二氧化碳电化学还原
氧化物
铜
X射线光电子能谱
无机化学
氧化铜
一氧化碳
电化学
二氧化碳
氧气
材料科学
催化作用
碳纤维
化学
化学工程
电极
冶金
复合材料
物理化学
有机化学
工程类
复合数
作者
André Eilert,Filippo Cavalca,F. Sloan Roberts,Jürg Osterwalder,Chang Liu,Marco Favaro,Ethan J. Crumlin,Hirohito Ogasawara,Daniel Friebel,Lars G. M. Pettersson,Anders Nilsson
标识
DOI:10.1021/acs.jpclett.6b02273
摘要
Copper electrocatalysts derived from an oxide have shown extraordinary electrochemical properties for the carbon dioxide reduction reaction (CO2RR). Using in situ ambient pressure X-ray photoelectron spectroscopy and quasi in situ electron energy-loss spectroscopy in a transmission electron microscope, we show that there is a substantial amount of residual oxygen in nanostructured, oxide-derived copper electrocatalysts but no residual copper oxide. On the basis of these findings in combination with density functional theory simulations, we propose that residual subsurface oxygen changes the electronic structure of the catalyst and creates sites with higher carbon monoxide binding energy. If such sites are stable under the strongly reducing conditions found in CO2RR, these findings would explain the high efficiencies of oxide-derived copper in reducing carbon dioxide to multicarbon compounds such as ethylene.
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