Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto

Detalhes bibliográficos
Autor(a) principal: Fernandes, Carlos Henrique Magalhães
Data de Publicação: 2021
Tipo de documento: Tese
Idioma: por
Título da fonte: Repositório Institucional da UFSCAR
Texto Completo: https://repositorio.ufscar.br/handle/ufscar/14112
Resumo: In this work, two different advanced oxidation processes (AOP) were investigated: i) electrochemical processes (electro FeredFenton and photoelectro Fered-Fenton with BDD and DSA® electrodes under UVA/UVC irradiation (9 W) and ii) AOP based on solar radiation and using distinct oxidants (HOCℓ, H2O2, S2O82–, HSO5–) in the presence and absence of Fe2+ ions for the oxidation and mineralization of imidacloprid insecticide (IMDC: 50 mg L– 1). The FEF-Fered process, under UVA/UVC irradiation and HOCℓ/UVC with BDD and DSA®, respectively, had similar performances for the oxidation and mineralization of IMDC, reaching ~90% removal with an energy consumption of only ~0.3 kW hg–1. IMDC was readily oxidized when H2O2 concentrations of 50 and 100 mg L–1 (<30 min) compared to 25 mg L–1 (~90 min) were used. A similar behavior considering the removal of TOC was observed when using 50 (6.4 ±0.6 × 10–3 min–1) and 100 mg L–1 of H2O2 (5.91 ±0.04 × 10–3 min–1). High oxidation (100%; <30 min) and mineralization values (~9 × 10–3 min–1) were observed for the HOCℓ/UVC process in a wide pH range (3 to 6). The amount of electrogenerated oxidant (HOCℓ) for the HOCℓ/UVC process was determined and remained among 5 to 15 mg L–1. The HOCℓ/UVC process led to a more oxidizing chemical environment leading to the rupture of the IMDC imidazolic ring, in addition to dechlorination and hydroxylation reactions in all analyzed compounds. Such reactions were also observed for the FEF-Fered/UVA/Fe2+ process. Taking into account the main produced carboxylic acids, oxamic, succinic, formic and propionic acids were identified for the FEF-Fered/UVA/Fe2+ process, in addition to maleic, oxamic, malonic, glycolic, formic, acetic and dichloroacetic for the HOCℓ/UVC process. For the second investigated AOP based on solar radiation, all oxidants led to oxidation of IMDC in 3 h; however, removal levels of TOC were only significant when H2O2 and HOCℓ (~70% and ~60%, respectively) were used after 6 h. The use of Fe2+ (0.5 or 1.0 mmol L–1) did not show significant improvement in the oxidation and mineralization of IMDC.
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spelling Fernandes, Carlos Henrique MagalhãesAquino, José Mario dehttp://lattes.cnpq.br/8847710280926769http://lattes.cnpq.br/46697478698453390717d478-9b1f-4170-835d-76627dd667422021-04-15T12:32:06Z2021-04-15T12:32:06Z2021-02-12FERNANDES, Carlos Henrique Magalhães. Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto. 2021. Tese (Doutorado em Química) – Universidade Federal de São Carlos, São Carlos, 2021. Disponível em: https://repositorio.ufscar.br/handle/ufscar/14112.https://repositorio.ufscar.br/handle/ufscar/14112In this work, two different advanced oxidation processes (AOP) were investigated: i) electrochemical processes (electro FeredFenton and photoelectro Fered-Fenton with BDD and DSA® electrodes under UVA/UVC irradiation (9 W) and ii) AOP based on solar radiation and using distinct oxidants (HOCℓ, H2O2, S2O82–, HSO5–) in the presence and absence of Fe2+ ions for the oxidation and mineralization of imidacloprid insecticide (IMDC: 50 mg L– 1). The FEF-Fered process, under UVA/UVC irradiation and HOCℓ/UVC with BDD and DSA®, respectively, had similar performances for the oxidation and mineralization of IMDC, reaching ~90% removal with an energy consumption