Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room Temperature

A semi-crystalline iron-based metal-organic framework (MOF), in particular Fe-BTC, that contained 20 wt.% Fe, was sustainably synthesized at room temperature and extensively characterized. Fe-BTC nanopowders could be used as an efficient heterogeneous catalyst for the synthesis of dihydroxybenzenes...

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Autores: Salazar-Aguilar, Alma D., Vega, Gonzalo, Casas, José A., Vega-Díaz, Sofía Magdalena, Tristan, Ferdinando, Meneses-Rodríguez, David, Belmonte, Manuel, Quintanilla, Asunción
Tipo de documento: artigo
Data de publicação:2020
País:España
Recursos:Consejo Superior de Investigaciones Científicas (CSIC)
Repositório:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/202393
Acesso em linha:http://hdl.handle.net/10261/202393
Access Level:Acceso aberto
Palavra-chave:Fe-BTC
MOF
Phenol hydroxylation
Dihydroxybenzenes
Selective oxidation
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spelling Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room TemperatureSalazar-Aguilar, Alma D.Vega, GonzaloCasas, José A.Vega-Díaz, Sofía MagdalenaTristan, FerdinandoMeneses-Rodríguez, DavidBelmonte, ManuelQuintanilla, AsunciónFe-BTCMOFPhenol hydroxylationDihydroxybenzenesSelective oxidationA semi-crystalline iron-based metal-organic framework (MOF), in particular Fe-BTC, that contained 20 wt.% Fe, was sustainably synthesized at room temperature and extensively characterized. Fe-BTC nanopowders could be used as an efficient heterogeneous catalyst for the synthesis of dihydroxybenzenes (DHBZ), from phenol with hydrogen peroxide (H2O2), as oxidant under organic solvent-free conditions. The influence of the reaction temperature, H2O2 concentration and catalyst dose were studied in the hydroxylation performance of phenol and MOF stability. Fe-BTC was active and stable (with negligible Fe leaching) at room conditions. By using intermittent dosing of H2O2, the catalytic performance resulted in a high DHBZ selectivity (65%) and yield (35%), higher than those obtained for other Fe-based MOFs that typically require reaction temperatures above 70 °C. The long-term experiments in a fixed-bed flow reactor demonstrated good Fe-BTC durability at the above conditions.The authors thank the financial support by Consejo Nacional de Ciencia y Tecnología (CONACYT) for the grant number 764635 and the project 256296; and to TNM for the supporting project 5627.19.P. Also, to the Spanish Ministerio de Ciencia, Innovación y Universidades (MICINN) and FEDER program (EU) through the projects: CTM2016-76454-R (MICINN) and RTI2018-095052-B-I00 ((MCIU/AEI/FEDER, UE).Multidisciplinary Digital Publishing InstituteConsejo Nacional de Ciencia y Tecnología (México)Ministerio de Ciencia, Innovación y Universidades (España)Ministerio de Economía y Competitividad (España)Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]2020202020202020info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501http://hdl.handle.net/10261/202393reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020RTI2018-095052-B-I00/info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/https://doi.org/10.3390/catal10020172Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/2023932026-05-22T06:33:51Z
dc.title.none.fl_str_mv Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room Temperature
title Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room Temperature
spellingShingle Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room Temperature
Salazar-Aguilar, Alma D.
Fe-BTC
MOF
Phenol hydroxylation
Dihydroxybenzenes
Selective oxidation
title_short Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room Temperature
title_full Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room Temperature
title_fullStr Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room Temperature
title_full_unstemmed Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room Temperature
title_sort Direct Hydroxylation of Phenol to Dihydroxybenzenes by H2O2 and Fe-based Metal-Organic Framework Catalyst at Room Temperature
dc.creator.none.fl_str_mv Salazar-Aguilar, Alma D.
Vega, Gonzalo
Casas, José A.
Vega-Díaz, Sofía Magdalena
Tristan, Ferdinando
Meneses-Rodríguez, David
Belmonte, Manuel
Quintanilla, Asunción
author Salazar-Aguilar, Alma D.
author_facet Salazar-Aguilar, Alma D.
Vega, Gonzalo
Casas, José A.
Vega-Díaz, Sofía Magdalena
Tristan, Ferdinando
Meneses-Rodríguez, David
Belmonte, Manuel
Quintanilla, Asunción
author_role author
author2 Vega, Gonzalo
Casas, José A.
Vega-Díaz, Sofía Magdalena
Tristan, Ferdinando
Meneses-Rodríguez, David
Belmonte, Manuel
Quintanilla, Asunción
author2_role author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Consejo Nacional de Ciencia y Tecnología (México)
Ministerio de Ciencia, Innovación y Universidades (España)
Ministerio de Economía y Competitividad (España)
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Fe-BTC
MOF
Phenol hydroxylation
Dihydroxybenzenes
Selective oxidation
topic Fe-BTC
MOF
Phenol hydroxylation
Dihydroxybenzenes
Selective oxidation
description A semi-crystalline iron-based metal-organic framework (MOF), in particular Fe-BTC, that contained 20 wt.% Fe, was sustainably synthesized at room temperature and extensively characterized. Fe-BTC nanopowders could be used as an efficient heterogeneous catalyst for the synthesis of dihydroxybenzenes (DHBZ), from phenol with hydrogen peroxide (H2O2), as oxidant under organic solvent-free conditions. The influence of the reaction temperature, H2O2 concentration and catalyst dose were studied in the hydroxylation performance of phenol and MOF stability. Fe-BTC was active and stable (with negligible Fe leaching) at room conditions. By using intermittent dosing of H2O2, the catalytic performance resulted in a high DHBZ selectivity (65%) and yield (35%), higher than those obtained for other Fe-based MOFs that typically require reaction temperatures above 70 °C. The long-term experiments in a fixed-bed flow reactor demonstrated good Fe-BTC durability at the above conditions.
publishDate 2020
dc.date.none.fl_str_mv 2020
2020
2020
2020
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/202393
url http://hdl.handle.net/10261/202393
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020RTI2018-095052-B-I00/
info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/
https://doi.org/10.3390/catal10020172
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Multidisciplinary Digital Publishing Institute
publisher.none.fl_str_mv Multidisciplinary Digital Publishing Institute
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.228081

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