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

[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 o...

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Autores: Santiago-Portillo, Andrea, Cabrero-Antonino, Maria, Alvaro Rodríguez, Maria Mercedes|||0000-0001-5070-4207, Navalón Oltra, Sergio|||0000-0001-8423-0759, García Gómez, Hermenegildo|||0000-0002-9664-493X
Tipo de recurso: artículo
Fecha de publicación:2019
País:España
Institución:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:riunet.upv.es:10251/155238
Acceso en línea:https://riunet.upv.es/handle/10251/155238
Access Level:acceso abierto
Palabra clave:Aerobic oxidation
Alcohol oxidation
Gold catalysis
Heterogeneous catalysis
MIL-101(Cr)-NH2
QUIMICA ORGANICA
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repository_id_str
spelling 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 LinkerSantiago-Portillo, AndreaCabrero-Antonino, MariaAlvaro Rodríguez, Maria Mercedes|||0000-0001-5070-4207Navalón Oltra, Sergio|||0000-0001-8423-0759García Gómez, Hermenegildo|||0000-0002-9664-493XAerobic oxidationAlcohol oxidationGold catalysisHeterogeneous catalysisMIL-101(Cr)-NH2QUIMICA ORGANICA[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.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).John Wiley & SonsInstituto Universitario Mixto de Tecnología QuímicaDepartamento de QuímicaEscuela Técnica Superior de Ingeniería IndustrialGrupo de Fotoquímica Heterogénea y MedioambientalGeneralitat ValencianaFundación Ramón ArecesMinisterio de Economía y CompetitividadRepositorio Institucional de la Universitat Politècnica de València Riunet20192019-07-11journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfapplication/pdfhttps://riunet.upv.es/handle/10251/155238reponame:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valénciainstname:Universitat Politècnica de València (UPV)InglésengMinisterio de Economía y Competitividad http://dx.doi.org/10.13039/501100003329 CTQ2015-69153-C2-1-R EXPLOTANDO EL USO DEL GRAFENO EN CATALISIS. USO DEL GRAFENO COMO CARBOCATALIZADOR O COMO SOPORTEMinisterio de Economía y Competitividad http://dx.doi.org/10.13039/501100003329 CTQ2014-53292-R MATERIALES GRAFENICOS COMO CATALIZADORES PARA REACCIONES ORGANICAS.Generalitat Valenciana https://doi.org/10.13039/501100003359 PROMETEO%2F2017%2F083open accesshttp://purl.org/coar/access_right/c_abf2Reserva de todos los derechoshttp://rightsstatements.org/vocab/InC/1.0/info:eu-repo/semantics/openAccessoai:riunet.upv.es:10251/1552382026-06-13T07:49:27Z
dc.title.none.fl_str_mv 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
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
spellingShingle 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
Santiago-Portillo, Andrea
Aerobic oxidation
Alcohol oxidation
Gold catalysis
Heterogeneous catalysis
MIL-101(Cr)-NH2
QUIMICA ORGANICA
title_short 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
title_full 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
title_fullStr 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
title_full_unstemmed 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
title_sort 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
dc.creator.none.fl_str_mv Santiago-Portillo, Andrea
Cabrero-Antonino, Maria
Alvaro Rodríguez, Maria Mercedes|||0000-0001-5070-4207
Navalón Oltra, Sergio|||0000-0001-8423-0759
García Gómez, Hermenegildo|||0000-0002-9664-493X
author Santiago-Portillo, Andrea
author_facet Santiago-Portillo, Andrea
Cabrero-Antonino, Maria
Alvaro Rodríguez, Maria Mercedes|||0000-0001-5070-4207
Navalón Oltra, Sergio|||0000-0001-8423-0759
García Gómez, Hermenegildo|||0000-0002-9664-493X
author_role author
author2 Cabrero-Antonino, Maria
Alvaro Rodríguez, Maria Mercedes|||0000-0001-5070-4207
Navalón Oltra, Sergio|||0000-0001-8423-0759
García Gómez, Hermenegildo|||0000-0002-9664-493X
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Instituto Universitario Mixto de Tecnología Química
Departamento de Química
Escuela Técnica Superior de Ingeniería Industrial
Grupo de Fotoquímica Heterogénea y Medioambiental
Generalitat Valenciana
Fundación Ramón Areces
Ministerio de Economía y Competitividad
Repositorio Institucional de la Universitat Politècnica de València Riunet
dc.subject.none.fl_str_mv Aerobic oxidation
Alcohol oxidation
Gold catalysis
Heterogeneous catalysis
MIL-101(Cr)-NH2
QUIMICA ORGANICA
topic Aerobic oxidation
Alcohol oxidation
Gold catalysis
Heterogeneous catalysis
MIL-101(Cr)-NH2
QUIMICA ORGANICA
description [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.
publishDate 2019
dc.date.none.fl_str_mv 2019
2019-07-11
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://riunet.upv.es/handle/10251/155238
url https://riunet.upv.es/handle/10251/155238
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Ministerio de Economía y Competitividad http://dx.doi.org/10.13039/501100003329 CTQ2015-69153-C2-1-R EXPLOTANDO EL USO DEL GRAFENO EN CATALISIS. USO DEL GRAFENO COMO CARBOCATALIZADOR O COMO SOPORTE
Ministerio de Economía y Competitividad http://dx.doi.org/10.13039/501100003329 CTQ2014-53292-R MATERIALES GRAFENICOS COMO CATALIZADORES PARA REACCIONES ORGANICAS.
Generalitat Valenciana https://doi.org/10.13039/501100003359 PROMETEO%2F2017%2F083
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reserva de todos los derechos
http://rightsstatements.org/vocab/InC/1.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reserva de todos los derechos
http://rightsstatements.org/vocab/InC/1.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv John Wiley & Sons
publisher.none.fl_str_mv John Wiley & Sons
dc.source.none.fl_str_mv reponame:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
instname:Universitat Politècnica de València (UPV)
instname_str Universitat Politècnica de València (UPV)
reponame_str RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
collection RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,300724

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