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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Authors: Gómez Avilés, Almudena, Solís, Rafael R., García-Frutos, Eva M., Bedia García-Matamoros, Jorge, Belver Coldeira, Carolina
Format: article
Publication Date:2023
Country:España
Institution:Universidad Autónoma de Madrid
Repository:Biblos-e Archivo. Repositorio Institucional de la UAM
Language:English
OAI Identifier:oai:repositorio.uam.es:10486/708316
Online Access:http://hdl.handle.net/10486/708316
https://dx.doi.org/10.1016/j.cej.2023.141889
Access Level:Open access
Keyword:Acetaminophen
Photocatalysis
UiO-66-NH 2
Linker Functionalization
Water Treatment
Química
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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, AlmudenaSolís, Rafael R.García-Frutos, Eva M.Bedia García-Matamoros, JorgeBelver Coldeira, CarolinaAcetaminophenPhotocatalysisUiO-66-NH 2Linker FunctionalizationWater TreatmentQuímicaThis 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 contaminantsThis 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 Formaci´ on, 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/CBUAElsevierDepartamento de Ingeniería QuímicaFacultad de CienciasUAM. Departamento de Ingeniería Química20232023-02-14research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/708316https://dx.doi.org/10.1016/j.cej.2023.141889reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengopen accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7083162026-06-23T12:46:27Z
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, Almudena
Acetaminophen
Photocatalysis
UiO-66-NH 2
Linker Functionalization
Water Treatment
Química
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, Almudena
Solís, Rafael R.
García-Frutos, Eva M.
Bedia García-Matamoros, Jorge
Belver Coldeira, Carolina
author Gómez Avilés, Almudena
author_facet Gómez Avilés, Almudena
Solís, Rafael R.
García-Frutos, Eva M.
Bedia García-Matamoros, Jorge
Belver Coldeira, Carolina
author_role author
author2 Solís, Rafael R.
García-Frutos, Eva M.
Bedia García-Matamoros, Jorge
Belver Coldeira, Carolina
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Departamento de Ingeniería Química
Facultad de Ciencias
UAM. Departamento de Ingeniería Química
dc.subject.none.fl_str_mv Acetaminophen
Photocatalysis
UiO-66-NH 2
Linker Functionalization
Water Treatment
Química
topic Acetaminophen
Photocatalysis
UiO-66-NH 2
Linker Functionalization
Water Treatment
Química
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
publishDate 2023
dc.date.none.fl_str_mv 2023
2023-02-14
dc.type.none.fl_str_mv research article
http://purl.org/coar/resource_type/c_2df8fbb1
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 http://hdl.handle.net/10486/708316
https://dx.doi.org/10.1016/j.cej.2023.141889
url http://hdl.handle.net/10486/708316
https://dx.doi.org/10.1016/j.cej.2023.141889
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
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
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
dc.source.none.fl_str_mv reponame:Biblos-e Archivo. Repositorio Institucional de la UAM
instname:Universidad Autónoma de Madrid
instname_str Universidad Autónoma de Madrid
reponame_str Biblos-e Archivo. Repositorio Institucional de la UAM
collection Biblos-e Archivo. Repositorio Institucional de la UAM
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.300724

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