On the interaction of Mg with the (111) and (110) surfaces of ceria
dc.contributor.author | Nolan, Michael | |
dc.contributor.author | Lykhach, Yaroslava | |
dc.contributor.author | Tsud, Nataliya | |
dc.contributor.author | Skala, Tomas | |
dc.contributor.author | Staudt, Thorsten | |
dc.contributor.author | Prince, Kevin C. | |
dc.contributor.author | Matolin, Vladimir | |
dc.contributor.author | Libuda, Jorg | |
dc.contributor.funder | Higher Education Authority | en |
dc.contributor.funder | Science Foundation Ireland | en |
dc.contributor.funder | Deutsche Forschungsgemeinschaft | |
dc.contributor.funder | Verband der Chemischen Industrie | |
dc.contributor.funder | Deutscher Akademischer Austauschdienst | |
dc.contributor.funder | Ministry of Education of the Czech Republic | |
dc.contributor.funder | Grantová Agentura České Republiky | |
dc.date.accessioned | 2014-07-28T15:26:58Z | |
dc.date.available | 2014-07-28T15:26:58Z | |
dc.date.issued | 2011-12-01 | |
dc.date.updated | 2013-10-29T21:43:52Z | |
dc.description.abstract | The catalytic activity of cerium dioxide can be modified by deposition of alkaline earth oxide layers or nanoparticles or by substitutional doping of metal cations at the Ce site in ceria. In order to understand the effect of Mg oxide deposition and doping, a combination of experiment and first principles simulations is a powerful tool. In this paper, we examine the interaction of Mg with the ceria (111) surface using both angle resolved X-ray (ARXPS) and resonant (RPES) photoelectron spectroscopy measurements and density functional theory (DFT) corrected for on-site Coulomb interactions (DFT + U). With DFT + U, we also examine the interaction of Mg with the ceria (110) surface. The experiments show that upon deposition of Mg, Ce ions are reduced to Ce3+, while Mg is oxidised. When Mg is incorporated into ceria, no reduced Ce3+ ions are found and oxygen vacancies are present. The DFT + U simulations show that each Mg that is introduced leads to formation of two reduced Ce3+ ions. When Mg is incorporated at a Ce site in the (111) surface, one oxygen vacancy is formed for each Mg to compensate the different valencies, so that all Ce ions are oxidised. The behaviour of Mg upon interaction with the (110) surface is the same as with the (111) surface. The combined results provide a basis for deeper insights into the catalytic behaviour of ceria-based mixed oxide catalysts. | en |
dc.description.sponsorship | Science Foundation Ireland and Higher Education Authority (SFI and HEA funded Irish Centre for High End Computing); Deutsche Forschungsgemeinschaft (Excellence Cluster ‘‘Engineering of Advanced Materials’’ in the framework of the excellence initiative); Ministry of Education of the Czech Republic (LA08022); Grantová Agentura České Republiky (Czech Grant Agency (P204/10/1169)) | en |
dc.description.status | Peer reviewed | en |
dc.description.version | Accepted Version | en |
dc.format.mimetype | application/pdf | en |
dc.identifier.citation | Nolan, M., Lykhach, Y., Tsud, N., Skala, T., Staudt, T., Prince, K. C., Matolin, V. and Libuda, J. (2012) 'On the interaction of Mg with the (111) and (110) surfaces of ceria', Physical Chemistry Chemical Physics, 14(3), pp. 1293-1301. doi: 10.1039/C1CP22863C | en |
dc.identifier.doi | 10.1039/C1CP22863C | |
dc.identifier.endpage | 1301 | en |
dc.identifier.issn | 1463-9076 | |
dc.identifier.issued | 3 | en |
dc.identifier.journaltitle | Physical Chemistry Chemical Physics | en |
dc.identifier.startpage | 1293 | en |
dc.identifier.uri | https://hdl.handle.net/10468/1605 | |
dc.identifier.volume | 14 | en |
dc.language.iso | en | en |
dc.publisher | Royal Society of Chemistry | en |
dc.relation.project | info:eu-repo/grantAgreement/SFI/SFI Starting Investigator Research Grant (SIRG)/09/SIRG/I1620/IE/EMOIN: Engineering Metal Oxide Interfaces For Renewable Energy Photocatalysis/ | |
dc.rights | © the Owner Societies 2012; Published by Royal Society of Chemistry. This is the Accepted Manuscript version of a published work that appeared in final form in Physical Chemistry Chemical Physics. To access the final published version of record, see http://pubs.rsc.org/en/content/articlepdf/2012/cp/c1cp22863c | en |
dc.subject | CEO2 | en |
dc.subject | Augmented-wave method | en |
dc.subject | Low-index surfaces | en |
dc.subject | Electronic structures | en |
dc.subject | Catalytic-properties | en |
dc.subject | Storage capacity | en |
dc.subject | CO oxidation | en |
dc.subject | Thin-film | en |
dc.subject | Oxide | en |
dc.subject | Adsorption | en |
dc.title | On the interaction of Mg with the (111) and (110) surfaces of ceria | en |
dc.type | Article (peer-reviewed) | en |