In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface

Detalhes bibliográficos
Autor(a) principal: Núñez de la Rosa, Yeison Neder
Data de Publicação: 2023
Tipo de documento: Tese
Idioma: eng
Título da fonte: Repositório Institucional da UFSCAR
Texto Completo: https://repositorio.ufscar.br/handle/ufscar/18318
Resumo: Nanometric MnOOH compound was synthesized by a green approach, characterized, and used to remove ciprofloxacin (CIP) antibiotic by in situ chemical oxidation using peroxymonosulfate (PMS). The effects of varying concentrations of MnOOH, PMS and pH, on morphological, structural, chemical, and electrochemical changes were studied during and after the experiments. The CIP molecule was completely oxidized and partially mineralized (~ 60%) after 6 h under acidic conditions. The mechanism of CIP degradation was induced by PMS activated oxidants (HO• and 1O2) and, to a lesser extent, directly on the surface of MnOOH. The latter process was evidenced by transmission electron microscopy showing the formation of an amorphous shell (MnOx) over MnOOH crystallites, as verified using X-ray photoelectron spectroscopy and the subsequent increase of the charge transfer resistance that hindered a further electron transfer to the PMS oxidant. Such behavior is recoverable when using a freshly prepared PMS solution.
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spelling Núñez de la Rosa, Yeison NederAquino, José Mario dehttp://lattes.cnpq.br/8847710280926769http://lattes.cnpq.br/7299008176913606https://orcid.org/0000-0001-9564-8384https://orcid.org/0000-0001-6099-98466b43d67d-c118-4e98-8344-dd48217675572023-07-26T13:32:26Z2023-07-26T13:32:26Z2023-05-24NÚÑEZ DE LA ROSA, Yeison Neder. In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface. 2023. Tese (Doutorado em Química) – Universidade Federal de São Carlos, São Carlos, 2023. Disponível em: https://repositorio.ufscar.br/handle/ufscar/18318.https://repositorio.ufscar.br/handle/ufscar/18318Nanometric MnOOH compound was synthesized by a green approach, characterized, and used to remove ciprofloxacin (CIP) antibiotic by in situ chemical oxidation using peroxymonosulfate (PMS). The effects of varying concentrations of MnOOH, PMS and pH, on morphological, structural, chemical, and electrochemical changes were studied during and after the experiments. The CIP molecule was completely oxidized and partially mineralized (~ 60%) after 6 h under acidic conditions. The mechanism of CIP degradation was induced by PMS activated oxidants (HO• and 1O2) and, to a lesser extent, directly on the surface of MnOOH. The latter process was evidenced by transmission electron microscopy showing the formation of an amorphous shell (MnOx) over MnOOH crystallites, as verified using X-ray photoelectron spectroscopy and the subsequent increase of the charge transfer resistance that hindered a further electron transfer to the PMS oxidant. Such behavior is recoverable when using a freshly prepared PMS solution.O composto nanométrico MnOOH foi sintetizado (por uma abordagem verde), caracterizado e usado para remover o antibiótico Ciprofloxacina (CIP) por oxidação química in situ usando peroximonossulfato (PMS). O efeito de diferentes concentrações de MnOOH, PMS e pH, as mudanças morfológicas, estruturais, químicas e eletroquímicas foram estudados durante e após os experimentos. A molécula CIP foi completamente oxidada e parcialmente mineralizada (~ 60%) após 6 h sob condições ácidas. O mecanismo de degradação do CIP foi conduzido por oxidantes gerados (HO• e 1O2) durante a ativação in situ do PMS e, em menor grau, diretamente na superfície do MnOOH. Este último processo foi confirmado por microscopia eletrônica de transmissão mostrando a formação de uma camada amorfa (MnOx) sobre cristais de MnOOH, também verificado por espectroscopia de fotoelétrons de raios X e o subsequente aumento da resistência à transferência de carga que impediu uma transferência adicional de elétrons para o oxidante PMS. Esse comportamento parece ser recuperável ao ser empregada uma solução PMS recém-preparada.