Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophen

This work reports for the first time the functionalization of the 2-aminoterephtalate linker of UiO-66-NH2 with cyclopentyl or cyclohexyl rings. The resulting materials displayed reduced bandgaps with enhanced separation of the photogenerated charges due to the inductive electron effect of the cyclo...

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Detalles Bibliográficos
Autores: Gómez-Avilés, A., Solís, R.R., García-Frutos, Eva M., Bedia, J., Belver, Carolina
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2023
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/350822
Acceso en línea:http://hdl.handle.net/10261/350822
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85148359975&doi=10.1016%2fj.cej.2023.141889&partnerID=40&md5=ae54058255619c3999c3d6a6ce99e9d1
Access Level:acceso abierto
Palabra clave:Acetaminophen
Linker functionalization
Photocatalysis
UiO-66-NH2
Water treatment
Dimers
Energy gap
Cyclohexyl rings
Electron effect
Functionalizations
Photocatalytic performance
Photogenerated charge
Resulting materials
Solar photocatalytic degradation
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spelling Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophenGómez-Avilés, A.Solís, R.R.García-Frutos, Eva M.Bedia, J.Belver, CarolinaAcetaminophenLinker functionalizationPhotocatalysisUiO-66-NH2Water treatmentDimersEnergy gapCyclohexyl ringsElectron effectFunctionalizationsPhotocatalytic performancePhotogenerated chargeResulting materialsSolar photocatalytic degradationUiO-66-NH2This work reports for the first time the functionalization of the 2-aminoterephtalate linker of UiO-66-NH2 with cyclopentyl or cyclohexyl rings. The resulting materials displayed reduced bandgaps with enhanced separation of the photogenerated charges due to the inductive electron effect of the cycloalkyl substituent. These functionalized materials displayed higher photocatalytic performance towards the solar abatement of acetaminophen than UiO-66-NH2. The photocatalytic activation mechanism was proposed based on the band alignment and scavenger tests, suggesting the major contribution of holes and superoxide radicals. In particular, UiO-66-NH-C5 exhibited high stability under reaction with low activity loss after reusing. The acetaminophen degradation pathway was also studied indicating that the ACE molecules were coupled to dimers and trimers that were further oxidized. The small bandgap, the band structure, and the photocatalytic performance resulting from the cycloalkyl functionalization of UiO-66-NH2 make it a promising approach to designing novel photocatalysts for solar abatement of emerging contaminants. © 2023 The Author(s)This research was funded by the Spanish State Research Agency (PID2019-106186RB-I00/AEI/10.13039/501100011033 and PID2019-105479RB-I00 MCIN/AEI/10.13039/501100011033). Rafael R. Solís thanks the Spanish Ministry of Science, Innovation, and Universities for his postdoctoral contract (Juan de la Cierva Formación, Ref. FJC2018-035513-I). The authors also thank the support provided by the external services of the Autonomous University of Madrid (SIdI) and the University of Extremadura (SAIUEx). Funding for open access charge: Universidad de Granada/CBUA.Appendix A. Supplementary dataPeer reviewedElsevier BVConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202420242023info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/350822https://www.scopus.com/inward/record.uri?eid=2-s2.0-85148359975&doi=10.1016%2fj.cej.2023.141889&partnerID=40&md5=ae54058255619c3999c3d6a6ce99e9d1reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)InglésChemical Engineering Journalhttps://doi.org/10.1016/j.cej.2023.141889Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3508222026-05-22T06:33:51Z
dc.title.none.fl_str_mv Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophen
title Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophen
spellingShingle Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophen
Gómez-Avilés, A.
Acetaminophen
Linker functionalization
Photocatalysis
UiO-66-NH2
Water treatment
Dimers
Energy gap
Cyclohexyl rings
Electron effect
Functionalizations
Photocatalytic performance
Photogenerated charge
Resulting materials
Solar photocatalytic degradation
UiO-66-NH2
title_short Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophen
title_full Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophen
title_fullStr Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophen
title_full_unstemmed Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophen
title_sort Novel isoreticular UiO-66-NH2 frameworks by N-cycloalkyl functionalization of the 2-aminoterephtalate linker with enhanced solar photocatalytic degradation of acetaminophen
dc.creator.none.fl_str_mv Gómez-Avilés, A.
Solís, R.R.
García-Frutos, Eva M.
Bedia, J.
Belver, Carolina
author Gómez-Avilés, A.
author_facet Gómez-Avilés, A.
Solís, R.R.
García-Frutos, Eva M.
Bedia, J.
Belver, Carolina
author_role author
author2 Solís, R.R.
García-Frutos, Eva M.
Bedia, J.
Belver, Carolina
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Acetaminophen
Linker functionalization
Photocatalysis
UiO-66-NH2
Water treatment
Dimers
Energy gap
Cyclohexyl rings
Electron effect
Functionalizations
Photocatalytic performance
Photogenerated charge
Resulting materials
Solar photocatalytic degradation
UiO-66-NH2
topic Acetaminophen
Linker functionalization
Photocatalysis
UiO-66-NH2
Water treatment
Dimers
Energy gap
Cyclohexyl rings
Electron effect
Functionalizations
Photocatalytic performance
Photogenerated charge
Resulting materials
Solar photocatalytic degradation
UiO-66-NH2
description This work reports for the first time the functionalization of the 2-aminoterephtalate linker of UiO-66-NH2 with cyclopentyl or cyclohexyl rings. The resulting materials displayed reduced bandgaps with enhanced separation of the photogenerated charges due to the inductive electron effect of the cycloalkyl substituent. These functionalized materials displayed higher photocatalytic performance towards the solar abatement of acetaminophen than UiO-66-NH2. The photocatalytic activation mechanism was proposed based on the band alignment and scavenger tests, suggesting the major contribution of holes and superoxide radicals. In particular, UiO-66-NH-C5 exhibited high stability under reaction with low activity loss after reusing. The acetaminophen degradation pathway was also studied indicating that the ACE molecules were coupled to dimers and trimers that were further oxidized. The small bandgap, the band structure, and the photocatalytic performance resulting from the cycloalkyl functionalization of UiO-66-NH2 make it a promising approach to designing novel photocatalysts for solar abatement of emerging contaminants. © 2023 The Author(s)
publishDate 2023
dc.date.none.fl_str_mv 2023
2024
2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/350822
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85148359975&doi=10.1016%2fj.cej.2023.141889&partnerID=40&md5=ae54058255619c3999c3d6a6ce99e9d1
url http://hdl.handle.net/10261/350822
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85148359975&doi=10.1016%2fj.cej.2023.141889&partnerID=40&md5=ae54058255619c3999c3d6a6ce99e9d1
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Chemical Engineering Journal
https://doi.org/10.1016/j.cej.2023.141889
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Elsevier BV
publisher.none.fl_str_mv Elsevier BV
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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