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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

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Velasco-Velez,  Juan Jesus
Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Gao,  Dunfeng
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Zhu,  Qingjun
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Knop-Gericke,  Axel
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Lunkenbein,  Thomas
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Schlögl,  Robert
Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Velasco-Velez, J. J., Mom V, R., Sandoval-Diaz, L.-E., Falling, L. J., Chuang, C.-H., Gao, D., et al. (2020). 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, 5(6), 2106-2111. doi:10.1021/acsenergylett.0c00802.


Cite as: http://hdl.handle.net/21.11116/0000-0007-D506-2
Abstract
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.