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Amorphous, Periodic Model of a Copper Electrocatalyst with Subsurface Oxygen for Enhanced CO Coverage and Dimerization
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-0123-631X
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0001-6496-6865
Stockholm University, Faculty of Science, Department of Physics.
Stockholm University, Faculty of Science, Department of Physics.
Number of Authors: 42019 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 123, no 8, p. 4961-4968Article in journal (Refereed) Published
Abstract [en]

Oxide-derived copper electrocatalysts have been found to possess excellent selectivity toward the production of multicarbon products from CO,. The presence of subsurface oxygen in these catalysts has been confirmed experimentally, but the resulting amorphous structure has yet to be captured by theoretical models. In this study, the role of subsurface oxygen atoms is investigated with density functional theory, using a disordered oxide-derived Cu surface model (d-ODCu). The presence of subsurface oxygen atoms increases the maximum adsorption coverage of the important CO intermediate but decreases that of H atoms because of electronic and geometric effects. However, this has no significant influence on the free-energy activation barrier or endothermicity of the CO-dimerization reaction step, allegedly the key to multicarbon product formation.

Place, publisher, year, edition, pages
2019. Vol. 123, no 8, p. 4961-4968
National Category
Physical Sciences
Research subject
Theoretical Physics
Identifiers
URN: urn:nbn:se:su:diva-167653DOI: 10.1021/acs.jpcc.8b12214ISI: 000460365200033OAI: oai:DiVA.org:su-167653DiVA, id: diva2:1302473
Available from: 2019-04-04 Created: 2019-04-04 Last updated: 2019-12-04Bibliographically approved
In thesis
1. Le Fantôme de l’Opéra - Studies on Atoms and Electrons Beneath
Open this publication in new window or tab >>Le Fantôme de l’Opéra - Studies on Atoms and Electrons Beneath
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The carbon dioxide reduction reaction is a promising candidate to tackle ecological challenges of our age. This is due to its capability of reducing carbon dioxide emission generated from the combustion of fossil fuels by converting carbon dioxide into valuable hydrocarbons. Oxide-derived metal nanostructures have been found to exhibit unique catalytic characteristics for facilitating the carbon dioxide reduction reaction. In this thesis work, the stability, influence, and effects of subsurface oxygen atoms are investigated by theoretical computations with various levels of theory and models. It is found that subsurface oxygen atoms are stable and that their presence increases the CO adsorption strength and coverage on oxide-derived Cu surface. This is explained by a reduced σ-repulsion and leads to the breaking of scaling relations. Although it does not directly reduce the CO dimerization barrier, the adsorption of H atoms is inhibited thus steering the selectivity. The presence of subsurface oxygen atoms is also concluded from a joint work with experimental and theoretical efforts of X-ray photoelectron spectroscopy. The precursor region of CO desorption from Ru(0001) is studied with the transition potential method. In contrast, for the simulation of the X-ray spectroscopy results on p4g C/Ni(100), which is a surface reconstruction when carbon atoms adsorb on Ni(100), vibrational effects are also needed for understanding the experimental data.

Place, publisher, year, edition, pages
Stockholm: Department of Physics, Stockholm University, 2019. p. 75
Keywords
Carbon dioxide reduction, Subsurface oxygen, X-ray spectroscopy, Density functional theory, CO desorption
National Category
Atom and Molecular Physics and Optics
Research subject
Theoretical Physics
Identifiers
urn:nbn:se:su:diva-174700 (URN)978-91-7797-863-3 (ISBN)978-91-7797-864-0 (ISBN)
Public defence
2019-11-22, sal FA32, AlbaNova universitetscentrum, Roslagstullsbacken 21, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2019-10-30 Created: 2019-10-08 Last updated: 2019-10-21Bibliographically approved

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Liu, ChangHedström, SvanteStenlid, Joakim H.Pettersson, Lars G. M.
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