Catalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-Fenton
Ano de defesa: | 2016 |
---|---|
Autor(a) principal: | |
Orientador(a): | |
Banca de defesa: | , |
Tipo de documento: | Dissertação |
Tipo de acesso: | Acesso aberto |
Idioma: | por |
Instituição de defesa: |
Universidade Federal de Santa Maria
Centro de Tecnologia |
Programa de Pós-Graduação: |
Programa de Pós-Graduação em Engenharia Química
|
Departamento: |
Engenharia Química
|
País: |
Brasil
|
Palavras-chave em Português: | |
Palavras-chave em Inglês: | |
Área do conhecimento CNPq: | |
Link de acesso: | http://repositorio.ufsm.br/handle/1/17690 |
Resumo: | This work evaluated the synthesis of hierarchical Fe2O3/ZSM -5 catalysts and their catalytic activity in the degradation of azo dye Yellow Tartrazine in photo-Fenton reaction. The chitin powder was applied as a mesopore template in the gel synthesis of ZSM -5, being removed after its crystallization by heat treatment. Removal of chitin generated voids, resulting in the formation of meso and macropores in the microporous structure of ZSM -5.The deposition of iron oxide nanoparticles on the zeolite was performed using the impregnation technique. Through the XRD analysis, it was observed that zeolites obtained showed typical MFI structure and, as higher the amount of chitin added in preparation of the synthesis gel, the lower the crystallinity of the material. Furthermore, the increase in chitin contents promoted a wide distribution range of meso and macropores in the zeolite, resulting in an increase in average pore size, as well as a larger volume, found, through analysis of N2 adsorption / desorption. Through the micrograph analysis of the obtained catalysts, it can be seen better dispersion of iron oxide on the hierarchical zeolite, which was attributed to higher porosity of the surface, resulting in higher anchor points for the iron oxide be deposited, and also in the formation of smaller sizes of clusters on the support. Unlike what was observed in the hierarchical support, the dispersion of iron oxide was less homogeneous in the microporous zeolite, resulting in a larger size of agglomerates on its surface. These characteristics in the structure of the catalysts had a strong influence on the catalytic activity of dye degradation by photo-Fenton process, where the hierarchical catalysts showed far superior results to catalysts with microporous surface as well as iron oxide unsupported, with the removal 99 %, 33 %, 10 % respectively. This enhancement in the reaction is due to the increased amount of active sites dispersed in the hierarchical catalyst available for decomposition of H2O2 and for formation of hydroxyl radicals, increasing the degradation rate of the dye. The optimum conditions for further removal of Yellow Tartrazine dye, used as a pollutant model in this work were determined by response surface methodology, which were pH 2.7, amount of catalyst of 0.4 g / L and 2 times the stoichiometric amount of H2O2 needed to complete mineralization of the colorant, promoting the removal of 99% of color of solution by 30 minutes of reaction. |
id |
UFSM_3a2aa8e165238479596b47e0e389390f |
---|---|
oai_identifier_str |
oai:repositorio.ufsm.br:1/17690 |
network_acronym_str |
UFSM |
network_name_str |
Biblioteca Digital de Teses e Dissertações do UFSM |
repository_id_str |
|
spelling |
