Healing of oxygen vacancies on reduced surfaces of gold-doped ceria

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dc.contributor.authorNolan, Michael
dc.contributor.funderEuropean Commissionen
dc.contributor.funderSixth Framework Programmeen
dc.contributor.funderScience Foundation Irelanden
dc.contributor.funderHigher Education Authorityen
dc.date.accessioned2018-01-03T12:10:12Z
dc.date.available2018-01-03T12:10:12Z
dc.date.issued2009-04-08
dc.date.updated2017-12-20T16:18:52Z
dc.description.abstractAs an oxidation-reduction catalyst, ceria can catalyze molecular oxidation and reduction. There has been a focus on understanding and enhancing the vacancy formation process to improve the oxidative power of ceria. However, it is important to also address healing of the surface vacancy. To investigate healing of oxygen vacancies in ceria, we study the interaction of atomic and molecular oxygen and NO2 with oxygen vacancies on gold-doped (110) and (100) surfaces using density functional theory, corrected for on-site Coulomb interactions (DFT+U). For atomic and molecular oxygen, adsorption at the reduced surface is favorable and results in an oxygen atom sitting in an oxygen lattice site, healing the oxygen vacancy. On undoped surfaces, O-2 adsorbs as a peroxo (O(2)2-) species. However, on the doped (110) surface a superoxo (O-2-) species is present. When NO2 adsorbs (exothermically) at a divacancy surface, one oxygen of the molecule sits in the vacancy site and the N-O distances are elongated and an [NO2](-) anion forms, similar to the undoped surface. Vacancy healing of ceria surfaces is favorable, even if vacancy formation is enhanced, justifying the current focus on improving the oxidative power of ceria. We briefly examine a catalytic cycle: the reaction of CO with adsorbed O-2 on the undoped and doped surfaces, and find that the doped (110) surface facilitates CO oxidation.en
dc.description.sponsorshipEuropean Commission (NATCO, Grant No. FP6-511925 and REALISE, Grant No. FP6-16172); Science Foundation Ireland (SFI funded computing resources at Tyndall and the SFI/Higher Education Authority funded Irish Centre for High End Computing (ICHEC))en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationNolan, M. (2009) 'Healing of oxygen vacancies on reduced surfaces of gold-doped ceria', The Journal of Chemical Physics, 130(14), 144702 (9pp). doi: 10.1063/1.3110702en
dc.identifier.doi10.1063/1.3110702
dc.identifier.endpage144702-9en
dc.identifier.issn0021-9606
dc.identifier.journaltitleJournal of Chemical Physicsen
dc.identifier.startpage144702-1en
dc.identifier.urihttps://hdl.handle.net/10468/5215
dc.identifier.volume130en
dc.language.isoenen
dc.publisherAIP Publishingen
dc.rights© 2009 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. The following article appeared in The Journal of Chemical Physics 2009 130:14, and may be found at http://aip.scitation.org/doi/abs/10.1063/1.3110702en
dc.subjectVacanciesen
dc.subjectSurface oxidationen
dc.subjectDopingen
dc.subjectAdsorptionen
dc.subjectSurface structureen
dc.subjectCatalystsen
dc.subjectCerium compoundsen
dc.subjectDensity functional theoryen
dc.subjectGolden
dc.subjectOxidationen
dc.subjectOxygenen
dc.subjectReduction (chemical)en
dc.subjectSurface chemistryen
dc.subjectVacancies (crystal)en
dc.subjectAugmented-wave methoden
dc.subjectLow-index surfacesen
dc.subjectElectronic-structureen
dc.subjectCo adsorptionen
dc.subjectCeO2en
dc.subjectCrystalen
dc.subjectMetalsen
dc.subjectNanoparticlesen
dc.subjectSpectroscopyen
dc.subjectTransitionen
dc.titleHealing of oxygen vacancies on reduced surfaces of gold-doped ceriaen
dc.typeArticle (peer-reviewed)en
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