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Tuning the Microenvironment of Gold Nanoparticles Encapsulated within MIL-101(Cr) for the Selective Oxidation of Alcohols with O-2: Influence of the Amino Terephthalate Linker

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Tuning the Microenvironment of Gold Nanoparticles Encapsulated within MIL-101(Cr) for the Selective Oxidation of Alcohols with O-2: Influence of the Amino Terephthalate Linker

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dc.contributor.author Santiago-Portillo, Andrea es_ES
dc.contributor.author Cabrero-Antonino, Maria es_ES
dc.contributor.author Alvaro Rodríguez, Maria Mercedes es_ES
dc.contributor.author Navalón Oltra, Sergio es_ES
dc.contributor.author García Gómez, Hermenegildo es_ES
dc.date.accessioned 2020-11-18T04:31:25Z
dc.date.available 2020-11-18T04:31:25Z
dc.date.issued 2019-07-11 es_ES
dc.identifier.issn 0947-6539 es_ES
dc.identifier.uri http://hdl.handle.net/10251/155238
dc.description This is the peer reviewed version of the following article: Chem. Eur. J. 2019, 25, 9280 9286, which has been published in final form at https://doi.org/10.1002/chem.201901361. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving. es_ES
dc.description.abstract [EN] This manuscript reports a comparative study of the catalytic performance of gold nanoparticles (NPs) encapsulated within MIL-101(Cr) with or without amino groups in the terephthalate linker. The purpose is to show how the amino groups can influence the microenvironment and catalytic stability of incorporated gold nanoparticles. The first influence of the presence of this substituent is the smaller particle size of Au NPs hosted in MIL-101(Cr)-NH2 (2.45 +/- 0.19 nm) compared with the parent MIL-101(Cr)-H (3.02 +/- 0.39 nm). Both materials are highly active to promote the aerobic alcohol oxidation and exhibit a wide substrate scope. Although both catalysts can achieve turnover numbers as high as 10(6) for the solvent-free aerobic oxidation of benzyl alcohol, Au@MIL-101(Cr)-NH2 exhibits higher turnover frequency values (12 000 h(-1)) than Au@MIL-101(Cr)-H (6800 h(-1)). Au@MIL-101(Cr)-NH2 also exhibits higher catalytic stability, being recyclable for 20 times with coincident temporal conversion profiles, in comparison with some decay observed in the parent Au@MIL-101(Cr)-H. Characterization by transmission electron microscopy of the 20-times used samples shows a very minor particle size increase in the case of Au@MIL-101(Cr)-NH2 (2.97 +/- 0.27 nm) in comparison with the Au@MIL-101(Cr)-H analog (5.32 +/- 0.72 nm). The data presented show the potential of better control of the microenvironment to improve the performance of encapsulated Au nanoparticles. es_ES
dc.description.sponsorship Financial support by the Spanish Ministry of Economy and Competitiveness (Severo Ochoa, CTQ2015-65963-CQ-R1 and CTQ2014-53292-R) is gratefully acknowledged. Generalidad Valenciana is also thanked for funding (Prometeo 2017/083). S.N. thanks financial support by the Fundación Ramón Areces (XVIII Concurso Nacional para la Adjudicación de Ayudas a la Investigación en Ciencias de la Vida y de la Materia, 2016). es_ES
dc.language Inglés es_ES
dc.publisher John Wiley & Sons es_ES
dc.relation.ispartof Chemistry - A European Journal es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Aerobic oxidation es_ES
dc.subject Alcohol oxidation es_ES
dc.subject Gold catalysis es_ES
dc.subject Heterogeneous catalysis es_ES
dc.subject MIL-101(Cr)-NH2 es_ES
dc.subject.classification QUIMICA ORGANICA es_ES
dc.title Tuning the Microenvironment of Gold Nanoparticles Encapsulated within MIL-101(Cr) for the Selective Oxidation of Alcohols with O-2: Influence of the Amino Terephthalate Linker es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1002/chem.201901361 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//CTQ2014-53292-R/ES/MATERIALES GRAFENICOS COMO CATALIZADORES PARA REACCIONES ORGANICAS./ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//CTQ2015-69153-C2-1-R/ES/EXPLOTANDO EL USO DEL GRAFENO EN CATALISIS. USO DEL GRAFENO COMO CARBOCATALIZADOR O COMO SOPORTE/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/GVA//PROMETEO%2F2017%2F083/ es_ES
dc.rights.accessRights Abierto es_ES
dc.contributor.affiliation Universitat Politècnica de València. Departamento de Química - Departament de Química es_ES
dc.description.bibliographicCitation Santiago-Portillo, A.; Cabrero-Antonino, M.; Alvaro Rodríguez, MM.; Navalón Oltra, S.; García Gómez, H. (2019). Tuning the Microenvironment of Gold Nanoparticles Encapsulated within MIL-101(Cr) for the Selective Oxidation of Alcohols with O-2: Influence of the Amino Terephthalate Linker. Chemistry - A European Journal. 25(39):9280-9286. https://doi.org/10.1002/chem.201901361 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1002/chem.201901361 es_ES
dc.description.upvformatpinicio 9280 es_ES
dc.description.upvformatpfin 9286 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 25 es_ES
dc.description.issue 39 es_ES
dc.identifier.pmid 31063224 es_ES
dc.relation.pasarela S\398873 es_ES
dc.contributor.funder Generalitat Valenciana es_ES
dc.contributor.funder Fundación Ramón Areces es_ES
dc.contributor.funder Ministerio de Economía y Competitividad es_ES
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