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On the Activity/Selectivity and Phase Stability of Thermally Grown Copper Oxides during the Electrocatalytic Reduction of CO2

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Velasco Vélez,  Juan
Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion;
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Gao,  Dunfeng
Interface Science, Fritz Haber Institute, Max Planck Society;
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences;

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Zhu,  Qingjun
Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion;
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Ivanov,  Danail
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Mom,  Rik
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Stotz,  Eugen
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Jones,  Travis
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Roldan Cuenya,  Beatriz
Interface Science, Fritz Haber Institute, Max Planck Society;

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Knop-Gericke,  Axel
Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion;
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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

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Fulltext (public)

acscatal.0c03484.pdf
(Publisher version), 4MB

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Citation

Velasco Vélez, J., Chuang, C.-H., Gao, D., Zhu, Q., Ivanov, D., Jeon, H. S., et al. (2020). On the Activity/Selectivity and Phase Stability of Thermally Grown Copper Oxides during the Electrocatalytic Reduction of CO2. ACS Catalysis, 10(19), 11510-11518. doi:10.1021/acscatal.0c03484.


Cite as: http://hdl.handle.net/21.11116/0000-0007-0829-3
Abstract
Revealing the active nature of oxide derived copper (OD-Cu) is of key importance to understand its remarkable catalytic performance during the cathodic CO2 reduction reaction (CO2RR) to produce valuable hydrocarbons. Using advanced spectroscopy, electron microscopy and electro active surface area characterization techniques, the electronic structure and the changes in the morphology/roughness of thermally oxidized copper thin films were revealed during CO2RR. For this purpose we developed an in situ cell for X-ray spectroscopy able to be operated accurately in the presence of gases or liquids to unite the role of the initial thermal oxide-phase and its active phase during the electrocatalytic reduction of CO2. It was found that the Cu(I) species formed during the thermal treatment are readily reduced to Cu0 during the CO2RR, whereas Cu(II) species are hardly reduced. In addition, Cu(II) oxide electrode dissolution was found to yield a porous/void structure, where the lack of electrical connection between isolated islands prohibits the CO2RR. Therefore, the active/stable phase for CO2RR is metallic copper, independent of its initial phase, with a significant change in its morphology upon its reduction yielding the formation of a rougher surface with higher number of under coordinated sites. Thus, the initial thermal oxidation of copper in air controls the reaction activity/selectivity due to the changes induced in electrode surface morphology/roughness and the presence of more under coordinated sites during the CO2RR.