化学
催化作用
一氧化碳
氧合物
氧化物
电化学
拉曼光谱
无机化学
反应性(心理学)
氢氧化物
箔法
电解质
氧化还原
电极
物理化学
有机化学
复合材料
材料科学
替代医学
病理
物理
光学
医学
作者
Youbo Zhao,Xiaoxia Chang,Arnav S. Malkani,Xuan Yang,Levi T. Thompson,Feng Jiao,Bingjun Xu
摘要
Cu-catalyzed selective electrocatalytic upgrading of carbon dioxide/monoxide to valuable multicarbon oxygenates and hydrocarbons is an attractive strategy for combating climate change. Despite recent research on Cu-based catalysts for the CO2 and CO reduction reactions, surface speciation of the various types of Cu surfaces under reaction conditions remains a topic of discussion. Herein, in situ surface-enhanced Raman spectroscopy (SERS) is employed to investigate the speciation of four commonly used Cu surfaces, i.e., Cu foil, Cu micro/nanoparticles, electrochemically deposited Cu film, and oxide-derived Cu, at potentials relevant to the CO reduction reaction in an alkaline electrolyte. Multiple oxide and hydroxide species exist on all Cu surfaces at negative potentials, however, the speciation on the Cu foil is distinct from that on micro/nanostructured Cu. The surface speciation is demonstrated to correlate with the initial degree of oxidation of the Cu surface prior to the exposure to negative potentials. Combining reactivity and spectroscopic results on these four types of Cu surfaces, we conclude that the oxygen containing surface species identified by Raman spectroscopy are unlikely to be active in facilitating the formation of C2+ oxygenates in the CO reduction reaction.
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