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Title: A density functional theory study of the adsorption behaviour of CO{sub 2} on Cu{sub 2}O surfaces

Abstract

Copper has many applications, particularly in electro-catalysis, where the oxidation state of the copper electrode plays a significant role in the selectivity towards products. Although copper-based materials have clear potential as catalysts in the reduction of CO{sub 2} and conversion to products, fundamental understanding of CO{sub 2} adsorption and activation on different copper oxide surfaces is still limited. We have used DFT+U methodology to study the surface reconstruction of the three most exposed (111), (110), and (001) surfaces of Cu{sub 2}O with different possible terminations. Considering several adsorbate geometries, we have investigated CO{sub 2} adsorption on five different possible terminations and proposed eight different configurations in which CO{sub 2} binds with the surface. Similar to earlier findings, CO{sub 2} binds weakly with the most stable Cu{sub 2}O(111):O surface showing no molecular activation, whereas a number of other surfaces, which can appear in the Cu{sub 2}O particles morphology, show stronger binding as well as activation of the CO{sub 2} molecule. Different CO{sub 2} coverages were studied and a detailed structural and electronic charge analysis is presented. The activation of the CO{sub 2} molecule is characterized by structural transformations and charge transfer between the surface and the CO{sub 2} molecule, which ismore » further confirmed by considerable red shifts in the vibrational frequencies.« less

Authors:
 [1];  [2]
  1. School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT (United Kingdom)
  2. Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ (United Kingdom)
Publication Date:
OSTI Identifier:
22679009
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 145; Journal Issue: 4; Other Information: (c) 2016 Author(s); Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ACTIVATED CARBON; ADSORPTION; CARBON DIOXIDE; COPPER OXIDES; CRYSTAL LATTICES; DENSITY FUNCTIONAL METHOD; EXPERIMENTAL DATA; OXIDATION; RED SHIFT; SURFACES

Citation Formats

Mishra, Abhishek Kumar, E-mail: akmishra@ddn.upes.ac.in, E-mail: abhishek.mishra@ucl.ac.uk, E-mail: deleeuwn@cardiff.ac.uk, Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, Roldan, Alberto, Leeuw, Nora H. de,, and School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT. A density functional theory study of the adsorption behaviour of CO{sub 2} on Cu{sub 2}O surfaces. United States: N. p., 2016. Web. doi:10.1063/1.4958804.
Mishra, Abhishek Kumar, E-mail: akmishra@ddn.upes.ac.in, E-mail: abhishek.mishra@ucl.ac.uk, E-mail: deleeuwn@cardiff.ac.uk, Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, Roldan, Alberto, Leeuw, Nora H. de,, & School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT. A density functional theory study of the adsorption behaviour of CO{sub 2} on Cu{sub 2}O surfaces. United States. https://doi.org/10.1063/1.4958804
Mishra, Abhishek Kumar, E-mail: akmishra@ddn.upes.ac.in, E-mail: abhishek.mishra@ucl.ac.uk, E-mail: deleeuwn@cardiff.ac.uk, Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, Roldan, Alberto, Leeuw, Nora H. de,, and School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT. 2016. "A density functional theory study of the adsorption behaviour of CO{sub 2} on Cu{sub 2}O surfaces". United States. https://doi.org/10.1063/1.4958804.
@article{osti_22679009,
title = {A density functional theory study of the adsorption behaviour of CO{sub 2} on Cu{sub 2}O surfaces},
author = {Mishra, Abhishek Kumar, E-mail: akmishra@ddn.upes.ac.in, E-mail: abhishek.mishra@ucl.ac.uk, E-mail: deleeuwn@cardiff.ac.uk and Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ and Roldan, Alberto and Leeuw, Nora H. de, and School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT},
abstractNote = {Copper has many applications, particularly in electro-catalysis, where the oxidation state of the copper electrode plays a significant role in the selectivity towards products. Although copper-based materials have clear potential as catalysts in the reduction of CO{sub 2} and conversion to products, fundamental understanding of CO{sub 2} adsorption and activation on different copper oxide surfaces is still limited. We have used DFT+U methodology to study the surface reconstruction of the three most exposed (111), (110), and (001) surfaces of Cu{sub 2}O with different possible terminations. Considering several adsorbate geometries, we have investigated CO{sub 2} adsorption on five different possible terminations and proposed eight different configurations in which CO{sub 2} binds with the surface. Similar to earlier findings, CO{sub 2} binds weakly with the most stable Cu{sub 2}O(111):O surface showing no molecular activation, whereas a number of other surfaces, which can appear in the Cu{sub 2}O particles morphology, show stronger binding as well as activation of the CO{sub 2} molecule. Different CO{sub 2} coverages were studied and a detailed structural and electronic charge analysis is presented. The activation of the CO{sub 2} molecule is characterized by structural transformations and charge transfer between the surface and the CO{sub 2} molecule, which is further confirmed by considerable red shifts in the vibrational frequencies.},
doi = {10.1063/1.4958804},
url = {https://www.osti.gov/biblio/22679009}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 4,
volume = 145,
place = {United States},
year = {Thu Jul 28 00:00:00 EDT 2016},
month = {Thu Jul 28 00:00:00 EDT 2016}
}