electroreduction on size-controlled Cu nanoparticles (NPs) is presented. Cu NP catalysts in the 2-15 nm mean size range were prepared, and their catalytic activity and selectivity during CO2 electroreduction were analyzed and compared to a bulk Cu electrode. A dramatic increase in the catalytic activity and selectivity for H-2 and CO was observed with decreasing Cu particle size, in particular, for NPs below 5 nm. Hydrocarbon (methane and ethylene) selectivity was increasingly suppressed for nanoscale Cu surfaces. The size dependence of the surface atomic coordination of model spherical Cu particles was used to rationalize the experimental results. Changes in the population of low-coordinated surface sites and their stronger chemisorption were linked to surging H-2 and CO selectivities, higher catalytic activity, and smaller hydrocarbon selectivity. The presented activity-selectivity-size relations provide novel insights in the CO2 electroreduction reaction on nanoscale surfaces. Our smallest nanoparticles (similar to 2 nm) enter the ab initio computationally accessible size regime, and therefore, the results obtained lend themselves well to density functional theory (DFT) evaluation and reaction mechanism verification.
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