of only ~0.3 kW hg–1. IMDC was readily oxidized when H2O2 concentrations of 50 and 100 mg L–1 (<30 min) compared to 25 mg L–1 (~90 min) were used. A similar behavior considering the removal of TOC was observed when using 50 (6.4 ±0.6 × 10–3 min–1) and 100 mg L–1 of H2O2 (5.91 ±0.04 × 10–3 min–1). High oxidation (100%; <30 min) and mineralization values (~9 × 10–3 min–1) were observed for the HOCℓ/UVC process in a wide pH range (3 to 6). The amount of electrogenerated oxidant (HOCℓ) for the HOCℓ/UVC process was determined and remained among 5 to 15 mg L–1. The HOCℓ/UVC process led to a more oxidizing chemical environment leading to the rupture of the IMDC imidazolic ring, in addition to dechlorination and hydroxylation reactions in all analyzed compounds. Such reactions were also observed for the FEF-Fered/UVA/Fe2+ process. Taking into account the main produced carboxylic acids, oxamic, succinic, formic and propionic acids were identified for the FEF-Fered/UVA/Fe2+ process, in addition to maleic, oxamic, malonic, glycolic, formic, acetic and dichloroacetic for the HOCℓ/UVC process. For the second investigated AOP based on solar radiation, all oxidants led to oxidation of IMDC in 3 h; however, removal levels of TOC were only significant when H2O2 and HOCℓ (~70% and ~60%, respectively) were used after 6 h. The use of Fe2+ (0.5 or 1.0 mmol L–1) did not show significant improvement in the oxidation and mineralization of IMDC.Neste trabalho, dois diferentes processos de oxidação avançada (POA) foram investigados: i) processos eletroquímicos (eletro-Fered-Fenton e fotoeletro Fered-Fenton com eletrodos de Diamante Dopado com Boro (DDB) e Ânodo Dimensionalmente Estável (ADE) sob irradiação UVA/UVC (9 W) e ii) POA baseado na radiação solar usando distintos oxidantes (HOCℓ, H2O2, S2O82–, HSO5–) na presença e ausência de íons Fe2+ para oxidação e mineralização do imidacloprida (IMDC: 50 mg L–1). O processo FEF-Fered (DDB/H2O2/UVAUVC/Fe2+), e o HOCℓ/UVC com DDB e ADE, respectivamente, tiveram desempenhos similares para a oxidação e mineralização do IMDC, alcançando ~90% de remoção com consumo energético (CE) de apenas ~0,3 kW h g–1. O IMDC foi prontamente oxidado ao se utilizar concentrações de H2O2 de 50 e 100 mg L–1 (<30 min) em comparação a 25 mg L–1 (~90 min). Um comportamento similar em relação à remoção de COT foi observado ao usar 50 (6,4 ±0,6 × 10–3 min–1) e 100 mg L–1 de H2O2 (5,91 ±0,04 × 10–3 min–1). Altos valores de oxidação (100%; <30 min) e de remoção do COT (~9 × 10–3 min–1) foram observados para o processo HOCℓ/UVC em ampla faixa de pH (3 a 6). A quantidade de oxidante (HOCℓ) eletrogerado para o processo HOCℓ/UVC foi determinada e permaneceu entre 5 a 15 mg L–1. O processo HOCℓ/UVC conduziu à um ambiente químico mais oxidante, provocando a ruptura do anel imidazólico do IMDC, além de reações de hidroxilação em todos compostos analisados e descloração. Tais reações também foram observadas para o processo FEF-Fered/UVA/Fe2+. Com relação aos ácidos carboxílicos, identificou-se os ácidos oxâmico, succínico, fórmico e propiônico para o processo FEF-Fered/UVA/Fe2+ além de maléico, oxâmico, malônico, glicólico, fórmico, ácético e dicloroacético para o processo HOCℓ/UVC. Para o segundo POA investigado, baseado na radiação solar, todos os oxidantes promoveram a oxidação do IMDC em 3 h; entretanto, o teor de remoção de COT foi significativo quando se utilizou H2O2 e HOCℓ (~70% e ~60%, respectivamente) após 6 h. O uso de Fe2+ (0,5 ou 1,0 mmol L–1) não apresentou melhora significativa na oxidação e mineralização do IMDC.