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dc.contributor.author | Prieto González, Gonzalo | es_ES |
dc.contributor.author | Concepción Heydorn, Patricia | es_ES |
dc.contributor.author | Martinez Feliu, Agustin | es_ES |
dc.contributor.author | Mendoza, Ernest | es_ES |
dc.date.accessioned | 2016-09-29T07:25:19Z | |
dc.date.available | 2016-09-29T07:25:19Z | |
dc.date.issued | 2011-06-13 | |
dc.identifier.issn | 0021-9517 | |
dc.identifier.uri | http://hdl.handle.net/10251/70604 | |
dc.description.abstract | [EN] A series of 2.5% Rh/M@Al2O3 model catalysts were prepared by supporting Rh on high-area gamma-Al2O3, resulting in a surface covered by a monolayer (4.5-7 atoms/nm(2)) of MO promoter oxides (M = Fe, V. Nb, Ta, Ti, Y, Pr, Nd, Sm). The catalysts were extensively characterized and evaluated for the conversion of synthesis gas to oxygenates at 553 K, 5.0 MPa, H-2/CO = 1, and space velocity adjusted to attain CO conversion around 15%. The broad range of products formed depending on the specific promoter were, for the first time, quantitatively described using the selectivity parameter (Phi) defined here, which indicates, for a given reaction product, the contribution of carbon atoms derived from dissociative (C-dis) and nondissociative (C-ins) activation of CO. Both the catalytic activity and, more interestingly, the selectivity pattern given by the Phi parameter were correlated with the electronic properties of the MOx promoters (i.e., electron-donating/electron-withdrawing capacity) for an extensive series of catalysts. Low-temperature and at-work CO-FTIR experiments suggested that the high activity and hydrocarbon selectivity displayed by catalysts promoted by more electron-withdrawing (acidic) oxide promoters (e.g., TaOx) were related to a higher proportion of bridged Rh-2(CO)(B) adsorption sites and to a higher electron density (i.e., a higher electron back-donation ability) of the Rh-0 surface sites, both factors promoting CO dissociation events. In contrast, linear CO adsorption on Rh-0 sites displaying decreased electron back-donation in catalysts promoted by electron-donating (basic) oxides (e.g., PrOx, SmOx) was likely related to nondissociative CO activation and thus to the selective formation of oxygenates. TEM. XPS, and CO-FTIR results pointed to differences in morphology, rather than size or partial electronic charge, of the nano-sized Rh-0 crystallites as the likely cause for the different proportions of CO adsorption sites. The Rh NP morphology, both as-reduced and at-work, is a function of the electronic properties of the underlying promoter oxide. (C) 2011 Elsevier Inc. All rights reserved. | es_ES |
dc.language | Inglés | es_ES |
dc.publisher | Elsevier | es_ES |
dc.relation.ispartof | Journal of Catalysis | es_ES |
dc.rights | Reserva de todos los derechos | es_ES |
dc.subject | Synthesis gas | es_ES |
dc.subject | Oxygenates | es_ES |
dc.subject | Rhodium | es_ES |
dc.subject | Promoters | es_ES |
dc.subject | Electronic properties | es_ES |
dc.subject | Model catalysts | es_ES |
dc.subject | At-work CO-FTIR | es_ES |
dc.title | New insights into the role of the electronic properties of oxide promoters in Rh-catalyzed selective synthesis of oxygenates from synthesis gas | es_ES |
dc.type | Artículo | es_ES |
dc.identifier.doi | 10.1016/j.jcat.2011.03.025 | |
dc.rights.accessRights | Cerrado | es_ES |
dc.contributor.affiliation | Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química | es_ES |
dc.description.bibliographicCitation | Prieto González, G.; Concepción Heydorn, P.; Martinez Feliu, A.; Mendoza, E. (2011). New insights into the role of the electronic properties of oxide promoters in Rh-catalyzed selective synthesis of oxygenates from synthesis gas. Journal of Catalysis. 280(2):274-288. doi:10.1016/j.jcat.2011.03.025 | es_ES |
dc.description.accrualMethod | S | es_ES |
dc.relation.publisherversion | https://dx.doi.org/10.1016/j.jcat.2011.03.025 | es_ES |
dc.description.upvformatpinicio | 274 | es_ES |
dc.description.upvformatpfin | 288 | es_ES |
dc.type.version | info:eu-repo/semantics/publishedVersion | es_ES |
dc.description.volume | 280 | es_ES |
dc.description.issue | 2 | es_ES |
dc.relation.senia | 217696 | es_ES |