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Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions

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Resumo:Literature describes a kinetic degradation profile for sulfamethoxazole (SMX) and trimethoprim (TMP) antibiotics in aqueous solutions using a photo-Fenton reaction characterized by a very fast initial reaction rate followed by a slow degradation process. This work tries to elucidate that the slow decay on SMX and TMP concentration observed in the second part of the photo-Fenton kinetic degradation profile is not only entirely attributed to the competition of hydroxyl radicals between the initial intermediates generated and the antibiotic molecules, but also associated to the formation of strong and stable Fe(III)-antibiotic complexes, which limits the photoreduction of Fe3+, decreasing the decomposition of H2O2 in the Fenton reaction and the overall efficiency of the photo-Fenton process. Ferric speciation diagrams, including the ferric hydroxide complexes, antibiotic species and their interaction with ferric ions, showed the formation of those strong Fe(III)-antibiotic complexes. Process intensification of the photo-Fenton reaction with ferrioxalate complexes was able to reduce the formation of those Fe(III)-antibiotic complexes, enhancing the reaction efficiency at near neutral pH values (5.0) and using low iron concentration (5.0 mg/L). Ferrioxalate complexes are stronger than Fe(III)-antibiotic complexes, improving the quantum yield for ferrous ions production. The efficiency of the photo-Fenton reaction was also compared with the heterogeneous photocatalysis (TiO2/UV and TiO2/H2O2/UV), driven by natural solar radiation using photoreactors with compound parabolic collectors (CPCs) at pilot scale. The speciation of antibiotics molecules in solution as a function of pH plays also an important role in the reactivity of ROS.
Autores principais:Isabelli N. Dias
Outros Autores:João H. O. S. Pereira; Francisca C. Moreira; Márcia Dezotti; Rui A. R. Boaventura; Vítor J. P. Vilar; Bruno S. Souza
Assunto:Tecnologia ambiental, Engenharia do ambiente Environmental technology, Environmental engineering
Ano:2014
País:Portugal
Tipo de documento:artigo
Tipo de acesso:acesso restrito
Instituição associada:Universidade do Porto
Idioma:inglês
Origem:Repositório Aberto da Universidade do Porto
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author Isabelli N. Dias
author2 João H. O. S. Pereira
Francisca C. Moreira
Márcia Dezotti
Rui A. R. Boaventura
Vítor J. P. Vilar
Bruno S. Souza
author2_role author
author
author
author
author
author
author_facet Isabelli N. Dias
João H. O. S. Pereira
Francisca C. Moreira
Márcia Dezotti
Rui A. R. Boaventura
Vítor J. P. Vilar
Bruno S. Souza
author_role author
country_str PT
creators_json_txt [{\"Person.name\":\"Isabelli N. Dias\"},{\"Person.name\":\"João H. O. S. Pereira\"},{\"Person.name\":\"Francisca C. Moreira\"},{\"Person.name\":\"Márcia Dezotti\"},{\"Person.name\":\"Rui A. R. Boaventura\"},{\"Person.name\":\"Vítor J. P. Vilar\"},{\"Person.name\":\"Bruno S. Souza\"}]
datacite.creators.creator.creatorName.fl_str_mv Isabelli N. Dias
João H. O. S. Pereira
Francisca C. Moreira
Márcia Dezotti
Rui A. R. Boaventura
Vítor J. P. Vilar
Bruno S. Souza
datacite.date.Accepted.fl_str_mv 2014-01-01T00:00:00Z
datacite.rights.fl_str_mv http://purl.org/coar/access_right/c_16ec
datacite.subjects.subject.fl_str_mv Tecnologia ambiental, Engenharia do ambiente
Environmental technology, Environmental engineering
datacite.titles.title.fl_str_mv Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions
dc.creator.none.fl_str_mv Isabelli N. Dias
João H. O. S. Pereira
Francisca C. Moreira
Márcia Dezotti
Rui A. R. Boaventura
Vítor J. P. Vilar
Bruno S. Souza
dc.date.Accepted.fl_str_mv 2014-01-01T00:00:00Z
dc.format.none.fl_str_mv application/pdf
dc.identifier.none.fl_str_mv https://hdl.handle.net/10216/105768
dc.language.none.fl_str_mv eng
dc.rights.none.fl_str_mv http://purl.org/coar/access_right/c_16ec
dc.subject.none.fl_str_mv Tecnologia ambiental, Engenharia do ambiente
Environmental technology, Environmental engineering
dc.title.fl_str_mv Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions
dc.type.none.fl_str_mv http://purl.org/coar/resource_type/c_6501
description Literature describes a kinetic degradation profile for sulfamethoxazole (SMX) and trimethoprim (TMP) antibiotics in aqueous solutions using a photo-Fenton reaction characterized by a very fast initial reaction rate followed by a slow degradation process. This work tries to elucidate that the slow decay on SMX and TMP concentration observed in the second part of the photo-Fenton kinetic degradation profile is not only entirely attributed to the competition of hydroxyl radicals between the initial intermediates generated and the antibiotic molecules, but also associated to the formation of strong and stable Fe(III)-antibiotic complexes, which limits the photoreduction of Fe3+, decreasing the decomposition of H2O2 in the Fenton reaction and the overall efficiency of the photo-Fenton process. Ferric speciation diagrams, including the ferric hydroxide complexes, antibiotic species and their interaction with ferric ions, showed the formation of those strong Fe(III)-antibiotic complexes. Process intensification of the photo-Fenton reaction with ferrioxalate complexes was able to reduce the formation of those Fe(III)-antibiotic complexes, enhancing the reaction efficiency at near neutral pH values (5.0) and using low iron concentration (5.0 mg/L). Ferrioxalate complexes are stronger than Fe(III)-antibiotic complexes, improving the quantum yield for ferrous ions production. The efficiency of the photo-Fenton reaction was also compared with the heterogeneous photocatalysis (TiO2/UV and TiO2/H2O2/UV), driven by natural solar radiation using photoreactors with compound parabolic collectors (CPCs) at pilot scale. The speciation of antibiotics molecules in solution as a function of pH plays also an important role in the reactivity of ROS.
