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dc.contributor.authorVentura Espinosa, David
dc.contributor.authorVicent Barrera, Cristian
dc.contributor.authorBaya, Miguel
dc.contributor.authorMata Martínez, Jose A
dc.date.accessioned2016-10-17T11:20:26Z
dc.date.available2016-10-17T11:20:26Z
dc.date.issued2016-09
dc.identifier.citationVENTURA-ESPINOSA, David, et al. Ruthenium molecular complexes immobilized on graphene as active catalysts for the synthesis of carboxylic acids from alcohol dehydrogenation. Catalysis Science & Technology, 2016.ca_CA
dc.identifier.issn2044-4753
dc.identifier.issn2044-4761
dc.identifier.urihttp://hdl.handle.net/10234/163626
dc.description.abstractRuthenium complexes containing N-heterocyclic carbene ligands functionalized with different polyaromatic groups (pentafluorophenyl, anthracene, and pyrene) are immobilized onto the surface of reduced graphene oxide. The hybrid materials composed of organometallic complexes and graphene are obtained in a single-step process. The hybrid materials are efficient catalysts for the synthesis of carboxylic acids from the dehydrogenation of alcohols in aqueous media. The catalytic materials can be recycled up to ten times without significant loss of activity. The catalytic activity of the pyrene derivative, Pyr-Ru (3) is enhanced when the ruthenium complex is anchored onto the surface of graphene. The carbonaceous material limits the degradation of the ruthenium complex resulting in increased activity and requiring lower catalyst loadings. The catalytic process of the pyrene hybrid material is heterogeneous in nature due to the strong interaction between the pyrene and graphene. The catalytic process of the anthracene and pentafluorophenyl hybrid materials is governed by the so-called ‘boomerang effect’. The ruthenium molecular complex is released from and returned to the graphene surface during the catalytic reaction. Mechanistic insight has been obtained experimentally and theoretically. The energy profile suggests that the rate-determining step is the water nucleophilic attack to a coordinated aldehyde complex to form a gem-diolate complex.ca_CA
dc.description.sponsorShipThe authors thank the financial support from MINECO (CTQ2015-69153-C2-2-R and CTQ2015- 67461-P), Generalitat Valenciana (AICO/2015/039), Universitat Jaume I (P1.1B2015-09) and Universidad de Zaragoza (UZ2014-CIE-01).
dc.format.extent24 p.ca_CA
dc.format.mimetypeapplication/pdfca_CA
dc.language.isoengca_CA
dc.publisherRoyal Society of Chemistryca_CA
dc.relation.isPartOfCatalysis Science & Technology, 2016ca_CA
dc.rightsThis is an Accepted Manuscript, which has been through the Royal Society of Chemistry peer review process and has been accepted for publication: D. Ventura-Espinosa, C. Vicent, M. Baya and J. A. A. Mata Martínez, Catalysis Science & Technology, 2016, DOI: 10.1039/C6CY01455K.ca_CA
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/*
dc.subjectsupported catalysisca_CA
dc.subjectacceptorless alcohol dehydrogenationca_CA
dc.subjectsynthesis of carboxylic acidsca_CA
dc.subjectgrapheneca_CA
dc.subjectrutheniumca_CA
dc.subjectN-heterocyclic carbenesca_CA
dc.titleRuthenium molecular complexes immobilized on graphene as active catalysts for the synthesis of carboxylic acids from alcohol dehydrogenationca_CA
dc.typeinfo:eu-repo/semantics/articleca_CA
dc.identifier.doihttp://dx.doi.org/10.1039/C6CY01455K
dc.rights.accessRightsinfo:eu-repo/semantics/openAccessca_CA
dc.relation.publisherVersionhttp://pubs.rsc.org/en/content/articlelanding/2016/cy/c6cy01455k#!divAbstractca_CA


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