000127881 001__ 127881
000127881 005__ 20231023120953.0
000127881 0247_ $$2doi$$a10.1021/acsanm.9b02398
000127881 0248_ $$2sideral$$a117656
000127881 037__ $$aART-2020-117656
000127881 041__ $$aeng
000127881 100__ $$0(orcid)0000-0001-6675-7450$$aSanchez-Page, B.
000127881 245__ $$aHybrid Catalysts Comprised of Graphene Modified with Rhodium-Based N-Heterocyclic Carbenes for Alkyne Hydrosilylation
000127881 260__ $$c2020
000127881 5060_ $$aAccess copy available to the general public$$fUnrestricted
000127881 5203_ $$aThermally partially reduced graphene oxide has been covalently modified with 3-methyl-4-phenyl-1, 2, 3-triazolium salts making use of the epoxy functionalities on the carbon nanomaterial. Characterization of the functionalized materials through adequate solid characterization techniques, particularly X-ray photoelectron spectroscopy (XPS), allows one to follow the stepwise building up of the triazolium fragments on the graphene oxide attached to the wall via covalent C-N linkage. The hydroxyl-triazolium-functionalized materials have been used to prepare rhodium hybrid materials containing either alkoxo or triazolylidene molecular rhodium(I) complexes depending on the protection of the hydroxyl groups present in the material. Characterization of the heterogeneous systems, especially by means of XPS and extended X-ray absorption fine structure (EXAFS) spectroscopy, has evidenced the coordination sphere of the supported rhodium(I) complexes in both rhodium hybrid materials. The graphene-oxide-supported rhodium triazolylidene hybrid catalysts show excellent activity, comparable to that of the homogeneous [RhI(cod)(Triaz)] (Triaz = 1, 4-diphenyl-3-methyl-1, 2, 3-triazol-5-ylidene) catalyst, for the hydrosilylation of terminal and internal alkynes. In addition, these catalysts have shown good selectivity to the beta-(Z) vinylsilane isomers (for the not hindered terminal substrates) or syn-additions (for the internal substrates). In contrast to the rhodium(I)-alkoxo-based hybrid material, the silyl-protected rhodium(I)-triazolylidene-based hybrid catalyst can be reused in consecutive cycles without loss of activity maintaining the selectivity. The lack of leaching of active rhodium species demonstrates the strength of the C-N covalent bond of the triazolylidene linker to the graphitic wall.
000127881 536__ $$9info:eu-repo/grantAgreement/ES/DGA/E12-R17$$9info:eu-repo/grantAgreement/ES/DGA-FSE/Building Europe from Aragon$$9info:eu-repo/grantAgreement/ES/DGA-FSE/E42-17R$$9info:eu-repo/grantAgreement/ES/MICINN-FEDER/CTQ2016-75884-P$$9info:eu-repo/grantAgreement/ES/MICINN-FEDER/RTI2018-098537-B-C22
000127881 540__ $$9info:eu-repo/semantics/openAccess$$aby-nc-nd$$uhttp://creativecommons.org/licenses/by-nc-nd/3.0/es/
000127881 590__ $$a5.097$$b2020
000127881 591__ $$aNANOSCIENCE & NANOTECHNOLOGY$$b48 / 106 = 0.453$$c2020$$dQ2$$eT2
000127881 591__ $$aMATERIALS SCIENCE, MULTIDISCIPLINARY$$b101 / 333 = 0.303$$c2020$$dQ2$$eT1
000127881 592__ $$a1.227$$b2020
000127881 593__ $$aMaterials Science (miscellaneous)$$c2020$$dQ1
000127881 655_4 $$ainfo:eu-repo/semantics/article$$vinfo:eu-repo/semantics/acceptedVersion
000127881 700__ $$0(orcid)0000-0002-0545-9107$$aJimenez, M.V.$$uUniversidad de Zaragoza
000127881 700__ $$0(orcid)0000-0002-3327-0918$$aPerez-Torrente, J.J.$$uUniversidad de Zaragoza
000127881 700__ $$0(orcid)0000-0002-1735-6439$$aPassarelli, V.$$uUniversidad de Zaragoza
000127881 700__ $$0(orcid)0000-0002-9706-3272$$aBlasco, J.$$uUniversidad de Zaragoza
000127881 700__ $$0(orcid)0000-0002-9029-1977$$aSubias, G.$$uUniversidad de Zaragoza
000127881 700__ $$aGranda, M.
000127881 700__ $$aAlvarez, P.
000127881 7102_ $$12010$$2760$$aUniversidad de Zaragoza$$bDpto. Química Inorgánica$$cÁrea Química Inorgánica
000127881 7102_ $$12003$$2395$$aUniversidad de Zaragoza$$bDpto. Física Materia Condensa.$$cÁrea Física Materia Condensada
000127881 773__ $$g3, 2 (2020), 1640-1655$$pACS appl. nano mater.$$tACS APPLIED NANO MATERIALS$$x2574-0970
000127881 8564_ $$s2315343$$uhttps://zaguan.unizar.es/record/127881/files/texto_completo.pdf$$yPostprint
000127881 8564_ $$s887810$$uhttps://zaguan.unizar.es/record/127881/files/texto_completo.jpg?subformat=icon$$xicon$$yPostprint
000127881 909CO $$ooai:zaguan.unizar.es:127881$$particulos$$pdriver
000127881 951__ $$a2023-10-23-11:03:37
000127881 980__ $$aARTICLE