Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes

Detalhes bibliográficos
Ano de defesa: 2021
Autor(a) principal: Rodríguez-Pérez, Adriana Patricia
Orientador(a): Não Informado pela instituição
Banca de defesa: Não Informado pela instituição
Tipo de documento: Dissertação
Tipo de acesso: Acesso aberto
Idioma: por
Instituição de defesa: Universidade Tecnológica Federal do Paraná
Curitiba
Brasil
Programa de Pós-Graduação em Ciência e Tecnologia Ambiental
UTFPR
Programa de Pós-Graduação: Não Informado pela instituição
Departamento: Não Informado pela instituição
País: Não Informado pela instituição
Palavras-chave em Português:
Link de acesso: http://repositorio.utfpr.edu.br/jspui/handle/1/30810
Resumo: Due to the limitation of conventional treatment processes, some contaminants are not efficiently removed, in this context, heterogeneous photocatalysis appears as an alternative for contaminant degradation. Recently, graphitic carbon nitride (g-C3N4) has attracted attention as a metal-free catalyst due to its characteristics of electronic conductivity, visible light absorption, and low cost. In this work, the synthesis of photocatalysts was proposed: g-C3N4 from urea (U) or melamine (M), called g-C3N4/U and g-C3N4/M via carbonization; and spherical heterostructures of chitosan (Q) with urea (U) or melamine (M), called: Q:U and Q:M in different proportions. The materials were characterized by: X-ray diffraction, with characteristic peaks at 12.92° (1 0 0) and 27.58° (0 0 2) , corresponding to the formation of g-C3N4, in addition to microcrystallinities associated with the chitosan (20°); diffuse reflectance spectroscopy, , determining band gap values around 3.15 eV; X-ray photoelectron spectroscopy, having the binding energies associated with the intermediate (melem) of g-C3N4/U also confirmed also with the data of the C/N radio in the CHN analysis, FTIR showing the functional groups of the tri-s-triazines (structural units of g-C3N4) and finally by scanning electron microscopy, morphological images of the material were taken before and after photodegradations, where morphological images of the material were obtained before and after photodegradations, observing that the chitosan spheres did not show wear. In the photocatalytic studies, the removal of model pollutant – Rhodamine B (RhB) dye was evaluated with all synthesized materials; in the desethyl-atrazine (DEA) and Rifampicin (RIF) was used the materials that showed better removal of the model pollutant; in addition to the evaluation of physicochemical parameters using g-C3N4/U and g-C3N4/M before (pre-treatment) and after (post-treatment) of biological treatment, using an anaerobic upflow reactor and sludge blanket (UASB type) in a hospital wastewater. Different configurations were used for each degradation: type of radiation (UVA-Vis, Vis) / lamp (high pressure of mercury vapor, LED, Halogen) configurations were used with ad without the use of filter (f) cut at λ > 420 nm, in addition to using a suspended lamp (S) at 10 cm from the solution or submerged lamp (M). Preliminary results in the UVAM region were obtained with dye degradation of up to 99.9%. In the Vis LEDS region, there was an increase of 9.3% of g-C3N4/M up to 15.2% with chitosan (3Q:1M), showing that recombination problems are improved by mixing the photocatalyst with the carbon matrix (chitosan) as well as being easily separated from the solution and reused. In the removal of DEA and RIF, in all configurations, higher removal efficiencies were obtained with the heterostructures (3Q:1U, 3Q:1M) compared to pure g-C3N4, obtaining degradations in up to 30-45 minutes in some cases. The raw hospital effluent, after the anaerobic biological treatment by a UASB reactor, obtained a considerable decrease in COD and BOD5, thus establishing a degradation of almost 87% of the organic matter. In the combined process, COD removal efficiencies of 84.7% for g-C3N4/U and 77% for g-C3N4/M were obtained. Thus, materials based on g-C3N4 constitute an alternative for use in photocatalytic processes.
