In situ investigation of methane dry reforming on metal/ceria(111) surfaces: metal-support interactions and C-H bond activation at low temperature

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dc.check.date2018-09-05
dc.check.infoAccess to this article is restricted until 12 months after publication by request of the publisher.en
dc.contributor.authorLiu, Zongyuan
dc.contributor.authorLustemberg, Pablo
dc.contributor.authorGutiérrez, Ramón A.
dc.contributor.authorCarey, John J.
dc.contributor.authorPalomino, Robert M.
dc.contributor.authorVorokhta, Mykhailo
dc.contributor.authorGrinter, David C.
dc.contributor.authorRamírez, Pedro J.
dc.contributor.authorMatolín, Vladimír
dc.contributor.authorNolan, Michael
dc.contributor.authorGanduglia-Pirovano, M. Verónica
dc.contributor.authorSenanayake, Sanjaya D.
dc.contributor.authorRodriguez, José A.
dc.contributor.funderU.S. Department of Energyen
dc.contributor.funderMinisterio de Economía y Competitividaden
dc.contributor.funderSeventh Framework Programmeen
dc.contributor.funderEuropean Cooperation in Science and Technologyen
dc.contributor.funderMinisterstvo Školství, Mládeže a Tělovýchovyen
dc.date.accessioned2017-09-08T12:15:45Z
dc.date.available2017-09-08T12:15:45Z
dc.date.issued2017-09-05
dc.date.updated2017-09-08T11:29:48Z
dc.description.abstractStudies with a series of metal/ceria(111) (metal=Co, Ni, Cu; ceria=CeO2) surfaces indicate that metal–oxide interactions can play a very important role for the activation of methane and its reforming with CO2 at relatively low temperatures (600–700 K). Among the systems examined, Co/CeO2(111) exhibits the best performance and Cu/CeO2(111) has negligible activity. Experiments using ambient pressure X-ray photoelectron spectroscopy indicate that methane dissociates on Co/CeO2(111) at temperatures as low as 300 K—generating CHx and COx species on the catalyst surface. The results of density functional calculations show a reduction in the methane activation barrier from 1.07 eV on Co(0001) to 0.87 eV on Co2+/CeO2(111), and to only 0.05 eV on Co0/CeO2−x(111). At 700 K, under methane dry reforming conditions, CO2 dissociates on the oxide surface and a catalytic cycle is established without coke deposition. A significant part of the CHx formed on the Co0/CeO2−x(111) catalyst recombines to yield ethane or ethylene.en
dc.description.sponsorshipU.S. Department of Energy (DE-SC0012704); Ministerio de Economía y Competitividad (CTQ2015-78823-R); European Cooperation in Science and Technology (COST action CM1104); Ministerstvo Školství, Mládeže a Tělovýchovy (Project LH15277)en
dc.description.statusPeer revieweden
dc.description.versionAccepted Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationLiu, Z., Lustemberg, P., Gutiérrez, R. A., Carey, J. J., Palomino, R. M., Vorokhta, M., Grinter, D. C., Ramírez, P. J., Matolín, V., Nolan, M., Ganduglia-Pirovano, M. V., Senanayake, S. D. and Rodriguez, J. A. (2017) ‘In situ investigation of methane dry reforming on metal/ceria(111) surfaces: metal-support interactions and C-H bond activation at low temperature’, Angewandte Chemie, 129(42), pp. 13221-13226. doi:10.1002/ange.201707538en
dc.identifier.doi10.1002/ange.201707538
dc.identifier.endpage13226
dc.identifier.issn1521-3757
dc.identifier.issued42
dc.identifier.journaltitleAngewandte Chemieen
dc.identifier.startpage13221
dc.identifier.urihttps://hdl.handle.net/10468/4674
dc.identifier.volume129
dc.language.isoenen
dc.publisherJohn Wiley & Sons, Inc.en
dc.relation.projectinfo:eu-repo/grantAgreement/EC/FP7::SP1::NMP/604296/EU/Catalytic Partial Oxidation of Bio Gas and Reforming of Pyrolysis Oil (Bio Oil) for an Autothermal Synthesis Gas Production and Conversion into Fuels/BIOGO-FOR-PRODUCTIONen
dc.rights© 2017, John Wiley & Sons Ltd. This peer reviewed manuscript has been published in final form at http://dx.doi.org/10.1002/ange.201707538. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving.en
dc.subjectCobalten
dc.subjectXPSen
dc.subjectDensity functional theoryen
dc.subjectMethane dissociationen
dc.subjectCeriaen
dc.titleIn situ investigation of methane dry reforming on metal/ceria(111) surfaces: metal-support interactions and C-H bond activation at low temperatureen
dc.typeArticle (peer-reviewed)en
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