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dc.contributor.author | Lu, Jing | es_ES |
dc.contributor.author | Serna Merino, Pedro Manuel | es_ES |
dc.contributor.author | Aydin, Ceren | es_ES |
dc.contributor.author | Browning, Nigel D. | es_ES |
dc.contributor.author | Gates, Bruce C. | es_ES |
dc.date.accessioned | 2013-05-08T10:58:46Z | |
dc.date.issued | 2011-08 | |
dc.identifier.issn | 0002-7863 | |
dc.identifier.uri | http://hdl.handle.net/10251/28677 | |
dc.description.abstract | [EN] The performance of a supported catalyst is influenced by the size and structure of the metal species, the ligands bonded to the metal, and the support. Resolution of these effects has been lacking because of the lack of investigations of catalysts with uniform and systematically varied catalytic sites. We now demonstrate that the performance for ethene hydrogenation of isostructural iridium species on supports with contrasting properties as ligands (electron-donating MgO and electron-withdrawing HY zeolite) can be elucidated on the basis of molecular concepts. Spectra of the working catalysts show that the catalytic reaction rate is determined by the dissociation of H-2 when the iridium, either as mono- or tetra-nuclear species, is supported on MgO and is not when the support is the zeolite. The neighboring iridium sites in clusters are crucial for activation of both H-2 and C2H4 when the support is MgO but not when it is the zeolite, because the electron-withdrawing properties of the zeolite support enable even single site-isolated Ir atoms to bond to both C2H4 and H-2 and facilitate the catalysis. | es_ES |
dc.description.sponsorship | This research was supported by the DOE (Basic Energy Sciences, Contract FG02-04ER15513) (J.L. and C.A.). The research leading to these results has received funding from the European Union Seventh Framework Programme (FP7/2007-2013) under grant agreement no. PIOF-GA-2009-253129 (P.S.) We acknowledge beam time and the support of the DOE Division of Materials Sciences for its role in the operation and development of beamlines MR-CAT and Sector 9 at the Advanced Photon Source at Argonne National Laboratory. We thank Rodrigo Lobo-Lapidus, Tomohiro Shibata, and Trudy Bolin for valuable support. | |
dc.language | Inglés | es_ES |
dc.publisher | American Chemical Society | es_ES |
dc.relation.ispartof | Journal of the American Chemical Society | es_ES |
dc.rights | Reserva de todos los derechos | es_ES |
dc.title | Supported Molecular Iridium Catalysts: Resolving Effects of Metal Nuclearity and Supports as Ligands | es_ES |
dc.type | Artículo | es_ES |
dc.embargo.lift | 10000-01-01 | |
dc.embargo.terms | forever | es_ES |
dc.identifier.doi | 10.1021/ja206486j | |
dc.relation.projectID | info:eu-repo/grantAgreement/EC/FP7/253129/EU/Study of uniform supported metal complexes and metal clusters at atomic level for catalytic applications/ | en_EN |
dc.relation.projectID | info:eu-repo/grantAgreement/DOE//FG02-04ER15513/ | es_ES |
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 | Lu, J.; Serna Merino, PM.; Aydin, C.; Browning, ND.; Gates, BC. (2011). Supported Molecular Iridium Catalysts: Resolving Effects of Metal Nuclearity and Supports as Ligands. Journal of the American Chemical Society. 133(40):16186-16195. https://doi.org/10.1021/ja206486j | es_ES |
dc.description.accrualMethod | S | es_ES |
dc.relation.publisherversion | http://dx.doi.org/10.1021/ja206486j | es_ES |
dc.description.upvformatpinicio | 16186 | es_ES |
dc.description.upvformatpfin | 16195 | es_ES |
dc.type.version | info:eu-repo/semantics/publishedVersion | es_ES |
dc.description.volume | 133 | es_ES |
dc.description.issue | 40 | es_ES |
dc.relation.senia | 224126 | |
dc.identifier.pmid | 21866969 | |
dc.contributor.funder | European Commission | |
dc.contributor.funder | U.S. Department of Energy |