Ruthenium molecular complexes immobilized on graphene as active catalysts for the synthesis of carboxylic acids from alcohol dehydrogenation
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Otros documentos de la autoría: Ventura Espinosa, David; Vicent Barrera, Cristian; Baya, Miguel; Mata Martínez, Jose A
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Título
Ruthenium molecular complexes immobilized on graphene as active catalysts for the synthesis of carboxylic acids from alcohol dehydrogenationFecha de publicación
2016-09Editor
Royal Society of ChemistryISSN
2044-4753; 2044-4761Cita bibliográfica
VENTURA-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.Tipo de documento
info:eu-repo/semantics/articleVersión de la editorial
http://pubs.rsc.org/en/content/articlelanding/2016/cy/c6cy01455k#!divAbstractPalabras clave / Materias
Resumen
Ruthenium complexes containing N-heterocyclic carbene ligands functionalized
with different polyaromatic groups (pentafluorophenyl, anthracene, and pyrene) are
immobilized onto the surface of reduced graphene oxide. ... [+]
Ruthenium 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. [-]
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Catalysis Science & Technology, 2016Derechos de acceso
This 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.
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info:eu-repo/semantics/openAccess
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