2019-08-02T19:55:53Z2019-08-02T19:55:53Z2016-08-18http://repositorio.ufsm.br/handle/1/17690This work evaluated the synthesis of hierarchical Fe2O3/ZSM -5 catalysts and their catalytic activity in the degradation of azo dye Yellow Tartrazine in photo-Fenton reaction. The chitin powder was applied as a mesopore template in the gel synthesis of ZSM -5, being removed after its crystallization by heat treatment. Removal of chitin generated voids, resulting in the formation of meso and macropores in the microporous structure of ZSM -5.The deposition of iron oxide nanoparticles on the zeolite was performed using the impregnation technique. Through the XRD analysis, it was observed that zeolites obtained showed typical MFI structure and, as higher the amount of chitin added in preparation of the synthesis gel, the lower the crystallinity of the material. Furthermore, the increase in chitin contents promoted a wide distribution range of meso and macropores in the zeolite, resulting in an increase in average pore size, as well as a larger volume, found, through analysis of N2 adsorption / desorption. Through the micrograph analysis of the obtained catalysts, it can be seen better dispersion of iron oxide on the hierarchical zeolite, which was attributed to higher porosity of the surface, resulting in higher anchor points for the iron oxide be deposited, and also in the formation of smaller sizes of clusters on the support. Unlike what was observed in the hierarchical support, the dispersion of iron oxide was less homogeneous in the microporous zeolite, resulting in a larger size of agglomerates on its surface. These characteristics in the structure of the catalysts had a strong influence on the catalytic activity of dye degradation by photo-Fenton process, where the hierarchical catalysts showed far superior results to catalysts with microporous surface as well as iron oxide unsupported, with the removal 99 %, 33 %, 10 % respectively. This enhancement in the reaction is due to the increased amount of active sites dispersed in the hierarchical catalyst available for decomposition of H2O2 and for formation of hydroxyl radicals, increasing the degradation rate of the dye. The optimum conditions for further removal of Yellow Tartrazine dye, used as a pollutant model in this work were determined by response surface methodology, which were pH 2.7, amount of catalyst of 0.4 g / L and 2 times the stoichiometric amount of H2O2 needed to complete mineralization of the colorant, promoting the removal of 99% of color of solution by 30 minutes of reaction.O presente trabalho avaliou a síntese de catalisadores Fe2O3/ZSM-5 hierárquicos e sua atividade catalítica na degradação do azo corante Amarelo Tartrazina em reação foto-Fenton. A quitina em pó foi aplicada como molde de mesoporos no gel da síntese da ZSM-5, sendo removida após sua cristalização por meio de tratamento térmico. A remoção da quitina gerou espaços vazios, resultando na formação de meso e macroporos na estrutura microporosa da ZSM-5. A deposição de nanoparticulas de óxido de ferro sobre as zeólitas foi realizada utilizando a técnica de impregnação. Por meio das análises de DRX, observou-se que as zeólitas obtidas apresentaram estrutura típica MFI e que, conforme maior a quantidade de quitina adicionada na preparação do gel de síntese, menor a cristalinidade do material. Além disso, o aumento dos teores de quitina promoveu uma ampla faixa de distribuição de meso e macroporos nas zeólitas, resultando num aumento no tamanho médio de poros, assim como num maior volume, constatados, por meio de análise de adsorção/dessorção de N2. Através das análises de micrografia dos catalisadores obtidos, se pode constatar melhor dispersão do óxido de ferro sobre a zeólita hierárquica, à qual foi atribuída a maior porosidade de sua superfície, resultando em maiores pontos de ancoragem para o óxido de ferro se depositar e, também, na formação de menores tamanhos de aglomerados sobre o suporte. Diferentemente do observado no suporte hierárquico, a dispersão do óxido de ferro ocorreu de forma menos homogênea na zeólita microporosa, resultando em um maior tamanho de aglomerados em sua superfície. Essas