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)engUniversidade Federal de São CarlosCâmpus São CarlosPrograma de Pós-Graduação em Química - PPGQUFSCarAttribution-NonCommercial-NoDerivs 3.0 Brazilhttp://creativecommons.org/licenses/by-nc-nd/3.0/br/info:eu-repo/semantics/openAccessAdvanced oxidation processHeterogeneous catalysisEmerging contaminantsHydroxyl radicalsPMS induced Mn(IV) reductionProcessos oxidativos avançadosCatálise heterogêneaContaminantes emergentesRadical hidroxilaRedução de Mn(IV) induzida por PMSCIENCIAS EXATAS E DA TERRA::QUIMICAIn situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surfaceOxidação química in situ da ciprofloxacina mediada pela ativação de peroximonosulfato usando MnOOH nanométrico: investigação de parâmetros operacionais e mudanças na superfície do catalisadorinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesis600600f136e88e-dfa7-4409-8a6e-063cb254af2ereponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINALTese de doutorado.pdfTese de doutorado.pdfTese de doutoradoapplication/pdf4922310https://repositorio.ufscar.br/bitstream/ufscar/18318/1/Tese%20de%20doutorado.pdfd82386835e23f445f6e6516e8bce9dd3MD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8810https://repositorio.ufscar.br/bitstream/ufscar/18318/2/license_rdff337d95da1fce0a22c77480e5e9a7aecMD52TEXTTese de doutorado.pdf.txtTese de doutorado.pdf.txtExtracted texttext/plain124494https://repositorio.ufscar.br/bitstream/ufscar/18318/3/Tese%20de%20doutorado.pdf.txtb11455f193175519c7f8e7e1a65cf699MD53ufscar/183182024-05-14 18:28:34.008oai:repositorio.ufscar.br:ufscar/18318Repositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestopendoar:43222024-05-14T18:28:34Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false
dc.title.eng.fl_str_mv In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface
dc.title.alternative.por.fl_str_mv Oxidação química in situ da ciprofloxacina mediada pela ativação de peroximonosulfato usando MnOOH nanométrico: investigação de parâmetros operacionais e mudanças na superfície do catalisador
title In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface
spellingShingle In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface
Núñez de la Rosa, Yeison Neder
Advanced oxidation process
Heterogeneous catalysis
Emerging contaminants
Hydroxyl radicals
PMS induced Mn(IV) reduction
Processos oxidativos avançados
Catálise heterogênea
Contaminantes emergentes
Radical hidroxila
Redução de Mn(IV) induzida por PMS
CIENCIAS EXATAS E DA TERRA::QUIMICA
title_short In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface
title_full In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface
title_fullStr In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface
title_full_unstemmed In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface
title_sort In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface
author Núñez de la Rosa, Yeison Neder
author_facet Núñez de la Rosa, Yeison Neder
author_role author
dc.contributor.authorlattes.por.fl_str_mv http://lattes.cnpq.br/7299008176913606
dc.contributor.authororcid.por.fl_str_mv https://orcid.org/0000-0001-9564-8384
dc.contributor.advisor1orcid.por.fl_str_mv https://orcid.org/0000-0001-6099-9846
dc.contributor.author.fl_str_mv Núñez de la Rosa, Yeison Neder
dc.contributor.advisor1.fl_str_mv Aquino, José Mario de
dc.contributor.advisor1Lattes.fl_str_mv http://lattes.cnpq.br/8847710280926769
dc.contributor.authorID.fl_str_mv 6b43d67d-c118-4e98-8344-dd4821767557
