Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalyst

Conventional electro-Fenton (EF) process at acidic pH ∼3 is recognized as a highly effective strategy to degrade organic pollutants; however, homogeneous metal catalysts cannot be employed in more alkaline media. To overcome this limitation, pyrolytic derivatives from metal-organic frameworks (MOFs)...

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Autores: Zhao, Lele, Padilla, José A., Xuriguera Martín, María Elena, Cabot Julià, Pere-Lluís, Brillas, Enric, Sirés Sadornil, Ignacio
Formato: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2024
País:España
Recursos:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2445/215974
Acesso em linha:https://hdl.handle.net/2445/215974
Access Level:acceso embargado
Palavra-chave:Depuració de l'aigua
Electroquímica
Oxidació
Water purification
Electrochemistry
Oxidation
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spelling Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalystZhao, LelePadilla, José A.Xuriguera Martín, María ElenaCabot Julià, Pere-LluísBrillas, EnricSirés Sadornil, IgnacioDepuració de l'aiguaElectroquímicaOxidacióWater purificationElectrochemistryOxidationConventional electro-Fenton (EF) process at acidic pH ∼3 is recognized as a highly effective strategy to degrade organic pollutants; however, homogeneous metal catalysts cannot be employed in more alkaline media. To overcome this limitation, pyrolytic derivatives from metal-organic frameworks (MOFs) have emerged as promising heterogeneous catalysts. Cu-based MOFs were prepared using trimesic acid as the organic ligand and different pyrolysis conditions, yielding a set of nano-Cu/C catalysts that were analyzed by conventional methods. Among them, XPS revealed the surface of the Cu/C-A2-Ar/H2 catalyst was slightly oxidized to Cu(I) and, combined with XRD and HRTEM data, it can be concluded that the catalyst presents a core-shell structure where metallic copper is embedded in a carbon layer. The antihistamine diphenhydramine (DPH), spiked into either synthetic Na2SO4 solutions or actual urban wastewater, was treated in an undivided electrolytic cell equipped with a DSA-Cl2 anode and a commercial air-diffusion cathode able to electrogenerate H2O2. Using Cu/C as suspended catalyst, DPH was completely degraded in both media at pH 6–8, outperforming the EF process with Fe2+ catalyst at pH 3 in terms of degradation rate and mineralization degree thanks to the absence of refractory Fe(III)-carboxylate complexes that typically decelerate the TOC abatement. From the by-products detected by GC/MS, a reaction sequence for DPH mineralization is proposed.Elsevier Ltd202420242024infoinfo:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersion11 p.application/pdfhttps://hdl.handle.net/2445/215974Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésVersió postprint del document publicat a: https://doi.org/10.1016/j.chemosphere.2024.143249Chemosphere, 2024, vol. 364, p. 1-11https://doi.org/10.1016/j.chemosphere.2024.143249cc-by-nc-nd (c) Elsevier Ltd, 2024http://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/embargoedAccessoai:recercat.cat:2445/2159742026-05-29T05:05:01Z
dc.title.none.fl_str_mv Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalyst
title Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalyst
spellingShingle Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalyst
Zhao, Lele
Depuració de l'aigua
Electroquímica
Oxidació
Water purification
Electrochemistry
Oxidation
title_short Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalyst
title_full Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalyst
title_fullStr Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalyst
title_full_unstemmed Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalyst
title_sort Enhanced mineralization of pharmaceutical residues at circumneutral pH by heterogeneous electro-Fenton-like process with Cu/C catalyst
dc.creator.none.fl_str_mv Zhao, Lele
Padilla, José A.
Xuriguera Martín, María Elena
Cabot Julià, Pere-Lluís
Brillas, Enric
Sirés Sadornil, Ignacio
author Zhao, Lele
author_facet Zhao, Lele
Padilla, José A.
Xuriguera Martín, María Elena
Cabot Julià, Pere-Lluís
Brillas, Enric
Sirés Sadornil, Ignacio
author_role author
author2 Padilla, José A.
Xuriguera Martín, María Elena
Cabot Julià, Pere-Lluís
Brillas, Enric
Sirés Sadornil, Ignacio
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Depuració de l'aigua
Electroquímica
Oxidació
Water purification
Electrochemistry
Oxidation
topic Depuració de l'aigua
Electroquímica
Oxidació
Water purification
Electrochemistry
Oxidation
description Conventional electro-Fenton (EF) process at acidic pH ∼3 is recognized as a highly effective strategy to degrade organic pollutants; however, homogeneous metal catalysts cannot be employed in more alkaline media. To overcome this limitation, pyrolytic derivatives from metal-organic frameworks (MOFs) have emerged as promising heterogeneous catalysts. Cu-based MOFs were prepared using trimesic acid as the organic ligand and different pyrolysis conditions, yielding a set of nano-Cu/C catalysts that were analyzed by conventional methods. Among them, XPS revealed the surface of the Cu/C-A2-Ar/H2 catalyst was slightly oxidized to Cu(I) and, combined with XRD and HRTEM data, it can be concluded that the catalyst presents a core-shell structure where metallic copper is embedded in a carbon layer. The antihistamine diphenhydramine (DPH), spiked into either synthetic Na2SO4 solutions or actual urban wastewater, was treated in an undivided electrolytic cell equipped with a DSA-Cl2 anode and a commercial air-diffusion cathode able to electrogenerate H2O2. Using Cu/C as suspended catalyst, DPH was completely degraded in both media at pH 6–8, outperforming the EF process with Fe2+ catalyst at pH 3 in terms of degradation rate and mineralization degree thanks to the absence of refractory Fe(III)-carboxylate complexes that typically decelerate the TOC abatement. From the by-products detected by GC/MS, a reaction sequence for DPH mineralization is proposed.
publishDate 2024
dc.date.none.fl_str_mv 2024
2024
2024
info
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/2445/215974
url https://hdl.handle.net/2445/215974
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.chemosphere.2024.143249
Chemosphere, 2024, vol. 364, p. 1-11
https://doi.org/10.1016/j.chemosphere.2024.143249
dc.rights.none.fl_str_mv cc-by-nc-nd (c) Elsevier Ltd, 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 Ltd, 2024
http://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv embargoedAccess
dc.format.none.fl_str_mv 11 p.
application/pdf
dc.publisher.none.fl_str_mv Elsevier Ltd
publisher.none.fl_str_mv Elsevier Ltd
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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