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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.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.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.subjectÀrees temàtiques de la UPC::Enginyeria química
dc.subject.lcshCerium oxides
dc.subject.otherin situ XRD
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.subject.lemacMetà -- Anàlisi
dc.contributor.groupUniversitat Politècnica de Catalunya. NEMEN - Nanoenginyeria de materials aplicats a l'energia
dc.description.peerreviewedPeer Reviewed
dc.rights.accessOpen Access
dc.description.versionPostprint (author's final draft)
local.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.
local.citation.publicationNameACS catalysis

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