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organization_str_mv urn:organizationAcronym:up
person_str_mv Isabelli N. Dias
João H. O. S. Pereira
Francisca C. Moreira
Márcia Dezotti
Rui A. R. Boaventura
Vítor J. P. Vilar
Bruno S. Souza
publishDate 2014
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spelling Literature describes a kinetic degradation profile for sulfamethoxazole (SMX) and trimethoprim (TMP) antibiotics in aqueous solutions using a photo-Fenton reaction characterized by a very fast initial reaction rate followed by a slow degradation process. This work tries to elucidate that the slow decay on SMX and TMP concentration observed in the second part of the photo-Fenton kinetic degradation profile is not only entirely attributed to the competition of hydroxyl radicals between the initial intermediates generated and the antibiotic molecules, but also associated to the formation of strong and stable Fe(III)-antibiotic complexes, which limits the photoreduction of Fe3+, decreasing the decomposition of H2O2 in the Fenton reaction and the overall efficiency of the photo-Fenton process. Ferric speciation diagrams, including the ferric hydroxide complexes, antibiotic species and their interaction with ferric ions, showed the formation of those strong Fe(III)-antibiotic complexes. Process intensification of the photo-Fenton reaction with ferrioxalate complexes was able to reduce the formation of those Fe(III)-antibiotic complexes, enhancing the reaction efficiency at near neutral pH values (5.0) and using low iron concentration (5.0 mg/L). Ferrioxalate complexes are stronger than Fe(III)-antibiotic complexes, improving the quantum yield for ferrous ions production. The efficiency of the photo-Fenton reaction was also compared with the heterogeneous photocatalysis (TiO2/UV and TiO2/H2O2/UV), driven by natural solar radiation using photoreactors with compound parabolic collectors (CPCs) at pilot scale. The speciation of antibiotics molecules in solution as a function of pH plays also an important role in the reactivity of ROS.application/pdfengEnhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutionsIsabelli N. DiasJoão H. O. S. PereiraFrancisca C. MoreiraMárcia DezottiRui A. R. BoaventuraVítor J. P. VilarBruno S. SouzaHandlehttps://hdl.handle.net/10216/105768ISSNIsPartOf1385-8947DOIIsPartOf10.1016/j.cej.2014.03.02020142014-01-01T00:00:00Zhttp://purl.org/coar/access_right/c_16ecrestricted accessTecnologia ambiental, Engenharia do ambienteEnvironmental technology, Environmental engineering3370839 byteshttp://purl.org/coar/access_right/c_16ecapplication/pdffulltexthttps://repositorio-aberto.up.pt/bitstream/10216/105768/2/93950.pdfliteraturehttp://purl.org/coar/resource_type/c_6501journal article
spellingShingle Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions
Isabelli N. Dias
Tecnologia ambiental, Engenharia do ambiente
Environmental technology, Environmental engineering
status SINGLETON
subject.fl_str_mv Tecnologia ambiental, Engenharia do ambiente
Environmental technology, Environmental engineering
title Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions
title_full Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions
title_fullStr Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions
title_full_unstemmed Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions
title_short Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions
title_sort Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: A case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions
topic Tecnologia ambiental, Engenharia do ambiente
Environmental technology, Environmental engineering
topic_facet Tecnologia ambiental, Engenharia do ambiente
Environmental technology, Environmental engineering
url https://hdl.handle.net/10216/105768
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