Por favor, use este identificador para citar o enlazar a este item:
http://hdl.handle.net/10261/202935
COMPARTIR / EXPORTAR:
SHARE CORE BASE | |
Visualizar otros formatos: MARC | Dublin Core | RDF | ORE | MODS | METS | DIDL | DATACITE | |
Título: | Hybrid catalysts comprised of graphene modified with rhodium-based N-heterocyclic carbenes for alkyne hydrosilylation |
Autor: | Sánchez-Page, Beatriz CSIC ORCID; Jiménez, M. Victoria CSIC ORCID ; Pérez-Torrente, Jesús J. CSIC ORCID; Passarelli, Vincenzo CSIC ORCID; Blasco, Javier CSIC ORCID; Subías, G. CSIC ORCID; Granda Ferreira, Marcos CSIC ORCID ; Álvarez Rodríguez, Patricia CSIC ORCID | Palabras clave: | Graphene Covalent functionalization Hydrosilylation N-heterocyclic carbenes Rhodium |
Fecha de publicación: | 7-ene-2020 | Editor: | American Chemical Society | Citación: | ACS Applied Nano Materials 3(2): 1640-1655 (2020) | Resumen: | Thermally partially reduced graphene oxide has been covalently modified with 3-methyl-4-phenyl-1,2,3-triazolium salts making use of the epoxy functionalities on the carbon nanomaterial. Characterization of the functionalized materials through adequate solid characterization techniques, particularly X-ray photoelectron spectroscopy (XPS), allows one to follow the stepwise building up of the triazolium fragments on the graphene oxide attached to the wall via covalent C–N linkage. The hydroxyl-triazolium-functionalized materials have been used to prepare rhodium hybrid materials containing either alkoxo or triazolylidene molecular rhodium(I) complexes depending on the protection of the hydroxyl groups present in the material. Characterization of the heterogeneous systems, especially by means of XPS and extended X-ray absorption fine structure (EXAFS) spectroscopy, has evidenced the coordination sphere of the supported rhodium(I) complexes in both rhodium hybrid materials. The graphene-oxide-supported rhodium–triazolylidene hybrid catalysts show excellent activity, comparable to that of the homogeneous [RhI(cod)(Triaz)] (Triaz = 1,4-diphenyl-3-methyl-1,2,3-triazol-5-ylidene) catalyst, for the hydrosilylation of terminal and internal alkynes. In addition, these catalysts have shown good selectivity to the β-(Z) vinylsilane isomers (for the not hindered terminal substrates) or syn-additions (for the internal substrates). In contrast to the rhodium(I)–alkoxo-based hybrid material, the silyl-protected rhodium(I)–triazolylidene-based hybrid catalyst can be reused in consecutive cycles without loss of activity maintaining the selectivity. The lack of leaching of active rhodium species demonstrates the strength of the C–N covalent bond of the triazolylidene linker to the graphitic wall. | Descripción: | This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Nano Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsanm.9b02398 | Versión del editor: | https://doi.org/10.1021/acsanm.9b02398 | URI: | http://hdl.handle.net/10261/202935 | DOI: | 10.1021/acsanm.9b02398 | ISSN: | 2574-0970 |
Aparece en las colecciones: | (INCAR) Artículos (ICMA) Artículos (ISQCH) Artículos |
Ficheros en este ítem:
Fichero | Descripción | Tamaño | Formato | |
---|---|---|---|---|
Rh-NHC-Hybrid catalysts_Sanchez-Page.pdf | 2,44 MB | Adobe PDF | Visualizar/Abrir | |
Rh-NHC-Hybrid catalysts_Sanchez-Page_SI.pdf | Supplementary Information | 3,8 MB | Adobe PDF | Visualizar/Abrir |
CORE Recommender
SCOPUSTM
Citations
25
checked on 22-abr-2024
WEB OF SCIENCETM
Citations
19
checked on 21-feb-2024
Page view(s)
199
checked on 23-abr-2024
Download(s)
334
checked on 23-abr-2024
Google ScholarTM
Check
Altmetric
Altmetric
Este item está licenciado bajo una Licencia Creative Commons