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Assessment of the Degradation Mechanisms of Cu Electrodes during the CO

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

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Authors

Rik V Mom

Luis-Ernesto Sandoval-Diaz

Dunfeng Gao

Cheng-Hao Chuang

Emilia A Carbonio

Travis E Jones

Danail Ivanov

Michael Hävecker

Beatriz Roldan Cuenya

Robert Schlögl

Thomas Lunkenbein

Axel Knop-Gericke

Juan-Jesús Velasco-Vélez



Abstract

Catalyst degradation and product selectivity changes are two of the key challenges in the electrochemical reduction of CO on copper electrodes. Yet, these aspects are often overlooked. Here, we combine X-ray spectroscopy, electron microscopy, and 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 CO 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 CO 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, , 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 CO into hydrocarbons and oxygenated products.

Citation

Mom, R. V., Sandoval-Diaz, L.-E., Gao, D., Chuang, C.-H., Carbonio, E. A., Jones, T. E., …Velasco-Vélez, J.-J. (in press). Assessment of the Degradation Mechanisms of Cu Electrodes during the CO. ACS applied materials & interfaces, 15(25), https://doi.org/10.1021/acsami.2c23007

Journal Article Type Article
Acceptance Date Jun 4, 2023
Online Publication Date Jun 15, 2023
Deposit Date Jul 6, 2023
Publicly Available Date Jul 6, 2023
Journal ACS applied materials & interfaces
Print ISSN 1944-8244
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 15
Issue 25
DOI https://doi.org/10.1021/acsami.2c23007
Keywords in situ X-ray spectroscopy, in situ EC-SEM, long-term reactions, electrocatalysis, CO2RR, copper degradation

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