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spelling Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentesSynthesis and characterization of chitosan/ G-C3n4 heterostructures for micropollutants photodegradationCatalisadoresCatálise heterogêneaCarbonizaçãoÁgua - ContaminaçãoPoluentesCatalystsHeterogeneous catalysesCarbonizationWater - ContaminationPollutantsCNPQ::ENGENHARIAS::ENGENHARIA SANITARIACiências AmbientaisDue to the limitation of conventional treatment processes, some contaminants are not efficiently removed, in this context, heterogeneous photocatalysis appears as an alternative for contaminant degradation. Recently, graphitic carbon nitride (g-C3N4) has attracted attention as a metal-free catalyst due to its characteristics of electronic conductivity, visible light absorption, and low cost. In this work, the synthesis of photocatalysts was proposed: g-C3N4 from urea (U) or melamine (M), called g-C3N4/U and g-C3N4/M via carbonization; and spherical heterostructures of chitosan (Q) with urea (U) or melamine (M), called: Q:U and Q:M in different proportions. The materials were characterized by: X-ray diffraction, with characteristic peaks at 12.92° (1 0 0) and 27.58° (0 0 2) , corresponding to the formation of g-C3N4, in addition to microcrystallinities associated with the chitosan (20°); diffuse reflectance spectroscopy, , determining band gap values around 3.15 eV; X-ray photoelectron spectroscopy, having the binding energies associated with the intermediate (melem) of g-C3N4/U also confirmed also with the data of the C/N radio in the CHN analysis, FTIR showing the functional groups of the tri-s-triazines (structural units of g-C3N4) and finally by scanning electron microscopy, morphological images of the material were taken before and after photodegradations, where morphological images of the material were obtained before and after photodegradations, observing that the chitosan spheres did not show wear. In the photocatalytic studies, the removal of model pollutant – Rhodamine B (RhB) dye was evaluated with all synthesized materials; in the desethyl-atrazine (DEA) and Rifampicin (RIF) was used the materials that showed better removal of the model pollutant; in addition to the evaluation of physicochemical parameters using g-C3N4/U and g-C3N4/M before (pre-treatment) and after (post-treatment) of biological treatment, using an anaerobic upflow reactor and sludge blanket (UASB type) in a hospital wastewater. Different configurations were used for each degradation: type of radiation (UVA-Vis, Vis) / lamp (high pressure of mercury vapor, LED, Halogen) configurations were used with ad without the use of filter (f) cut at λ > 420 nm, in addition to using a suspended lamp (S) at 10 cm from the solution or submerged lamp (M). Preliminary results in the UVAM region were obtained with dye degradation of up to 99.9%. In the Vis LEDS region, there was an increase of 9.3% of g-C3N4/M up to 15.2% with chitosan (3Q:1M), showing that recombination problems are improved by mixing the photocatalyst with the carbon matrix (chitosan) as well as being easily separated from the solution and reused. In the removal of DEA and RIF, in all configurations, higher removal efficiencies were obtained with the heterostructures (3Q:1U, 3Q:1M) compared to pure g-C3N4, obtaining degradations in up to 30-45 minutes in some cases. The raw hospital effluent, after the anaerobic biological treatment by a UASB reactor, obtained a considerable decrease in COD and BOD5, thus establishing a degradation of almost 87% of the organic matter. In the combined process, COD removal efficiencies of 84.7% for g-C3N4/U and 77% for g-C3N4/M were obtained. Thus, materials based on g-C3N4 constitute an alternative for use in photocatalytic processes.