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dc.contributor.authorZhang, Feng
dc.contributor.authorLiu, Zongyuan
dc.contributor.authorZhang, Shuhao
dc.contributor.authorAkter, Nusnin
dc.contributor.authorPalomino, Robert M.
dc.contributor.authorVovchok, Dimitriy
dc.contributor.authorOrozco, Ivan
dc.contributor.authorSalazar, David
dc.contributor.authorRodriguez, José A.
dc.contributor.authorLlorca Piqué, Jordi
dc.contributor.authorLee, Jaeha
dc.contributor.authorKim, DoHeui
dc.contributor.authorXu, Wenqian
dc.contributor.authorFrenkel, Anatoly I.
dc.contributor.authorLi, Yuangyuang
dc.contributor.authorKim, Taejin
dc.contributor.authorSenanayake, S. D.
dc.contributor.otherUniversitat Politècnica de Catalunya. Departament d'Enginyeria Química
dc.date.accessioned2018-06-22T06:37:22Z
dc.date.available2019-03-12T01:30:32Z
dc.date.issued2018-04-01
dc.identifier.citationZhang, F., Liu, Z., Zhang, S., Akter, N., Palomino, R., Vovchok, D., Orozco, I., Salazar, D., Rodriguez, J., Llorca, J., Lee, J., Kim, ., Xu, W., Frenkel, A., Li, Y., Kim , T., Senanayake, S. In situ elucidation of the active state of Co-CeOx catalysts in the dry reforming of methane: the important role of the reducible oxide support and interactions with cobalt. "ACS catalysis", 1 Abril 2018, vol. 8, núm. 4, p. 3550-3560.
dc.identifier.issn2155-5435
dc.identifier.urihttp://hdl.handle.net/2117/118330
dc.description.abstractThe dry reforming of methane was systematically studied over a series (2-30 wt%) of Co (~5nm in size) loaded CeO2 catalysts, with an effort to elucidate the behavior of Co and ceria in the catalytic process using in-situ methods. For the systems under study, the reaction activity scaled with increasing Co loading, and a 10 wt% Co-CeO2 catalyst exhibiting the best catalytic activity and good stability at 500 °C with little evidence for carbon accumulation. The phase transitions and the nature of active components in the catalyst were investigated during pretreatment and under reaction conditions by ex-situ/in-situ techniques including X-ray diffraction (XRD) and ambient-pressure X-ray photoelectron spectroscopy (AP-XPS). These studies showed a dynamical evolution in the chemical composition of the catalysts under reaction conditions. A clear transition of Co3O4 → CoO → Co, and Ce4+ to Ce3+, was observed during the temperature programmed reduction under H2 and CH4. However, introduction of CO2, led to partial re-oxidation of all components at low temperatures, followed by reduction at high temperatures. Under optimum CO and H2 producing conditions both XRD and AP-XPS indicated that the active phase involved a majority of metallic Co with a small amount of CoO both supported on a partially reduced ceria (Ce3+/Ce4+). We identified the importance of dispersing Co, anchoring it onto ceria surface sites, and then utilizing the redox properties of ceria for activating and then oxidatively converting methane while inhibiting coke formation. Furthermore, a synergistic effect between cobalt and ceria and the interfacial site are essential to successfully close the catalytic cycle.
dc.format.extent11 p.
dc.language.isoeng
dc.subjectÀrees temàtiques de la UPC::Enginyeria química
dc.subject.lcshCobalt
dc.subject.lcshCerium oxides
dc.subject.lcshMethane
dc.subject.othercobalt
dc.subject.otherceria
dc.subject.otherin situ XRD
dc.subject.otherAP-XPS
dc.subject.othermethane dry reforming
dc.titleIn situ elucidation of the active state of Co-CeOx catalysts in the dry reforming of methane: the important role of the reducible oxide support and interactions with cobalt
dc.typeArticle
dc.subject.lemacCobalt
dc.subject.lemacMetà -- Anàlisi
dc.subject.lemacMetà
dc.contributor.groupUniversitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia
dc.identifier.doi10.1021/acscatal.7b03640
dc.description.peerreviewedPeer Reviewed
dc.rights.accessOpen Access
drac.iddocument23169997
dc.description.versionPostprint (author's final draft)
upcommons.citation.authorZhang, F.; Liu, Z.; Zhang, S.; Akter, N.; Palomino, R.; Vovchok, D.; Orozco, I.; Salazar, D.; Rodriguez, J.; Llorca, J.; Lee, J.; Kim, .; Xu, W.; Frenkel, A.; Li, Y.; Kim, T.; Senanayake, S.
upcommons.citation.publishedtrue
upcommons.citation.publicationNameACS catalysis
upcommons.citation.volume8
upcommons.citation.number4
upcommons.citation.startingPage3550
upcommons.citation.endingPage3560


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