Graphene-NHC-iridium hybrid catalysts built through -OH covalent linkage Dedicated to the lasting Memory of Prof. Dr. María Pilar García for her valuable talent as human, teacher and chemist

Blanco,M. ; Álvarez,P. ; Blanco,C. ; Jiménez,M. V. (Universidad de Zaragoza) ; Fernández-Tornos,J. ; Pérez-Torrente,J. J. (Universidad de Zaragoza) ; Oro,L. A. (Universidad de Zaragoza) ; Menéndez,R.

Resumen: Graphene oxide (GO) and thermally reduced graphene oxide (TRGO) were covalently modified with imidazolium salts through their hydroxyl surface groups. The selective reaction of the -OH groups with p-nitrophenylchloroformate produced labile intermediate organic carbonate functions which were used for the covalent anchoring of a hydroxy-functionalized imidazolium salt. Nanohybrid materials containing iridium N-heterocyclic carbene (NHC)-type organometallic complexes were prepared by causing the imidazolium-functionalized materials to react with Ir(µ-OMe)(cod)]2. The iridium content of the graphene-based hybrid catalysts, as determined by XPS and ICP-MS was the order of ~5 and 10 wt.%, for the TRGO and GO-based materials, respectively. The graphene-supported iridium hybrid materials were active in the heterogeneous hydrogen-transfer reduction of cyclohexanone to cyclohexanol with 2-propanol/KOH as the hydrogen source. The thermally reduced graphene-NHC-iridium hybrid catalyst showed the best catalytic performance with an initial TOF of 11.500 h-1, slightly better than the related acetoxy-functionalized NHC iridium homogeneous catalyst. A good catalyst recyclability and stability were achieved.

Idioma: Inglés

DOI: 10.1016/j.carbon.2014.11.016

Año: 2015

Publicado en: Carbon 83 (2015), 21-31
ISSN: 0008-6223

Factor impacto JCR: 6.198 (2015)

Categ. JCR: MATERIALS SCIENCE, MULTIDISCIPLINARY rank: 27 / 270 = 0.1 (2015) - Q1 - T1
Categ. JCR: CHEMISTRY, PHYSICAL rank: 24 / 144 = 0.167 (2015) - Q1 - T1

Factor impacto SCIMAGO: 1.988 - Chemistry (miscellaneous) (Q1)

Financiación: info:eu-repo/grantAgreement/ES/MINECO/CSD2009-00050
Financiación: info:eu-repo/grantAgreement/ES/MINECO/CTQ2013-42532-P

Tipo y forma: Article (PostPrint)

Área (Departamento): Área Química Inorgánica (Dpto. Química Inorgánica)