Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic Frameworks

The presence of hexavalent chromium water pollution is a growing global concern. Among the currently applied technologies to remove CrVI, its adsorption and photocatalytic reduction to CrIII less mobile and toxic forms are the most appealing because of their simplicity, reusability, and low energy c...

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Autores: González Saiz, Paula, Valverde de Mingo, Ainara, González Navarrete, Bárbara, Rosales, Maibelin, Quintero, Yurieth Marcela, Fidalgo Marijuán, Arkaitz, Orive, Joseba, Reizabal López-Para, Ander, Larrea, Edurne S., Arriortua Marcaida, María Isabel, Lanceros Méndez, Senentxu, García, Andreina, Fernández de Luis, Roberto
Tipo de documento: artigo
Data de publicação:2021
País:España
Recursos:Universidad del País Vasco
Repositório:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/49854
Acesso em linha:http://hdl.handle.net/10810/49854
Access Level:Acceso aberto
Palavra-chave:metal–organic frameworks
photocatalysis
chromium
photoreduction
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spelling Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic FrameworksGonzález Saiz, PaulaValverde de Mingo, AinaraGonzález Navarrete, BárbaraRosales, MaibelinQuintero, Yurieth MarcelaFidalgo Marijuán, ArkaitzOrive, JosebaReizabal López-Para, AnderLarrea, Edurne S.Arriortua Marcaida, María IsabelLanceros Méndez, SenentxuGarcía, AndreinaFernández de Luis, Robertometal–organic frameworksphotocatalysischromiumphotoreductionThe presence of hexavalent chromium water pollution is a growing global concern. Among the currently applied technologies to remove CrVI, its adsorption and photocatalytic reduction to CrIII less mobile and toxic forms are the most appealing because of their simplicity, reusability, and low energy consumption. However, little attention has been paid to bifunctional catalysts, that is, materials that can reduce CrVI to CrIII and retain both hexavalent and trivalent chromium species at the same time. In this work, the dual CrVI adsorption–reduction capacity of two iconic photoactive water-stable zirconium and titanium-based metal–organic frameworks (MOFs) has been investigated: UiO-66-NH2 and MIL-125. The bifunctionality of photoactive MOFs depends on different parameters, such as the particle size in MIL-125 or organic linker functionalization/defective positions in UiO-66 type sorbents. For instance, the presence of organic linker defects in UiO-66 has shown to be detrimental for the chromium photoreduction but beneficial for the retention of the CrIII phototransformed species. Both compounds are able to retain from 90 to 98% of the initial chromium present at acidic solutions as well as immobilize the reduced CrIII species, demonstrating the suitability of the materials for CrVI environmental remediation. In addition, it has been demonstrated that adsorption can be carried out also in a continuous flux mode through a diluted photoactive MOF/sand chromatographic column. The obtained results open the perspective to assess the bifunctional sorption and photoreduction ability of a plethora of MOF materials that have been applied for chromium capture and photoreduction purposes. In parallel, this work opens the perspective to develop specific chemical encoding strategies within MOFs to transfer this bifunctionality to other related water remediation applications.The authors thank the financial support from the Spanish Ministry of Economy and Competitiveness (MINECO) through projects MAT2016-76739-R (AEI/FEDER, EU) and MAT2016-76039-C4-3-R (AEI/FEDER, UE) (including FEDER financial support) and from the Basque Government Industry and Education Departments under the ELKARTEK (LION, ACTIMAT), HAZITEK (SIMAN) and PIBA (PIBA-2018-06) programs, respectively. The European Commission Research & Innovation H2020-MSCA-RISE-2017 (Ref.: 778412) INDESMOF project.MDPIEuropean Commission2021202120212021info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10810/49854reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoInglésinfo:eu-repo/grantAgreement/MINECO/MAT2016-76739-R/info:eu-repo/grantAgreement/MINECO/MAT2016-76039-C4-3-R/info:eu-repo/grantAgreement/EC/H2020/778412https://www.mdpi.com/2073-4344/11/1/51/htminfo:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by/3.0/es/2021 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).oai:addi.ehu.eus:10810/498542026-06-18T09:23:17Z
dc.title.none.fl_str_mv Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic Frameworks
title Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic Frameworks
spellingShingle Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic Frameworks
González Saiz, Paula
metal–organic frameworks
photocatalysis
chromium
photoreduction
title_short Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic Frameworks
title_full Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic Frameworks
title_fullStr Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic Frameworks
title_full_unstemmed Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic Frameworks
title_sort Modulation of the Bifunctional CrVI to CrIII Photoreduction and Adsorption Capacity in ZrIV and TiIV Benchmark Metal-Organic Frameworks
dc.creator.none.fl_str_mv González Saiz, Paula
Valverde de Mingo, Ainara
González Navarrete, Bárbara
Rosales, Maibelin
Quintero, Yurieth Marcela
Fidalgo Marijuán, Arkaitz
Orive, Joseba
Reizabal López-Para, Ander
Larrea, Edurne S.
