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The oxamate route, a versatile post-functionalization for metal incorporation in MIL-101(Cr): Catalytic applications of Cu, Pd, and Au

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The oxamate route, a versatile post-functionalization for metal incorporation in MIL-101(Cr): Catalytic applications of Cu, Pd, and Au

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dc.contributor.author Juan Alcañiz, Jana es_ES
dc.contributor.author Ferrando-Soria, Jesus es_ES
dc.contributor.author Luz Mínguez, Ignacio es_ES
dc.contributor.author Serra-Crespo, Pablo es_ES
dc.contributor.author Skupien, Emmanuel es_ES
dc.contributor.author Santos, Vera P. es_ES
dc.contributor.author Pardo, Emilio es_ES
dc.contributor.author Llabrés i Xamena, Francesc Xavier es_ES
dc.contributor.author Kapteijn, Freek es_ES
dc.contributor.author Gascon, Jorge es_ES
dc.date.accessioned 2016-10-31T13:16:48Z
dc.date.available 2016-10-31T13:16:48Z
dc.date.issued 2013-11
dc.identifier.issn 0021-9517
dc.identifier.uri http://hdl.handle.net/10251/73007
dc.description.abstract A new consecutive post-functionalization method has been developed for the inclusion of additional metal functionalities in Metal Organic Frameworks (MOFs) through oxamate as chelating agent. This may result in catalytic centers of metal organic complexes or in controlled formation of metal nanoparticles, demonstrated for Cu, Pd and Au, in the highly stable MIL-101(Cr) framework. In a first post-synthesis step, reduction of the NO2-MIL-101(Cr) leads to the formation of NH2-MIL-101(Cr). The second functionalization consists of a straightforward condensation of the amino groups of the ligand with ethyl chloro-oxoacetate resulting in the formation of free oxamates attached to the linker. Two different copper complexes have been coordinated through the oxamate ligand, attaining loadings as high as 9 wt.% and showing similar performance as the best reported copper MOFs (HKUST-1, [Cu(2-pymo)2] and [Cu(im)2]) in click chemistry catalysis (1,3-dipolar cycloaddition reactions) and multicomponent coupling reactions (propargylamine formation). Highly dispersed palladium and gold nanoparticles can be incorporated and stabilized in the MOF. The resultant Pd-catalysts are very active and selective in Suzuki Miyaura condensation, although palladium leaching is observed. After reduction of the Au-catalysts, immobilized gold nanoparticles are formed, which maintain a good performance in BA oxidation to benzaldehyde for at least 4 consecutive runs. No side reactions (further oxidation and esterification) are observed, which are attributed to the absence of any cationic gold species. TEM analysis and DRIFTS analysis during CO adsorption show the very uniform size (∼2 nm) and metallic character of these gold particles encapsulated in the MIL-101 cages. es_ES
dc.language Inglés es_ES
dc.publisher Elsevier es_ES
dc.relation.ispartof Journal of Catalysis es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Metal organic framework es_ES
dc.subject Post-functionalization es_ES
dc.subject Oxamate es_ES
dc.subject NH2-MIL-101(Cr) es_ES
dc.subject Metal complex es_ES
dc.subject Nanoparticles es_ES
dc.subject Palladium es_ES
dc.subject Copper es_ES
dc.subject Gold es_ES
dc.subject Heterogeneous catalysis es_ES
dc.title The oxamate route, a versatile post-functionalization for metal incorporation in MIL-101(Cr): Catalytic applications of Cu, Pd, and Au es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1016/j.jcat.2013.08.001
dc.rights.accessRights Cerrado es_ES
dc.contributor.affiliation Universitat Politècnica de València. Escuela Técnica Superior de Ingenieros Industriales - Escola Tècnica Superior d'Enginyers Industrials es_ES
dc.contributor.affiliation Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química es_ES
dc.description.bibliographicCitation Juan Alcañiz, J.; Ferrando-Soria, J.; Luz Minguez, I.; Serra-Crespo, P.; Skupien, E.; Santos, VP.; Pardo, E.... (2013). The oxamate route, a versatile post-functionalization for metal incorporation in MIL-101(Cr): Catalytic applications of Cu, Pd, and Au. Journal of Catalysis. 307:295-304. doi:10.1016/j.jcat.2013.08.001 es_ES
dc.description.accrualMethod Senia es_ES
dc.relation.publisherversion http://dx.doi.org/10.1016/j.jcat.2013.08.001 es_ES
dc.description.upvformatpinicio 295 es_ES
dc.description.upvformatpfin 304 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 307 es_ES
dc.relation.senia 247258 es_ES


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