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Os processos convencionais de tratamento não removem eficientemente alguns contaminantes, neste contexto, a fotocatálise heterogênea surge como uma alternativa para sua degradação. Recentemente, o nitreto de carbono grafítico (g-C3N4) atraiu a atenção como um catalisador livre de metal devido às suas características de condutividade eletrônica, absorção de luz visível e baixo custo. Neste trabalho foi proposto, a síntese de fotocatalisadores: g-C3N4 a partir da uréia (U) ou melamina (M), denominados g-C3N4/U e g-C3N4/M via carbonização; e de heteroestruturas esféricas de quitosana com uréia ou melamina, denominados: Q:U e Q:M em diferentes proporções. Os materiais foram caracterizados por: difração de raio X, com picos característicos, em 12,92° (1 0 0) e 27,58° (0 0 2), correspondendo à formação de g-C3N4, além de microcristalinidades associadas à quitosana (20°); espectroscopia de reflectância difusa, determinando valores de band gap em torno de 3,15 eV; espectroscopia de fotoelétrons por raios X, tendo as energias de ligação associadas ao intermediário (melem) de g-C3N4/U confirmado também com os dados da relação C/N na análise CHN, FTIR, mostrando os grupos funcionais das tri-s-triazinas (unidades estruturais do g-C3N4) e finalmente por microscopia eletrônica de varredura onde foram obtidas imagens morfológicas do material antes e após fotodegradações, observando que as esferas com quitosana não apresentavam desgaste. Nos estudos fotocatalíticos foi avaliada a remoção de poluente modelo – corante Rodamina B (RhB) com todos os materiais sintetizados; o fármaco Rifampicina (RIF) e a desetil-atrazina (DEA) com os materiais que apresentaram melhor remoção do poluente modelo; além da avaliação dos parâmetros físico-químicos usando o g-C3N4/U e g-C3N4/M antes (pré-tratamento) e após (póstratamento) de tratamento biológico, usando um reator anaeróbio de fluxo ascendente e manta de lodo (tipo UASB) em efluente hospitalar. Para cada degradação se usaram diferentes configurações: tipo de radiação (UVA-Vis, Vis) / lâmpada (de alta pressão de vapor de mercúrio, LED, Halógena) suspensa (S) a 10 cm da solução ou mergulhada (M). Resultados preliminares na região UVAM foram obtidos com degradação do corantes de até 99,9 %. Na região Vis LEDS se obteve aumento de 9,3% de g-C3N4/M até 15,2% com a quitosana (3Q:1M), mostrando que problemas de recombinação são melhorados com a mistura do fotocatalisador com a matriz carbonada (quitosana), além de ser separadas facilmente da solução e reutilizadas. Na remoção de desetil-atrazina (DEA) e rifampicina (RIF), em todas as configurações, se obteve maiores eficiências de remoção com as heteroestruturas (3Q:1U e 3Q:1M) em comparação com g-C3N4 puro, obtendo-se degradações em 30-45 minutos em alguns casos. O efluente hospitalar bruto, após o tratamento biológico anaeróbio por reator tipo UASB obteve diminuição considerável da DQO e DBO5 estabelecendo-se assim degradação de quase 87% da matéria orgânica. No processo combinado foram obtidas eficiências de remoção de DQO de 84,7% para o g-C3N4/U e 77% para o g-C3N4. Assim, os materiais baseados em g-C3N4 constituem uma alternativa de utilização nos processos fotocatalíticos.Universidade Tecnológica Federal do ParanáCuritibaBrasilPrograma de Pós-Graduação em Ciência e Tecnologia AmbientalUTFPRLiz, Marcus Vinicius dehttps://orcid.org/0000-0003-1370-3365http://lattes.cnpq.br/6959317686443946Prola, Liziê Daniela Tentlerhttps://orcid.org/0000-0001-9176-5700http://lattes.cnpq.br/6809940830015445Carvalho, Karina Querne dehttps://orcid.org/0000-0003-4577-7537http://lattes.cnpq.br/8055585859691419Liz, Marcus Vinicius dehttps://orcid.org/0000-0003-1370-3365http://lattes.cnpq.br/6959317686443946Zamora, Patricio Guillermo Peraltahttps://orcid.org/0000-0002-9956-8442http://lattes.cnpq.br/8308983281636531Rodríguez-Pérez, Adriana Patricia2023-03-10T19:27:32Z2023-03-10T19:27:32Z2021-10-20info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisapplication/pdfRODRÍGUEZ-PÉREZ, Adriana Patricia. Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes. 2021. Dissertação (Mestrado em Ciência e Tecnologia Ambiental) - Universidade Tecnológica Federal do Paraná, Curitiba, 2021.http://repositorio.utfpr.edu.br/jspui/handle/1/30810porhttp://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessreponame:Repositório Institucional da UTFPR (da Universidade Tecnológica Federal do Paraná (RIUT))instname:Universidade Tecnológica Federal do Paraná (UTFPR)instacron:UTFPR2023-03-11T06:07:25Zoai:repositorio.utfpr.edu.br:1/30810Repositório InstitucionalPUBhttp://repositorio.utfpr.edu.br:8080/oai/requestriut@utfpr.edu.br || sibi@utfpr.edu.bropendoar:2023-03-11T06:07:25Repositório Institucional da UTFPR (da Universidade Tecnológica Federal do Paraná (RIUT)) - Universidade Tecnológica Federal do Paraná (UTFPR)false
