Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinopril

A bimetallic FeCu/NC core-shell catalyst, consisting in nanoparticles where zero-valent Fe and Cu atoms, slightly oxidized on their surface, are encapsulated by carbon has been successfully prepared by modifying the synthesis route of MIL(Fe)-88B. FeCu/NC possessed well-balanced textural and electro...

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Autores: Zhao, Lele, Murrieta, María F., Padilla, José A., Lanzalaco, Sonia, Cabot Julià, Pere-Lluís, Sirés Sadornil, Ignacio
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2024
País:España
Institución:Universidad de Barcelona
Repositorio:Dipòsit Digital de la UB
OAI Identifier:oai:diposit.ub.edu:2445/215994
Acceso en línea:https://hdl.handle.net/2445/215994
Access Level:acceso embargado
Palabra clave:Electroquímica
Contaminació de l'aigua
Electrochemistry
Water pollution
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spelling Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinoprilZhao, LeleMurrieta, María F.Padilla, José A.Lanzalaco, SoniaCabot Julià, Pere-LluísSirés Sadornil, IgnacioElectroquímicaContaminació de l'aiguaElectrochemistryWater pollutionA bimetallic FeCu/NC core-shell catalyst, consisting in nanoparticles where zero-valent Fe and Cu atoms, slightly oxidized on their surface, are encapsulated by carbon has been successfully prepared by modifying the synthesis route of MIL(Fe)-88B. FeCu/NC possessed well-balanced textural and electrochemical properties. According to voltammetric responses, in-situ Fe(III) reduction to Fe(II) by low-valent Cu was feasible, whereas the high double-layer capacitance confirmed the presence of a great number of electroactive sites that was essential for continuous H2O2 activation to •OH via Fenton's reaction. Electrochemical impedance and distribution of relaxation times (DRT) analysis informed about the strong leaching resistance of FeCu/NC. To validate the promising features of this catalyst, the advanced oxidation of the antihypertensive lisinopril (LSN) was investigated for the first time. The heterogeneous electro-Fenton (HEF) treatment of 16.1 mg L−1 LSN solutions was carried out in a DSA/air-diffusion cell. At pH 3, complete degradation was achieved within 6 min using only 0.05 g L−1 FeCu/NC; at near-neutral pH, 100 % removal was also feasible even in actual urban wastewater, requiring 60–75 min. The FeCu/NC catalyst demonstrated high stability, still maintaining 86.5 % of degradation efficiency after 5 cycles and undergoing low iron leaching. It outperformed the monometallic (Fe/NC and Cu/NC) catalysts, which is explained by the Cu(0)/Cu(I)-catalyzed Fe(II) regeneration mechanism that maintains the Fenton's cycle. LC-MS/MS analysis allowed the identification of two main primary LSN by-products. It can then be concluded that the FeCu/NC-based HEF process merits to be further scaled up for wastewater treatment.Elsevier B.V.2024info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionapplication/pdfhttps://hdl.handle.net/2445/215994Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaInglésVersió postprint del document publicat a: https://doi.org/10.1016/j.scitotenv.2024.176110Science of the Total Environment, 2024, vol. 953, p. 1-12https://doi.org/10.1016/j.scitotenv.2024.176110cc-by-nc-nd (c) Elsevier B.V., 2024http://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/embargoedAccessoai:diposit.ub.edu:2445/2159942026-05-27T06:46:51Z
dc.title.none.fl_str_mv Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinopril
title Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinopril
spellingShingle Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinopril
Zhao, Lele
Electroquímica
Contaminació de l'aigua
Electrochemistry
Water pollution
title_short Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinopril
title_full Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinopril
title_fullStr Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinopril
title_full_unstemmed Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinopril
title_sort Bimetallic FeCu-MOF derivatives as heterogeneous catalysts with enhanced stability for electro-Fenton degradation of lisinopril
dc.creator.none.fl_str_mv Zhao, Lele
Murrieta, María F.
Padilla, José A.
Lanzalaco, Sonia
Cabot Julià, Pere-Lluís
Sirés Sadornil, Ignacio
author Zhao, Lele
author_facet Zhao, Lele
Murrieta, María F.
Padilla, José A.
Lanzalaco, Sonia
Cabot Julià, Pere-Lluís
Sirés Sadornil, Ignacio
author_role author
author2 Murrieta, María F.
Padilla, José A.
Lanzalaco, Sonia
Cabot Julià, Pere-Lluís
Sirés Sadornil, Ignacio
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Electroquímica
Contaminació de l'aigua
Electrochemistry
Water pollution
topic Electroquímica
Contaminació de l'aigua
Electrochemistry
Water pollution
description A bimetallic FeCu/NC core-shell catalyst, consisting in nanoparticles where zero-valent Fe and Cu atoms, slightly oxidized on their surface, are encapsulated by carbon has been successfully prepared by modifying the synthesis route of MIL(Fe)-88B. FeCu/NC possessed well-balanced textural and electrochemical properties. According to voltammetric responses, in-situ Fe(III) reduction to Fe(II) by low-valent Cu was feasible, whereas the high double-layer capacitance confirmed the presence of a great number of electroactive sites that was essential for continuous H2O2 activation to •OH via Fenton's reaction. Electrochemical impedance and distribution of relaxation times (DRT) analysis informed about the strong leaching resistance of FeCu/NC. To validate the promising features of this catalyst, the advanced oxidation of the antihypertensive lisinopril (LSN) was investigated for the first time. The heterogeneous electro-Fenton (HEF) treatment of 16.1 mg L−1 LSN solutions was carried out in a DSA/air-diffusion cell. At pH 3, complete degradation was achieved within 6 min using only 0.05 g L−1 FeCu/NC; at near-neutral pH, 100 % removal was also feasible even in actual urban wastewater, requiring 60–75 min. The FeCu/NC catalyst demonstrated high stability, still maintaining 86.5 % of degradation efficiency after 5 cycles and undergoing low iron leaching. It outperformed the monometallic (Fe/NC and Cu/NC) catalysts, which is explained by the Cu(0)/Cu(I)-catalyzed Fe(II) regeneration mechanism that maintains the Fenton's cycle. LC-MS/MS analysis allowed the identification of two main primary LSN by-products. It can then be concluded that the FeCu/NC-based HEF process merits to be further scaled up for wastewater treatment.
publishDate 2024
dc.date.none.fl_str_mv 2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/215994
url https://hdl.handle.net/2445/215994
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Versió postprint del document publicat a: https://doi.org/10.1016/j.scitotenv.2024.176110
Science of the Total Environment, 2024, vol. 953, p. 1-12
https://doi.org/10.1016/j.scitotenv.2024.176110
dc.rights.none.fl_str_mv cc-by-nc-nd (c) Elsevier B.V., 2024
http://creativecommons.org/licenses/by-nc-nd/4.0/
info:eu-repo/semantics/embargoedAccess
rights_invalid_str_mv cc-by-nc-nd (c) Elsevier B.V., 2024
http://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv embargoedAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Elsevier B.V.
publisher.none.fl_str_mv Elsevier B.V.
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Dipòsit Digital de la UB
instname:Universidad de Barcelona
instname_str Universidad de Barcelona
reponame_str Dipòsit Digital de la UB
collection Dipòsit Digital de la UB
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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