Insight into the Carbon Monoxide Reduction Reaction on Cu(111) from <i>Operando</i> Electrochemical X‐ray Photoelectron Spectroscopy

In this work, we introduce a modified dip-and-pull electrochemical X-ray photoelectron spectroscopy (ECXPS) approach that offers new mechanistic insight into the alkaline carbon monoxide reduction reaction (CORR) over a Cu(111) single crystal surface. We tackle two major unresolved questions in the CORR mechanism that persist in the literature. Firstly, we address the mechanism for methane formation on Cu(111) and show that the mechanism likely proceeds via atomic carbon, which subsequently couples, leading to the accumulation of amorphous carbon on the surface. Secondly, we provide insight into whether the mechanism for acetate formation occurs entirely on the surface or partially within the solution phase, showing that acetate is present on the surface, indicating a surface-based reaction. These insights into surface-based mechanisms provide a handle for designing future catalysts that can efficiently target the binding of specific intermediates. Furthermore, we expect that our modified approach to dip-and-pull ECXPS - in which we have changed the electrode geometry, the method of introducing the reactant gas and used hard x-rays - will significantly expand the technique's applicability, enabling studies of the CO<sub>(2)</sub>RR and beyond.

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Publication Details

Journal
Angewandte Chemie International Edition
Published
2025-06-03
DOI
https://doi.org/10.1002/anie.202506402
Citations
4
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
1.45

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article

Insight into the Carbon Monoxide Reduction Reaction on Cu(111) from Operando Electrochemical X‐ray Photoelectron Spectroscopy

Harri Ali‐Löytty, Robin Y. Engel, Patrick Lömker, Tony Hansson et al.
4 citations
Angewandte Chemie International Edition
CO2 Reduction Techniques and Catalysts
1.45
article

Insight into the Carbon Monoxide Reduction Reaction on Cu(111) from Operando Electrochemical X‐ray Photoelectron Spectroscopy

Harri Ali‐Löytty, Robin Y. Engel, Patrick Lömker, Tony Hansson, Xiaodong Zou, Christoph Schlueter, Fernando García‐Martínez, Christopher M. Goodwin, Joakim Halldin Stenlid, Markus Soldemo, Bernadette Davies, Gabriel L. S. Rodrigues, Sergey Koroidov, David Degerman, В. В. Григорьев, Anders Nilsson, Vladimir Grigorev
article en
4 citations

Abstract

In this work, we introduce a modified dip-and-pull electrochemical X-ray photoelectron spectroscopy (ECXPS) approach that offers new mechanistic insight into the alkaline carbon monoxide reduction reaction (CORR) over a Cu(111) single crystal surface. We tackle two major unresolved questions in the CORR mechanism that persist in the literature. Firstly, we address the mechanism for methane formation on Cu(111) and show that the mechanism likely proceeds via atomic carbon, which subsequently couples, leading to the accumulation of amorphous carbon on the surface. Secondly, we provide insight into whether the mechanism for acetate formation occurs entirely on the surface or partially within the solution phase, showing that acetate is present on the surface, indicating a surface-based reaction. These insights into surface-based mechanisms provide a handle for designing future catalysts that can efficiently target the binding of specific intermediates. Furthermore, we expect that our modified approach to dip-and-pull ECXPS - in which we have changed the electrode geometry, the method of introducing the reactant gas and used hard x-rays - will significantly expand the technique's applicability, enabling studies of the CO<sub>(2)</sub>RR and beyond.

Angewandte Chemie International EditionVol. 64(33)
Stockholm University (SE), Tampere University (FI), University of Southern Denmark (DK), Deutsches Elektronen-Synchrotron DESY (DE), Wallenberg Wood Science Center (SE), AlbaNova (SE), Chalmers University of Technology (SE)
Chalmers Tekniska Högskola, Knut och Alice Wallenbergs Stiftelse, Kungliga Tekniska Högskolan, Vetenskapsrådet, Deutsches Elektronen-Synchrotron
Openalex Percentile: Top 18%
CO2 Reduction Techniques and Catalysts
1.45
DOIOpen Access PDFOpenAlex
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