dc.title.none.fl_str_mv Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes
Synthesis and characterization of chitosan/ G-C3n4 heterostructures for micropollutants photodegradation
title Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes
spellingShingle Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes
Rodríguez-Pérez, Adriana Patricia
Catalisadores
Catálise heterogênea
Carbonização
Água - Contaminação
Poluentes
Catalysts
Heterogeneous catalyses
Carbonization
Water - Contamination
Pollutants
CNPQ::ENGENHARIAS::ENGENHARIA SANITARIA
Ciências Ambientais
title_short Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes
title_full Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes
title_fullStr Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes
title_full_unstemmed Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes
title_sort Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes
author Rodríguez-Pérez, Adriana Patricia
author_facet Rodríguez-Pérez, Adriana Patricia
author_role author
dc.contributor.none.fl_str_mv Liz, Marcus Vinicius de
https://orcid.org/0000-0003-1370-3365
http://lattes.cnpq.br/6959317686443946
Prola, Liziê Daniela Tentler
https://orcid.org/0000-0001-9176-5700
http://lattes.cnpq.br/6809940830015445
Carvalho, Karina Querne de
https://orcid.org/0000-0003-4577-7537
http://lattes.cnpq.br/8055585859691419
Liz, Marcus Vinicius de
https://orcid.org/0000-0003-1370-3365
http://lattes.cnpq.br/6959317686443946
Zamora, Patricio Guillermo Peralta
https://orcid.org/0000-0002-9956-8442
http://lattes.cnpq.br/8308983281636531
dc.contributor.author.fl_str_mv Rodríguez-Pérez, Adriana Patricia
dc.subject.por.fl_str_mv Catalisadores
Catálise heterogênea
Carbonização
Água - Contaminação
Poluentes
Catalysts
Heterogeneous catalyses
Carbonization
Water - Contamination
Pollutants
CNPQ::ENGENHARIAS::ENGENHARIA SANITARIA
Ciências Ambientais
topic Catalisadores
Catálise heterogênea
Carbonização
Água - Contaminação
Poluentes
Catalysts
Heterogeneous catalyses
Carbonization
Water - Contamination
Pollutants
CNPQ::ENGENHARIAS::ENGENHARIA SANITARIA
Ciências Ambientais
description Due to the limitation of conventional treatment processes, some contaminants are not efficiently removed, in this context, heterogeneous photocatalysis appears as an alternative for contaminant degradation. Recently, graphitic carbon nitride (g-C3N4) has attracted attention as a metal-free catalyst due to its characteristics of electronic conductivity, visible light absorption, and low cost. In this work, the synthesis of photocatalysts was proposed: g-C3N4 from urea (U) or melamine (M), called g-C3N4/U and g-C3N4/M via carbonization; and spherical heterostructures of chitosan (Q) with urea (U) or melamine (M), called: Q:U and Q:M in different proportions. The materials were characterized by: X-ray diffraction, with characteristic peaks at 12.92° (1 0 0) and 27.58° (0 0 2) , corresponding to the formation of g-C3N4, in addition to microcrystallinities associated with the chitosan (20°); diffuse reflectance spectroscopy, , determining band gap values around 3.15 eV; X-ray photoelectron spectroscopy, having the binding energies associated with the intermediate (melem) of g-C3N4/U also confirmed also with the data of the C/N radio in the CHN analysis, FTIR showing the functional groups of the tri-s-triazines (structural units of g-C3N4) and finally by scanning electron microscopy, morphological images of the material were taken before and after photodegradations, where morphological images of the material were