Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicity

Electro-oxidation with electrogenerated H2O2 (EO-H2O2) was applied to treat acidic aqueous solutions of 4-aminoantipyrine (4-AA), a persistent drug metabolite of dipyrone, in sulfate medium. Trials were made using a boron-doped diamond anode in the presence of H2O2 electrogenerated on site. A 24 cen...

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Autores: Da Silva, Lucas de Melo, Gozzi, Fábio, Sirés Sadornil, Ignacio, Brillas, Enric, De Oliveira, Silvio César, Machulek Jr., Amílcar
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2018
País:España
Institución:Universidad de Barcelona
Repositorio:Dipòsit Digital de la UB
OAI Identifier:oai:diposit.ub.edu:2445/152815
Acceso en línea:https://hdl.handle.net/2445/152815
Access Level:acceso abierto
Palabra clave:Oxidació electroquímica
Depuració d'aigües residuals
Electrolytic oxidation
Purification of sewage
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spelling Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicityDa Silva, Lucas de MeloGozzi, FábioSirés Sadornil, IgnacioBrillas, EnricDe Oliveira, Silvio CésarMachulek Jr., AmílcarOxidació electroquímicaDepuració d'aigües residualsElectrolytic oxidationPurification of sewageElectro-oxidation with electrogenerated H2O2 (EO-H2O2) was applied to treat acidic aqueous solutions of 4-aminoantipyrine (4-AA), a persistent drug metabolite of dipyrone, in sulfate medium. Trials were made using a boron-doped diamond anode in the presence of H2O2 electrogenerated on site. A 24 central composite design (CCD) was employed to evaluate the effect of four independent variables, namely current density (j), pH, 4-AA concentration and electrolysis time, on the percentages of degradation and mineralization, as well as on mineralization current efficiency (MCE). Predicted responses agreed with observed values, showing linear trendlines with good R2 and R2adj values. The degradation was optimum at j = 77.5 mA cm-2, pH 3.5 and 62.5 mg L-1 4-AA, leading to 63% and 99% removal after 3 and 7 min, respectively. For those solutions, the largest mineralization was found at j = 77.5 mA cm-2, attaining 45% abatement at 175 min. Low MCE values were obtained in all electrolyses. An initial route for 4-AA degradation is proposed based on one dimer and eleven aromatic and aliphatic intermediates detected in the treated solutions at pH 3.5 by LC-MS. The initial 62.5 mg L-1 solution at pH 3.5 presented acute toxicity on Artemia salina larvae, with LC50 = 13.6 mg L-1, being substantially reduced after 3 and 7 min of EO-H2O2 at j = 77.5 mA cm-2 due to the formation of less toxic derivatives.Elsevier B.V.2018info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionapplication/pdfhttps://hdl.handle.net/2445/152815Articles 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.2018.03.092Science of the Total Environment, 2018, vol. 631-632, p. 1079-1088https://doi.org/10.1016/j.scitotenv.2018.03.092cc-by-nc-nd (c) Elsevier B.V., 2018http://creativecommons.org/licenses/by-nc-nd/3.0/esinfo:eu-repo/semantics/openAccessoai:diposit.ub.edu:2445/1528152026-05-27T06:46:51Z
dc.title.none.fl_str_mv Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicity
title Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicity
spellingShingle Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicity
Da Silva, Lucas de Melo
Oxidació electroquímica
Depuració d'aigües residuals
Electrolytic oxidation
Purification of sewage
title_short Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicity
title_full Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicity
title_fullStr Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicity
title_full_unstemmed Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicity
title_sort Degradation of 4-aminoantipyrine by elecro-oxidation with a boron-doped diamond anode: optimization by central composite design, oxidation products and toxicity
dc.creator.none.fl_str_mv Da Silva, Lucas de Melo
Gozzi, Fábio
Sirés Sadornil, Ignacio
Brillas, Enric
De Oliveira, Silvio César
Machulek Jr., Amílcar
author Da Silva, Lucas de Melo
author_facet Da Silva, Lucas de Melo
Gozzi, Fábio
Sirés Sadornil, Ignacio
Brillas, Enric
De Oliveira, Silvio César
Machulek Jr., Amílcar
author_role author
author2 Gozzi, Fábio
Sirés Sadornil, Ignacio
Brillas, Enric
De Oliveira, Silvio César
Machulek Jr., Amílcar
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Oxidació electroquímica
Depuració d'aigües residuals
Electrolytic oxidation
Purification of sewage
topic Oxidació electroquímica
Depuració d'aigües residuals
Electrolytic oxidation
Purification of sewage
description Electro-oxidation with electrogenerated H2O2 (EO-H2O2) was applied to treat acidic aqueous solutions of 4-aminoantipyrine (4-AA), a persistent drug metabolite of dipyrone, in sulfate medium. Trials were made using a boron-doped diamond anode in the presence of H2O2 electrogenerated on site. A 24 central composite design (CCD) was employed to evaluate the effect of four independent variables, namely current density (j), pH, 4-AA concentration and electrolysis time, on the percentages of degradation and mineralization, as well as on mineralization current efficiency (MCE). Predicted responses agreed with observed values, showing linear trendlines with good R2 and R2adj values. The degradation was optimum at j = 77.5 mA cm-2, pH 3.5 and 62.5 mg L-1 4-AA, leading to 63% and 99% removal after 3 and 7 min, respectively. For those solutions, the largest mineralization was found at j = 77.5 mA cm-2, attaining 45% abatement at 175 min. Low MCE values were obtained in all electrolyses. An initial route for 4-AA degradation is proposed based on one dimer and eleven aromatic and aliphatic intermediates detected in the treated solutions at pH 3.5 by LC-MS. The initial 62.5 mg L-1 solution at pH 3.5 presented acute toxicity on Artemia salina larvae, with LC50 = 13.6 mg L-1, being substantially reduced after 3 and 7 min of EO-H2O2 at j = 77.5 mA cm-2 due to the formation of less toxic derivatives.
publishDate 2018
dc.date.none.fl_str_mv 2018
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/2445/152815
url https://hdl.handle.net/2445/152815
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.2018.03.092
Science of the Total Environment, 2018, vol. 631-632, p. 1079-1088
https://doi.org/10.1016/j.scitotenv.2018.03.092
dc.rights.none.fl_str_mv cc-by-nc-nd (c) Elsevier B.V., 2018
http://creativecommons.org/licenses/by-nc-nd/3.0/es
info:eu-repo/semantics/openAccess
rights_invalid_str_mv cc-by-nc-nd (c) Elsevier B.V., 2018
http://creativecommons.org/licenses/by-nc-nd/3.0/es
eu_rights_str_mv openAccess
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 15,300724

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