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  Dynamics at Polarized Carbon Dioxide–Iron Oxyhydroxide Interfaces Unveil the Origin of Multicarbon Product Formation

Arrigo, R., Blume, R., Streibel, V., Genovese, C., Roldan, A., Schuster, M. E., et al. (2022). Dynamics at Polarized Carbon Dioxide–Iron Oxyhydroxide Interfaces Unveil the Origin of Multicarbon Product Formation. ACS Catalysis, 12(1), 411-430. doi:10.1021/acscatal.1c04296.

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 Creators:
Arrigo, Rosa1, 2, Author
Blume, Raoul3, 4, Author              
Streibel, Verena3, Author              
Genovese, Chiara5, Author
Roldan, Alberto6, Author
Schuster, Manfred E.7, Author
Ampelli, Claudio5, Author
Perathoner, Siglinda5, Author
Velasco Vélez, Juan3, 4, Author              
Hävecker, Michael3, 4, Author              
Knop-Gericke, Axel3, 4, Author              
Schlögl, Robert3, 4, Author              
Centi, Gabriele5, Author
Affiliations:
1School of Science, Engineering and Environment, University of Salford, Cockcroft Building, Greater Manchester M5 4WT, U.K., ou_persistent22              
2Diamond Light Source Ltd., Harwell Science & Innovation Campus, Didcot, Oxfordshire OX11 0DE, U.K., ou_persistent22              
3Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
4Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34-36, 45470 Mülheim an der Ruhr, Germany, ou_persistent22              
5Departments ChiBioFarAm, ERIC aisbl, and CASPE/INSTM, University of Messina, Viale F. Stagno d’Alcontres 31, 98166 Messina, Italy, ou_persistent22              
6Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff, CF10 3AT, Wales U.K., ou_persistent22              
7Johnson Matthey Technology Centre, Reading RG4 9NH, U.K., ou_persistent22              

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 Abstract: Surface-sensitive ambient pressure X-ray photoelectron spectroscopy and near-edge X-ray absorption fine structure spectroscopy combined with an electrocatalytic reactivity study, multilength-scale electron microscopy, and theoretical modeling provide insights into the gas-phase selective reduction of carbon dioxide to isopropanol on a nitrogen-doped carbon-supported iron oxyhydroxide electrocatalyst. Dissolved atomic carbon forms at relevant potentials for carbon dioxide reduction from the reduction of carbon monoxide chemisorbed on the surface of the ferrihydrite-like phase. Theoretical modeling reveals that the ferrihydrite structure allows vicinal chemisorbed carbon monoxide in the appropriate geometrical arrangement for coupling. Based on our observations, we suggest a mechanism of three-carbon-atom product formation, which involves the intermediate formation of atomic carbon that undergoes hydrogenation in the presence of hydrogen cations upon cathodic polarization. This mechanism is effective only in the case of thin ferrihydrite-like nanostructures coordinated at the edge planes of the graphitic support, where nitrogen edge sites stabilize these species and lower the overpotential for the reaction. Larger ferrihydrite-like nanoparticles are ineffective for electron transport.

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Language(s): eng - English
 Dates: 2021-11-222021-09-182021-122022-01-07
 Publication Status: Published online
 Pages: 20
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.1c04296
 Degree: -

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: 20 Volume / Issue: 12 (1) Sequence Number: - Start / End Page: 411 - 430 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435