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)CAPES: Código de Financiamento 001porUniversidade 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/openAccessOxidation byproductsSynthetic organic compoundsHydroxyl radicalHeterogeneous reactionHomogeneous reactionCIENCIAS EXATAS E DA TERRA::QUIMICAEstudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-pilotoOn the performance of different advanced electrochemical oxidation processes (e-AOP) and assessment of a semi-pilot scale solar reactorinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisf136e88e-dfa7-4409-8a6e-063cb254af2ereponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINALTese Doutorado Carlos Henrique.pdfTese Doutorado Carlos Henrique.pdfapplication/pdf4590303https://repositorio.ufscar.br/bitstream/ufscar/14112/2/Tese%20Doutorado%20Carlos%20Henrique.pdf73bce7921145f7e296e98ce765584ca4MD52Carta_homologação.pdfCarta_homologação.pdfCARLOS HENRIQUE MAGALHÃES FERNANDESapplication/pdf735199https://repositorio.ufscar.br/bitstream/ufscar/14112/1/Carta_homologa%c3%a7%c3%a3o.pdf6c62b6d94e65b1f06c991b219f3d28c0MD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8811https://repositorio.ufscar.br/bitstream/ufscar/14112/3/license_rdfe39d27027a6cc9cb039ad269a5db8e34MD53TEXTTese Doutorado Carlos Henrique.pdf.txtTese Doutorado Carlos Henrique.pdf.txtExtracted texttext/plain241692https://repositorio.ufscar.br/bitstream/ufscar/14112/4/Tese%20Doutorado%20Carlos%20Henrique.pdf.txtbac26dbf273420ba8a479d233d77e065MD54Carta_homologação.pdf.txtCarta_homologação.pdf.txtExtracted texttext/plain1411https://repositorio.ufscar.br/bitstream/ufscar/14112/6/Carta_homologa%c3%a7%c3%a3o.pdf.txtb3796cd2561c9d9aa3bfd18be2677e27MD56THUMBNAILTese Doutorado Carlos Henrique.pdf.jpgTese Doutorado Carlos Henrique.pdf.jpgIM Thumbnailimage/jpeg9516https://repositorio.ufscar.br/bitstream/ufscar/14112/5/Tese%20Doutorado%20Carlos%20Henrique.pdf.jpg495a939ce1ecfac5cac77e685704a104MD55Carta_homologação.pdf.jpgCarta_homologação.pdf.jpgIM Thumbnailimage/jpeg13291https://repositorio.ufscar.br/bitstream/ufscar/14112/7/Carta_homologa%c3%a7%c3%a3o.pdf.jpg8941c1b5e011138dfab3f44350c2d08eMD57ufscar/141122023-09-18 18:32:09.148oai:repositorio.ufscar.br:ufscar/14112Repositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestopendoar:43222023-09-18T18:32:09Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false
dc.title.por.fl_str_mv Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto
dc.title.alternative.eng.fl_str_mv On the performance of different advanced electrochemical oxidation processes (e-AOP) and assessment of a semi-pilot scale solar reactor
title Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto
spellingShingle Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto
Fernandes, Carlos Henrique Magalhães
Oxidation byproducts
Synthetic organic compounds
Hydroxyl radical
Heterogeneous reaction
Homogeneous reaction
CIENCIAS EXATAS E DA TERRA::QUIMICA
title_short Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto
title_full Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto
title_fullStr Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto
title_full_unstemmed Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto
title_sort Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto
author Fernandes, Carlos Henrique Magalhães
author_facet Fernandes, Carlos Henrique Magalhães
author_role author
dc.contributor.authorlattes.por.fl_str_mv http://lattes.cnpq.br/4669747869845339
dc.contributor.author.fl_str_mv Fernandes, Carlos Henrique Magalhães
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 0717d478-9b1f-4170-835d-76627dd66742
contributor_str_mv Aquino, José Mario de
dc.subject.eng.fl_str_mv Oxidation byproducts