características na estrutura dos catalisadores tiveram forte influência na atividade catalítica de degradação do corante por processo foto-Fenton, onde os catalisadores hierárquicos apresentaram resultados bem superiores aos catalisadores com superfície microporosa, assim como para o óxido de ferro não suportado, sendo a remoção de 99%, 33%, 10% respectivamente. Essa melhoria na reação deve-se a maior quantidade de sítios ativos dispersos no catalisador hierárquico, disponíveis para decomposição do H2O2 e formação dos radicais hidroxila, aumentando, assim, a velocidade de degradação do corante. As condições ótimas para maior remoção do corante Amarelo Tartrazina, utilizado como poluente modelo neste trabalho foram determinadas por meio de metodologia de superfície de resposta, as quais foram de pH 2,7, quantidade de catalisador de 0,4 g/L e 2 vezes a quantidade estequiométrica de H2O2 necessário para a mineralização completa do corante, promovendo remoção de 99 % da cor da solução em 30 minutos de reação.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESporUniversidade Federal de Santa MariaCentro de TecnologiaPrograma de Pós-Graduação em Engenharia QuímicaUFSMBrasilEngenharia QuímicaAttribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessCatalisadoresZeólita hierárquicaÓxido de ferroFoto-FentonQuitinaCatalystsHierarchical zeolitesIron oxidePhoto-FentonChitinCNPQ::ENGENHARIAS::ENGENHARIA QUIMICACatalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-FentonFe2O3/ZSM-5 hierarchical catalysts: effect of the mesoporosity support in the activity of iron oxide nanoparticles in photo-Fenton reactioninfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisJahn, Sérgio Luizhttp://lattes.cnpq.br/7735147410610776Foletto, Edson Luizhttp://lattes.cnpq.br/6550340290019699Dotto, Guilherme Luizhttp://lattes.cnpq.br/5412544199323879Salazar, Rodrigo Fernando dos Santoshttp://lattes.cnpq.br/9370462066771109http://lattes.cnpq.br/7458315977853354Drumm, Fernanda Caroline300600000006600bde015d5-5b86-4fa0-a49b-46d96b916908ec0f6c7d-dc44-48cb-b5e5-81ffd574df93f2cd03df-b30b-4de4-9391-a891a78471a3e0844fc7-d3e2-41b0-99b4-4470c9da324c4831ad85-c61b-4bdc-a7fa-70f5c5fc058creponame:Biblioteca Digital de Teses e Dissertações do UFSMinstname:Universidade Federal de Santa Maria (UFSM)instacron:UFSMORIGINALDIS_PPGEQ_2016_DRUMM_FERNANDA.pdfDIS_PPGEQ_2016_DRUMM_FERNANDA.pdfDissertação de Mestradoapplication/pdf1907992http://repositorio.ufsm.br/bitstream/1/17690/1/DIS_PPGEQ_2016_DRUMM_FERNANDA.pdf218b5fa924651b485189d15e3a48769cMD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8805http://repositorio.ufsm.br/bitstream/1/17690/2/license_rdf4460e5956bc1d1639be9ae6146a50347MD52LICENSElicense.txtlicense.txttext/plain; charset=utf-816http://repositorio.ufsm.br/bitstream/1/17690/3/license.txtf8fcb28efb1c8cf0dc096bec902bf4c4MD53TEXTDIS_PPGEQ_2016_DRUMM_FERNANDA.pdf.txtDIS_PPGEQ_2016_DRUMM_FERNANDA.pdf.txtExtracted texttext/plain189758http://repositorio.ufsm.br/bitstream/1/17690/4/DIS_PPGEQ_2016_DRUMM_FERNANDA.pdf.txt5745fe6c82462b9617d250a3b72cfa79MD54THUMBNAILDIS_PPGEQ_2016_DRUMM_FERNANDA.pdf.jpgDIS_PPGEQ_2016_DRUMM_FERNANDA.pdf.jpgIM Thumbnailimage/jpeg4513http://repositorio.ufsm.br/bitstream/1/17690/5/DIS_PPGEQ_2016_DRUMM_FERNANDA.pdf.jpg02e329b353e1a7e1072a50e2fdfabd57MD551/176902022-03-16 10:32:54.107oai:repositorio.ufsm.br:1/17690Q3JlYXRpdmUgQ29tbW9ucw==Biblioteca Digital de Teses e Dissertaçõeshttps://repositorio.ufsm.br/ONGhttps://repositorio.ufsm.br/oai/requestatendimento.sib@ufsm.br||tedebc@gmail.comopendoar:2022-03-16T13:32:54Biblioteca Digital de Teses e Dissertações do UFSM - Universidade Federal de Santa Maria (UFSM)false |
dc.title.por.fl_str_mv |
Catalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-Fenton |