contributor_str_mv Aquino, José Mario de
dc.subject.eng.fl_str_mv Advanced oxidation process
Heterogeneous catalysis
Emerging contaminants
Hydroxyl radicals
PMS induced Mn(IV) reduction
topic Advanced oxidation process
Heterogeneous catalysis
Emerging contaminants
Hydroxyl radicals
PMS induced Mn(IV) reduction
Processos oxidativos avançados
Catálise heterogênea
Contaminantes emergentes
Radical hidroxila
Redução de Mn(IV) induzida por PMS
CIENCIAS EXATAS E DA TERRA::QUIMICA
dc.subject.por.fl_str_mv Processos oxidativos avançados
Catálise heterogênea
Contaminantes emergentes
Radical hidroxila
Redução de Mn(IV) induzida por PMS
dc.subject.cnpq.fl_str_mv CIENCIAS EXATAS E DA TERRA::QUIMICA
description Nanometric MnOOH compound was synthesized by a green approach, characterized, and used to remove ciprofloxacin (CIP) antibiotic by in situ chemical oxidation using peroxymonosulfate (PMS). The effects of varying concentrations of MnOOH, PMS and pH, on morphological, structural, chemical, and electrochemical changes were studied during and after the experiments. The CIP molecule was completely oxidized and partially mineralized (~ 60%) after 6 h under acidic conditions. The mechanism of CIP degradation was induced by PMS activated oxidants (HO• and 1O2) and, to a lesser extent, directly on the surface of MnOOH. The latter process was evidenced by transmission electron microscopy showing the formation of an amorphous shell (MnOx) over MnOOH crystallites, as verified using X-ray photoelectron spectroscopy and the subsequent increase of the charge transfer resistance that hindered a further electron transfer to the PMS oxidant. Such behavior is recoverable when using a freshly prepared PMS solution.
publishDate 2023
dc.date.accessioned.fl_str_mv 2023-07-26T13:32:26Z
dc.date.available.fl_str_mv 2023-07-26T13:32:26Z
dc.date.issued.fl_str_mv 2023-05-24
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/doctoralThesis
format doctoralThesis
status_str publishedVersion
dc.identifier.citation.fl_str_mv NÚÑEZ DE LA ROSA, Yeison Neder. In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface. 2023. Tese (Doutorado em Química) – Universidade Federal de São Carlos, São Carlos, 2023. Disponível em: https://repositorio.ufscar.br/handle/ufscar/18318.
dc.identifier.uri.fl_str_mv https://repositorio.ufscar.br/handle/ufscar/18318
identifier_str_mv NÚÑEZ DE LA ROSA, Yeison Neder. In situ chemical oxidation of ciprofloxacin by activated peroxymonosulfate using nanometric MnOOH: investigation of operational parameters and changes on the catalyst surface. 2023. Tese (Doutorado em Química) – Universidade Federal de São Carlos, São Carlos, 2023. Disponível em: https://repositorio.ufscar.br/handle/ufscar/18318.
url https://repositorio.ufscar.br/handle/ufscar/18318
dc.language.iso.fl_str_mv eng
language eng
dc.relation.confidence.fl_str_mv 600
600
dc.relation.authority.fl_str_mv f136e88e-dfa7-4409-8a6e-063cb254af2e
dc.rights.driver.fl_str_mv Attribution-NonCommercial-NoDerivs 3.0 Brazil
http://creativecommons.org/licenses/by-nc-nd/3.0/br/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv Attribution-NonCommercial-NoDerivs 3.0 Brazil
http://creativecommons.org/licenses/by-nc-nd/3.0/br/
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Universidade Federal de São Carlos
Câmpus São Carlos
dc.publisher.program.fl_str_mv Programa de Pós-Graduação em Química - PPGQ
dc.publisher.initials.fl_str_mv UFSCar
publisher.none.fl_str_mv Universidade Federal de São Carlos
Câmpus São Carlos
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instname:Universidade Federal de São Carlos (UFSCAR)
instacron:UFSCAR
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reponame_str Repositório Institucional da UFSCAR
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