Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas
Autor(a) principal: | |
---|---|
Data de Publicação: | 2019 |
Tipo de documento: | Tese |
Idioma: | por |
Título da fonte: | Repositório Institucional da Universidade Federal de Alagoas (UFAL) |
Texto Completo: | http://www.repositorio.ufal.br/handle/riufal/5551 |
Resumo: | In this study, it was evaluated the crystallization of ZSM-5 with high Si/Al ratio (100 and 150) through combined use of crystallization seeds and addition of organic compounds which are not conventional templates of ZSM-5 (ethanol, methylamine, ethylamine, propylamine, butylamine, isopropylamine and diethylamine), intending to establish a route of synthesis with less environmental impact and low cost. In the first stage, it was verified the effect of ethanol and amines added to the synthesis gel, as well as the time of hydrothermal and ratios codirecting/silica and OH/silica in static crystallization conditions. In the second stage, it was analyzed the influence of agitation during the crystallization upon the ZSM-5’s proprieties obtained in optimized conditions on static experiments from the past stage. The zeolites formed were analyzed by X-ray diffractometry to comprehend the effects of template types and further studied parameters about this material’s formation, whilst for the most crystalline samples were realized additional characterizations for: desorption at the programmed temperature, nitrogen adsorption, scanning electronic microscopy, dispersive X-Ray energy spectroscopy and thermogravimetric analysis. Through these data, it was observed that the crystallinity decreased, due to the formation of the magadiite phase with increasement of the synthesis time. It was verified that the magadiite phase is thermally instable, disappearing after the stage of calcination at 550 °C. On synthesis under agitation, it was observed ZSM-5/magadiite/cristobalita composites. The cristobalite phase occurred due to prolonged times of hydrothermal treatment and the system agitation, making necessaire to adjust the synthesis parameters to establish a methodology able to produce the ZSM-5 with high crystallinity. This procedure was successfully obtained to the synthesis of ZSM-5, using propylamine as template agent of alternative structure, under static conditions. The material formed through this method showed a superior crystallinity rate over the standard commercial sample and average crystal size between 23 and 24 nm. Its superficial specific area was superior to 300 m2.g-1, and the microporous volume reached 0,09 cm3.g-1. The biggest accessibility to the catalyzer porous with propylamine led to superior catalytic results over further evaluated material, with low ratio of coke formation, showing high stability on n-hexane cracking. |
id |
UFAL_716d8455f4fa3c84d09694aa74f6b628 |
---|---|
oai_identifier_str |
oai:www.repositorio.ufal.br:riufal/5551 |
network_acronym_str |
UFAL |
network_name_str |
Repositório Institucional da Universidade Federal de Alagoas (UFAL) |
repository_id_str |
|
spelling |
Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminasZSM-5 (Zeolitas)SílicaAminasEtanolMicroscopia eletrônica de varreduraCristalizaçãoZeólitos sintéticosZSM-5 (Zeolites)AminesEthanolScanning electron microscopyCrystallizationSynthetic ZeolitesCNPQ::ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICAIn this study, it was evaluated the crystallization of ZSM-5 with high Si/Al ratio (100 and 150) through combined use of crystallization seeds and addition of organic compounds which are not conventional templates of ZSM-5 (ethanol, methylamine, ethylamine, propylamine, butylamine, isopropylamine and diethylamine), intending to establish a route of synthesis with less environmental impact and low cost. In the first stage, it was verified the effect of ethanol and amines added to the synthesis gel, as well as the time of hydrothermal and ratios codirecting/silica and OH/silica in static crystallization conditions. In the second stage, it was analyzed the influence of agitation during the crystallization upon the ZSM-5’s proprieties obtained in optimized conditions on static experiments from the past stage. The zeolites formed were analyzed by X-ray diffractometry to comprehend the effects of template types and further studied parameters about this material’s formation, whilst for the most crystalline samples were