dc.title.alternative.eng.fl_str_mv |
Fe2O3/ZSM-5 hierarchical catalysts: effect of the mesoporosity support in the activity of iron oxide nanoparticles in photo-Fenton reaction |
title |
Catalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-Fenton |
spellingShingle |
Catalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-Fenton Drumm, Fernanda Caroline Catalisadores Zeólita hierárquica Óxido de ferro Foto-Fenton Quitina Catalysts Hierarchical zeolites Iron oxide Photo-Fenton Chitin CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA |
title_short |
Catalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-Fenton |
title_full |
Catalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-Fenton |
title_fullStr |
Catalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-Fenton |
title_full_unstemmed |
Catalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-Fenton |
title_sort |
Catalisadores hierárquicos Fe2O3/ZSM-5: efeito da mesoporosidade do suporte na atividade de nanopartículas de óxido de ferro em reação foto-Fenton |
author |
Drumm, Fernanda Caroline |
author_facet |
Drumm, Fernanda Caroline |
author_role |
author |
dc.contributor.advisor1.fl_str_mv |
Jahn, Sérgio Luiz |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/7735147410610776 |
dc.contributor.advisor-co1.fl_str_mv |
Foletto, Edson Luiz |
dc.contributor.advisor-co1Lattes.fl_str_mv |
http://lattes.cnpq.br/6550340290019699 |
dc.contributor.referee1.fl_str_mv |
Dotto, Guilherme Luiz |
dc.contributor.referee1Lattes.fl_str_mv |
http://lattes.cnpq.br/5412544199323879 |
dc.contributor.referee2.fl_str_mv |
Salazar, Rodrigo Fernando dos Santos |
dc.contributor.referee2Lattes.fl_str_mv |
http://lattes.cnpq.br/9370462066771109 |
dc.contributor.authorLattes.fl_str_mv |
http://lattes.cnpq.br/7458315977853354 |
dc.contributor.author.fl_str_mv |
Drumm, Fernanda Caroline |
contributor_str_mv |
Jahn, Sérgio Luiz Foletto, Edson Luiz Dotto, Guilherme Luiz Salazar, Rodrigo Fernando dos Santos |
dc.subject.por.fl_str_mv |
Catalisadores Zeólita hierárquica Óxido de ferro Foto-Fenton Quitina |
topic |
Catalisadores Zeólita hierárquica Óxido de ferro Foto-Fenton Quitina Catalysts Hierarchical zeolites Iron oxide Photo-Fenton Chitin CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA |
dc.subject.eng.fl_str_mv |
Catalysts Hierarchical zeolites Iron oxide Photo-Fenton Chitin |
dc.subject.cnpq.fl_str_mv |
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA |
description |
This work evaluated the synthesis of hierarchical Fe2O3/ZSM -5 catalysts and their catalytic activity in the degradation of azo dye Yellow Tartrazine in photo-Fenton reaction. The chitin powder was applied as a mesopore template in the gel synthesis of ZSM -5, being removed after its crystallization by heat treatment. Removal of chitin generated voids, resulting in the formation of meso and macropores in the microporous structure of ZSM -5.The deposition of iron oxide nanoparticles on the zeolite was performed using the impregnation technique. Through the XRD analysis, it was observed that zeolites obtained showed typical MFI structure and, as higher the amount of chitin added in preparation of the synthesis gel, the lower the crystallinity of the material. Furthermore, the increase in chitin contents promoted a wide distribution range of meso and macropores in the zeolite, resulting in an increase in average pore size, as well as a larger volume, found, through analysis of N2 adsorption / desorption. Through the micrograph analysis of the obtained catalysts, it can be seen better dispersion of iron oxide on the hierarchical zeolite, which was attributed to higher porosity of the surface, resulting in higher anchor points for the iron oxide be deposited, and also in the formation