Synthetic organic compounds
Hydroxyl radical
Heterogeneous reaction
Homogeneous reaction
topic Oxidation byproducts
Synthetic organic compounds
Hydroxyl radical
Heterogeneous reaction
Homogeneous reaction
CIENCIAS EXATAS E DA TERRA::QUIMICA
dc.subject.cnpq.fl_str_mv CIENCIAS EXATAS E DA TERRA::QUIMICA
description In this work, two different advanced oxidation processes (AOP) were investigated: i) electrochemical processes (electro FeredFenton and photoelectro Fered-Fenton with BDD and DSA® electrodes under UVA/UVC irradiation (9 W) and ii) AOP based on solar radiation and using distinct oxidants (HOCℓ, H2O2, S2O82–, HSO5–) in the presence and absence of Fe2+ ions for the oxidation and mineralization of imidacloprid insecticide (IMDC: 50 mg L– 1). The FEF-Fered process, under UVA/UVC irradiation and HOCℓ/UVC with BDD and DSA®, respectively, had similar performances for the oxidation and mineralization of IMDC, reaching ~90% removal with an energy consumption of only ~0.3 kW hg–1. IMDC was readily oxidized when H2O2 concentrations of 50 and 100 mg L–1 (<30 min) compared to 25 mg L–1 (~90 min) were used. A similar behavior considering the removal of TOC was observed when using 50 (6.4 ±0.6 × 10–3 min–1) and 100 mg L–1 of H2O2 (5.91 ±0.04 × 10–3 min–1). High oxidation (100%; <30 min) and mineralization values (~9 × 10–3 min–1) were observed for the HOCℓ/UVC process in a wide pH range (3 to 6). The amount of electrogenerated oxidant (HOCℓ) for the HOCℓ/UVC process was determined and remained among 5 to 15 mg L–1. The HOCℓ/UVC process led to a more oxidizing chemical environment leading to the rupture of the IMDC imidazolic ring, in addition to dechlorination and hydroxylation reactions in all analyzed compounds. Such reactions were also observed for the FEF-Fered/UVA/Fe2+ process. Taking into account the main produced carboxylic acids, oxamic, succinic, formic and propionic acids were identified for the FEF-Fered/UVA/Fe2+ process, in addition to maleic, oxamic, malonic, glycolic, formic, acetic and dichloroacetic for the HOCℓ/UVC process. For the second investigated AOP based on solar radiation, all oxidants led to oxidation of IMDC in 3 h; however, removal levels of TOC were only significant when H2O2 and HOCℓ (~70% and ~60%, respectively) were used after 6 h. The use of Fe2+ (0.5 or 1.0 mmol L–1) did not show significant improvement in the oxidation and mineralization of IMDC.
publishDate 2021
dc.date.accessioned.fl_str_mv 2021-04-15T12:32:06Z
dc.date.available.fl_str_mv 2021-04-15T12:32:06Z
dc.date.issued.fl_str_mv 2021-02-12
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dc.identifier.citation.fl_str_mv FERNANDES, Carlos Henrique Magalhães. Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto. 2021. Tese (Doutorado em Química) – Universidade Federal de São Carlos, São Carlos, 2021. Disponível em: https://repositorio.ufscar.br/handle/ufscar/14112.
dc.identifier.uri.fl_str_mv https://repositorio.ufscar.br/handle/ufscar/14112
identifier_str_mv FERNANDES, Carlos Henrique Magalhães. Estudo de distintos processos oxidativos avançados eletroquímicos (e-POA) e teste de um reator solar em escala semi-piloto. 2021. Tese (Doutorado em Química) – Universidade Federal de São Carlos, São Carlos, 2021. Disponível em: https://repositorio.ufscar.br/handle/ufscar/14112.
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rights_invalid_str_mv Attribution-NonCommercial-NoDerivs 3.0 Brazil
http://creativecommons.org/licenses/by-nc-nd/3.0/br/
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dc.publisher.none.fl_str_mv Universidade Federal de São Carlos
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