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Surface-Mediated Synthesis of Dimeric Rhodium Catalysts on MgO: Tracking Changes in the Nuclearity and Ligand Environment of the Catalytically Active Sites by X-ray Absorption and Infrared Spectroscopies

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Surface-Mediated Synthesis of Dimeric Rhodium Catalysts on MgO: Tracking Changes in the Nuclearity and Ligand Environment of the Catalytically Active Sites by X-ray Absorption and Infrared Spectroscopies

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dc.contributor.author Yardimci, Dicle es_ES
dc.contributor.author Serna Merino, Pedro Manuel es_ES
dc.contributor.author Gates, Bruce C. es_ES
dc.date.accessioned 2016-06-24T09:36:53Z
dc.date.available 2016-06-24T09:36:53Z
dc.date.issued 2013-01
dc.identifier.issn 0947-6539
dc.identifier.uri http://hdl.handle.net/10251/66415
dc.description.abstract [EN] The preparation of dinuclear rhodium clusters and their use as catalysts is challenging because these clusters are unstable, evolving readily into species with higher nuclearities. We now present a novel synthetic route to generate rhodium dimers on the surface of MgO by a stoichiometrically simple surface-mediated reaction involving [Rh(C2H4)2] species and H2. X-ray absorption and IR spectra were used to characterize the changes in the nuclearity of the essentially molecular surface species as they formed, including the ligands on the rhodium and the metal-support interactions. The support plays a key role in stabilizing the dinuclear rhodium species, allowing the incorporation of small ligands (ethyl, hydride, and/or CO) and enabling a characterization of the catalytic performance of the supported species for the hydrogenation of ethylene as a function of the metal nuclearity and ligand environment. A change in the nuclearity from one to two Rh atoms leads to a 58-fold increase in the catalytic activity for ethylene hydrogenation, a reaction involving unsaturated, but stable, dimeric rhodium species. es_ES
dc.description.sponsorship The research was supported by the European Union Seventh Framework Programme (FP7/2007-2013) under grant agreement no. PIOF-GA-2009-253129 (P. S.) and by DOE Basic Energy Sciences (Contract No. FG02-04ER15513) (D.Y.). We thank the DOE Division of Materials Sciences for its role in the operation and development of beam line 4-1 at the Stanford Synchrotron Radiation Lightsource. We thank the beamline staff for valuable support.
dc.language Inglés es_ES
dc.publisher Wiley es_ES
dc.relation DOE/FG02-04ER15513 es_ES
dc.relation.ispartof Chemistry - A European Journal es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Catalysis es_ES
dc.subject Cluster compounds es_ES
dc.subject Dimerization es_ES
dc.subject Hydrogenation es_ES
dc.subject Rhodium es_ES
dc.subject Supported catalysts es_ES
dc.title Surface-Mediated Synthesis of Dimeric Rhodium Catalysts on MgO: Tracking Changes in the Nuclearity and Ligand Environment of the Catalytically Active Sites by X-ray Absorption and Infrared Spectroscopies es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1002/chem.201202514
dc.relation.projectID info:eu-repo/grantAgreement/EC/FP7/253129/EU
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 Yardimci, D.; Serna Merino, PM.; Gates, BC. (2013). Surface-Mediated Synthesis of Dimeric Rhodium Catalysts on MgO: Tracking Changes in the Nuclearity and Ligand Environment of the Catalytically Active Sites by X-ray Absorption and Infrared Spectroscopies. Chemistry - A European Journal. 19(4):1235-1245. doi:10.1002/chem.201202514 es_ES
dc.description.accrualMethod Senia es_ES
dc.relation.publisherversion http://dx.doi.org/10.1002/chem.201202514 es_ES
dc.description.upvformatpinicio 1235 es_ES
dc.description.upvformatpfin 1245 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 19 es_ES
dc.description.issue 4 es_ES
dc.relation.senia 252856 es_ES
dc.identifier.pmid 23208893
dc.contributor.funder European Commission
dc.contributor.funder Department of Energy, EEUU (DOE)


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