Arriortua Marcaida, María Isabel
Lanceros Méndez, Senentxu
García, Andreina
Fernández de Luis, Roberto
author González Saiz, Paula
author_facet González Saiz, Paula
Valverde de Mingo, Ainara
González Navarrete, Bárbara
Rosales, Maibelin
Quintero, Yurieth Marcela
Fidalgo Marijuán, Arkaitz
Orive, Joseba
Reizabal López-Para, Ander
Larrea, Edurne S.
Arriortua Marcaida, María Isabel
Lanceros Méndez, Senentxu
García, Andreina
Fernández de Luis, Roberto
author_role author
author2 Valverde de Mingo, Ainara
González Navarrete, Bárbara
Rosales, Maibelin
Quintero, Yurieth Marcela
Fidalgo Marijuán, Arkaitz
Orive, Joseba
Reizabal López-Para, Ander
Larrea, Edurne S.
Arriortua Marcaida, María Isabel
Lanceros Méndez, Senentxu
García, Andreina
Fernández de Luis, Roberto
author2_role author
author
author
author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv European Commission
dc.subject.none.fl_str_mv metal–organic frameworks
photocatalysis
chromium
photoreduction
topic metal–organic frameworks
photocatalysis
chromium
photoreduction
description The presence of hexavalent chromium water pollution is a growing global concern. Among the currently applied technologies to remove CrVI, its adsorption and photocatalytic reduction to CrIII less mobile and toxic forms are the most appealing because of their simplicity, reusability, and low energy consumption. However, little attention has been paid to bifunctional catalysts, that is, materials that can reduce CrVI to CrIII and retain both hexavalent and trivalent chromium species at the same time. In this work, the dual CrVI adsorption–reduction capacity of two iconic photoactive water-stable zirconium and titanium-based metal–organic frameworks (MOFs) has been investigated: UiO-66-NH2 and MIL-125. The bifunctionality of photoactive MOFs depends on different parameters, such as the particle size in MIL-125 or organic linker functionalization/defective positions in UiO-66 type sorbents. For instance, the presence of organic linker defects in UiO-66 has shown to be detrimental for the chromium photoreduction but beneficial for the retention of the CrIII phototransformed species. Both compounds are able to retain from 90 to 98% of the initial chromium present at acidic solutions as well as immobilize the reduced CrIII species, demonstrating the suitability of the materials for CrVI environmental remediation. In addition, it has been demonstrated that adsorption can be carried out also in a continuous flux mode through a diluted photoactive MOF/sand chromatographic column. The obtained results open the perspective to assess the bifunctional sorption and photoreduction ability of a plethora of MOF materials that have been applied for chromium capture and photoreduction purposes. In parallel, this work opens the perspective to develop specific chemical encoding strategies within MOFs to transfer this bifunctionality to other related water remediation applications.
publishDate 2021
dc.date.none.fl_str_mv 2021
2021
2021
2021
dc.type.none.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10810/49854
url http://hdl.handle.net/10810/49854
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/MINECO/MAT2016-76739-R/
info:eu-repo/grantAgreement/MINECO/MAT2016-76039-C4-3-R/
info:eu-repo/grantAgreement/EC/H2020/778412
https://www.mdpi.com/2073-4344/11/1/51/htm
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
http://creativecommons.org/licenses/by/3.0/es/
eu_rights_str_mv openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by/3.0/es/
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv MDPI
publisher.none.fl_str_mv MDPI
dc.source.none.fl_str_mv reponame:Addi. Archivo Digital para la Docencia y la Investigación
instname:Universidad del País Vasco
instname_str Universidad del País Vasco
reponame_str Addi. Archivo Digital para la Docencia y la Investigación
collection Addi. Archivo Digital para la Docencia y la Investigación
repository.name.fl_str_mv
repository.mail.fl_str_mv
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