Insight into the Carbon Monoxide Reduction Reaction on Cu(111) from Operando Electrochemical X-ray Photoelectron Spectroscopy
Artikel i vetenskaplig tidskrift, 2025
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(2)RR and beyond.
Heterogeneous catalysis
CO2 reduction
Photoelectron spectroscopy
CO reduction
Electrochemistry
Författare
Bernadette Davies
Stockholms universitet
Fernando Garcia-Martinez
Deutsches Elektronen-Synchrotron (DESY)
Christopher M. Goodwin
El Sincrotrón ALBA
Stockholms universitet
David Degerman
Stockholms universitet
Markus Soldemo
Stockholms universitet
Patrick Loemker
Stockholms universitet
Vladimir Grigorev
Stockholms universitet
Sara Boscolo Bibi
Stockholms universitet
Harri Ali-Loytty
Tampereen Yliopisto
Liquid Sun
Robin Y. Engel
Stockholms universitet
Joakim Halldin Stenlid
Chalmers, Kemi och kemiteknik, Kemi och biokemi
Gabriel L. S. Rodrigues
Syddansk Universitet
Tony Hansson
Stockholms universitet
Christoph Schlueter
Deutsches Elektronen-Synchrotron (DESY)
Xiaodong Zou
Stockholms universitet
Anders Nilsson
Stockholms universitet
Sergey Koroidov
Stockholms universitet
Angewandte Chemie - International Edition
1433-7851 (ISSN) 1521-3773 (eISSN)
Vol. 64 33 e202506402WASP-WISE STRATIFIER
Wallenberg Initiative Materials Science for Sustainability, 2024-01-01 -- 2025-01-01.
Wallenberg AI, Autonomous Systems and Software Program, 2024-01-01 -- 2025-01-01.
Ämneskategorier (SSIF 2025)
Fysikalisk kemi
DOI
10.1002/anie.202506402
PubMed
40460091