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Revealing the Active Phase of Copper during the Electroreduction of CO2 in Aqueous Electrolyte by Correlating In Situ X-ray Spectroscopy and In Situ Electron Microscopy.
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-05-27 , DOI: 10.1021/acsenergylett.0c00802
Juan-Jesus Velasco-Velez,Rik V Mom,Luis-Ernesto Sandoval-Diaz,Lorenz J Falling,Cheng-Hao Chuang,Dunfeng Gao,Travis E Jones,Qingjun Zhu,Rosa Arrigo,Beatriz Roldan Cuenya,Axel Knop-Gericke,Thomas Lunkenbein,Robert Schlögl

The variation in the morphology and electronic structure of copper during the electroreduction of CO2 into valuable hydrocarbons and alcohols was revealed by combining in situ surface- and bulk-sensitive X-ray spectroscopies with electrochemical scanning electron microscopy. These experiments proved that the electrified interface surface and near-surface are dominated by reduced copper. The selectivity to the formation of the key C–C bond is enhanced at higher cathodic potentials as a consequence of increased copper metallicity. In addition, the reduction of the copper oxide electrode and oxygen loss in the lattice reconstructs the electrode to yield a rougher surface with more uncoordinated sites, which controls the dissociation barrier of water and CO2. Thus, according to these results, copper oxide species can only be stabilized kinetically under CO2 reduction reaction conditions.

中文翻译:

通过将原位X射线光谱和原位电子显微镜相关联,揭示了在电解液中CO2电还原过程中铜的活性相。

通过将原位表面和本体敏感的X射线光谱学与电化学扫描电子显微镜相结合揭示了将CO 2电还原为有价值的烃和醇的过程中,铜的形态和电子结构的变化。这些实验证明,带电的界面表面和近表面以还原铜为主。由于铜金属度的增加,在较高的阴极电位下,形成关键碳原子键的选择性增加。另外,氧化铜电极的减少和晶格中的氧损失使电极重建,从而产生具有更不协调位置的粗糙表面,从而控制了水和CO 2的解离势垒。因此,根据这些结果,只能在CO 2还原反应条件下使氧化铜物质动力学稳定。
更新日期:2020-05-27
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