obtained before and after photodegradations, observing that the chitosan spheres did not show wear. In the photocatalytic studies, the removal of model pollutant – Rhodamine B (RhB) dye was evaluated with all synthesized materials; in the desethyl-atrazine (DEA) and Rifampicin (RIF) was used the materials that showed better removal of the model pollutant; in addition to the evaluation of physicochemical parameters using g-C3N4/U and g-C3N4/M before (pre-treatment) and after (post-treatment) of biological treatment, using an anaerobic upflow reactor and sludge blanket (UASB type) in a hospital wastewater. Different configurations were used for each degradation: type of radiation (UVA-Vis, Vis) / lamp (high pressure of mercury vapor, LED, Halogen) configurations were used with ad without the use of filter (f) cut at λ > 420 nm, in addition to using a suspended lamp (S) at 10 cm from the solution or submerged lamp (M). Preliminary results in the UVAM region were obtained with dye degradation of up to 99.9%. In the Vis LEDS region, there was an increase of 9.3% of g-C3N4/M up to 15.2% with chitosan (3Q:1M), showing that recombination problems are improved by mixing the photocatalyst with the carbon matrix (chitosan) as well as being easily separated from the solution and reused. In the removal of DEA and RIF, in all configurations, higher removal efficiencies were obtained with the heterostructures (3Q:1U, 3Q:1M) compared to pure g-C3N4, obtaining degradations in up to 30-45 minutes in some cases. The raw hospital effluent, after the anaerobic biological treatment by a UASB reactor, obtained a considerable decrease in COD and BOD5, thus establishing a degradation of almost 87% of the organic matter. In the combined process, COD removal efficiencies of 84.7% for g-C3N4/U and 77% for g-C3N4/M were obtained. Thus, materials based on g-C3N4 constitute an alternative for use in photocatalytic processes.
publishDate 2021
dc.date.none.fl_str_mv 2021-10-20
2023-03-10T19:27:32Z
2023-03-10T19:27:32Z
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/masterThesis
format masterThesis
status_str publishedVersion
dc.identifier.uri.fl_str_mv RODRÍGUEZ-PÉREZ, Adriana Patricia. Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes. 2021. Dissertação (Mestrado em Ciência e Tecnologia Ambiental) - Universidade Tecnológica Federal do Paraná, Curitiba, 2021.
http://repositorio.utfpr.edu.br/jspui/handle/1/30810
identifier_str_mv RODRÍGUEZ-PÉREZ, Adriana Patricia. Síntese e caracterização de heteroestruturas de quitosana/ G-C3n4 para fotodegradação de micropoluentes. 2021. Dissertação (Mestrado em Ciência e Tecnologia Ambiental) - Universidade Tecnológica Federal do Paraná, Curitiba, 2021.
url http://repositorio.utfpr.edu.br/jspui/handle/1/30810
dc.language.iso.fl_str_mv por
language por
dc.rights.driver.fl_str_mv http://creativecommons.org/licenses/by/4.0/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Universidade Tecnológica Federal do Paraná
Curitiba
Brasil
Programa de Pós-Graduação em Ciência e Tecnologia Ambiental
UTFPR
publisher.none.fl_str_mv Universidade Tecnológica Federal do Paraná
Curitiba
Brasil
Programa de Pós-Graduação em Ciência e Tecnologia Ambiental
UTFPR
dc.source.none.fl_str_mv reponame:Repositório Institucional da UTFPR (da Universidade Tecnológica Federal do Paraná (RIUT))
instname:Universidade Tecnológica Federal do Paraná (UTFPR)
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instname_str Universidade Tecnológica Federal do Paraná (UTFPR)
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institution UTFPR
reponame_str Repositório Institucional da UTFPR (da Universidade Tecnológica Federal do Paraná (RIUT))
collection Repositório Institucional da UTFPR (da Universidade Tecnológica Federal do Paraná (RIUT))
repository.name.fl_str_mv Repositório Institucional da UTFPR (da Universidade Tecnológica Federal do Paraná (RIUT)) - Universidade Tecnológica Federal do Paraná (UTFPR)
repository.mail.fl_str_mv riut@utfpr.edu.br || sibi@utfpr.edu.br
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