Assessment of the Degradation Mechanisms of Cu Electrodes during the CO2 
Reduction Reaction

Mom, Rik; Sandoval Diaz, Luis; Gao, Dunfeng; Chuang, Cheng-Hao; Carbonio, Emilia; Jones, Travis; Arrigo, Rosa; Ivanov, Danail; Hävecker, Michael; Roldan Cuenya, Beatriz; Schlögl, Robert; Lunkenbein, Thomas; Knop-Gericke, Axel; Velasco Vélez, Juan

doi:10.1021/acsami.2c23007

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Assessment of the Degradation Mechanisms of Cu Electrodes during the CO₂ Reduction Reaction

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/persons/resource/persons206875

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

/persons/resource/persons247186

Sandoval Diaz, Luis
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227597

Gao, Dunfeng
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons183245

Carbonio, Emilia
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons135780

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

/persons/resource/persons188969

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

/persons/resource/persons21590

Hävecker, Michael
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22020

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

/persons/resource/persons22071

Schlögl, Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons41515

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

/persons/resource/persons21743

Knop-Gericke, Axel
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons104341

Velasco Vélez, Juan
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Mom, R., Sandoval Diaz, L., Gao, D., Chuang, C.-H., Carbonio, E., Jones, T., et al. (2023). Assessment of the Degradation Mechanisms of Cu Electrodes during the CO₂ Reduction Reaction. ACS Applied Materials and Interfaces, 15(25), 30052-30059. doi:10.1021/acsami.2c23007.

Cite as: https://hdl.handle.net/21.11116/0000-000F-26FF-8

Abstract

Catalyst degradation and product selectivity changes are two of the key challenges in the electrochemical reduction of CO₂ on copper electrodes. Yet, these aspects are often overlooked. Here, we combine in situ X-ray spectroscopy, in situ electron microscopy, and ex situ characterization techniques to follow the long-term evolution of the catalyst morphology, electronic structure, surface composition, activity, and product selectivity of Cu nanosized crystals during the CO₂ reduction reaction. We found no changes in the electronic structure of the electrode under cathodic potentiostatic control over time, nor was there any build-up of contaminants. In contrast, the electrode morphology is modified by prolonged CO₂ electroreduction, which transforms the initially faceted Cu particles into a rough/rounded structure. In conjunction with these morphological changes, the current increases and the selectivity changes from value-added hydrocarbons to less valuable side reaction products, i.e., hydrogen and CO. Hence, our results suggest that the stabilization of a faceted Cu morphology is pivotal for ensuring optimal long-term performance in the selective reduction of CO₂ into hydrocarbons and oxygenated products.