of smaller sizes of clusters on the support. Unlike what was observed in the hierarchical support, the dispersion of iron oxide was less homogeneous in the microporous zeolite, resulting in a larger size of agglomerates on its surface. These characteristics in the structure of the catalysts had a strong influence on the catalytic activity of dye degradation by photo-Fenton process, where the hierarchical catalysts showed far superior results to catalysts with microporous surface as well as iron oxide unsupported, with the removal 99 %, 33 %, 10 % respectively. This enhancement in the reaction is due to the increased amount of active sites dispersed in the hierarchical catalyst available for decomposition of H2O2 and for formation of hydroxyl radicals, increasing the degradation rate of the dye. The optimum conditions for further removal of Yellow Tartrazine dye, used as a pollutant model in this work were determined by response surface methodology, which were pH 2.7, amount of catalyst of 0.4 g / L and 2 times the stoichiometric amount of H2O2 needed to complete mineralization of the colorant, promoting the removal of 99% of color of solution by 30 minutes of reaction. |
publishDate |
2016 |
dc.date.issued.fl_str_mv |
2016-08-18 |
dc.date.accessioned.fl_str_mv |
2019-08-02T19:55:53Z |
dc.date.available.fl_str_mv |
2019-08-02T19:55:53Z |
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 |
http://repositorio.ufsm.br/handle/1/17690 |
url |
http://repositorio.ufsm.br/handle/1/17690 |
dc.language.iso.fl_str_mv |
por |
language |
por |
dc.relation.cnpq.fl_str_mv |
300600000006 |
dc.relation.confidence.fl_str_mv |
600 |
dc.relation.authority.fl_str_mv |
bde015d5-5b86-4fa0-a49b-46d96b916908 ec0f6c7d-dc44-48cb-b5e5-81ffd574df93 f2cd03df-b30b-4de4-9391-a891a78471a3 e0844fc7-d3e2-41b0-99b4-4470c9da324c 4831ad85-c61b-4bdc-a7fa-70f5c5fc058c |
dc.rights.driver.fl_str_mv |
Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/ info:eu-repo/semantics/openAccess |
rights_invalid_str_mv |
Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/ |
eu_rights_str_mv |
openAccess |
dc.publisher.none.fl_str_mv |
Universidade Federal de Santa Maria Centro de Tecnologia |
dc.publisher.program.fl_str_mv |
Programa de Pós-Graduação em Engenharia Química |
dc.publisher.initials.fl_str_mv |
UFSM |
dc.publisher.country.fl_str_mv |
Brasil |
dc.publisher.department.fl_str_mv |
Engenharia Química |
publisher.none.fl_str_mv |
Universidade Federal de Santa Maria Centro de Tecnologia |
dc.source.none.fl_str_mv |
reponame:Biblioteca Digital de Teses e Dissertações do UFSM instname:Universidade Federal de Santa Maria (UFSM) instacron:UFSM |
instname_str |
Universidade Federal de Santa Maria (UFSM) |
instacron_str |
UFSM |
institution |
UFSM |
reponame_str |
Biblioteca Digital de Teses e Dissertações do UFSM |
collection |
Biblioteca Digital de Teses e Dissertações do UFSM |
bitstream.url.fl_str_mv |
http://repositorio.ufsm.br/bitstream/1/17690/1/DIS_PPGEQ_2016_DRUMM_FERNANDA.pdf http://repositorio.ufsm.br/bitstream/1/17690/2/license_rdf http://repositorio.ufsm.br/bitstream/1/17690/3/license.txt http://repositorio.ufsm.br/bitstream/1/17690/4/DIS_PPGEQ_2016_DRUMM_FERNANDA.pdf.txt http://repositorio.ufsm.br/bitstream/1/17690/5/DIS_PPGEQ_2016_DRUMM_FERNANDA.pdf.jpg |
bitstream.checksum.fl_str_mv |
218b5fa924651b485189d15e3a48769c 4460e5956bc1d1639be9ae6146a50347 f8fcb28efb1c8cf0dc096bec902bf4c4 5745fe6c82462b9617d250a3b72cfa79 02e329b353e1a7e1072a50e2fdfabd57 |
bitstream.checksumAlgorithm.fl_str_mv |
MD5 MD5 MD5 MD5 MD5 |
repository.name.fl_str_mv |
Biblioteca Digital de Teses e Dissertações do UFSM - Universidade Federal de Santa Maria (UFSM) |
repository.mail.fl_str_mv |
atendimento.sib@ufsm.br||tedebc@gmail.com |
_version_ |
1793240142285111296 |