realized additional characterizations for: desorption at the programmed temperature, nitrogen adsorption, scanning electronic microscopy, dispersive X-Ray energy spectroscopy and thermogravimetric analysis. Through these data, it was observed that the crystallinity decreased, due to the formation of the magadiite phase with increasement of the synthesis time. It was verified that the magadiite phase is thermally instable, disappearing after the stage of calcination at 550 °C. On synthesis under agitation, it was observed ZSM-5/magadiite/cristobalita composites. The cristobalite phase occurred due to prolonged times of hydrothermal treatment and the system agitation, making necessaire to adjust the synthesis parameters to establish a methodology able to produce the ZSM-5 with high crystallinity. This procedure was successfully obtained to the synthesis of ZSM-5, using propylamine as template agent of alternative structure, under static conditions. The material formed through this method showed a superior crystallinity rate over the standard commercial sample and average crystal size between 23 and 24 nm. Its superficial specific area was superior to 300 m2.g-1, and the microporous volume reached 0,09 cm3.g-1. The biggest accessibility to the catalyzer porous with propylamine led to superior catalytic results over further evaluated material, with low ratio of coke formation, showing high stability on n-hexane cracking.CAPES - Coordenação de Aperfeiçoamento de Pessoal de Nível SuperiorNeste estudo, foi avaliada a cristalização da ZSM-5 com razão Si/Al elevada (100 e 150) através do uso combinado de sementes de cristalização e adição de compostos orgânicos que não são direcionadores convencionais da ZSM-5 (etanol, metilamina, etilamina, propilamina, butilamina, isopropilamina e dietilamina), com intuito de estabelecer uma rota de síntese de menor impacto ambiental e baixo custo. Na etapa inicial, verificou-se o efeito do etanol e aminas adicionados ao gel de síntese, assim como, tempo de tratamento hidrotérmico e razões codirecionador/sílica e OH/sílica em condições de cristalização estáticas. Na segunda etapa, foi analisada a influência da agitação durante a cristalização sobre as propriedades da ZSM-5 obtida em condições otimizadas nos experimentos estáticos da etapa anterior. As zeólitas formadas foram analisadas por difratometria de raios X para compreender os efeitos dos tipos de direcionadores e demais parâmetros estudados sobre a formação desse material. Enquanto que, para as amostras mais cristalinas foram realizadas caracterizações adicionais por: dessorção de amônia à temperatura programada, adsorção de nitrogênio, microscopia eletrônica de varredura, espectroscopia de energia dispersiva de raios X e análises termogravimétricas. A partir desses dados, foi observado um decréscimo na cristalinidade devido a formação da fase contaminante magadiita com o aumento do tempo de síntese. Verificou que a fase magadiita é termicamente instável, desaparecendo após a etapa de calcinação a 550 ºC. Nas sínteses sob agitação, foram verificados compósitos de ZSM-5/magadiita/cristobalita, a fase cristobalita surgiu devido a tempos prolongados de tratamento hidrotérmico em conjunto com a agitação do sistema, sendo necessário, assim, ajustar os parâmetros de síntese para se estabelecer uma metodologia capaz de produzir a ZSM-5 com alta cristalinidade. Esse procedimento foi obtido com sucesso para a síntese da ZSM-5, utilizando propilamina como agente direcionador de estrutura alternativo, sob condições estáticas. O material formado por esse método exibiu um grau de cristalinidade superiore a amostra comercial padrão e tamanho médio de cristalito entre 23 e 24 nm. Sua área superficial específica foi superior a 300 m2.g-1 e o volume de microporos alcançou 0,09 cm3.g-1. A maior acessibilidade aos poros do catalisador com propilamina levaram a resultados catalíticos superiores em relação aos demais materiais avaliados, com baixa formação de coque, possuindo alta estabilidade no craqueamento do n-hexano.Universidade Federal de AlagoasBrasilPrograma de Pós-Graduação em MateriaisUFALSilva, Antonio Osimar Sousa dahttp://lattes.cnpq.br/5289388662589522Galdino, Fabiane Caxico de Abreuhttp://lattes.cnpq.br/4203326795155880Meili, Lucashttp://lattes.cnpq.br/3802018064427795Santos, Jailma Barros doshttp://lattes.cnpq.br/4737558086696037Souza, Felipe Thiago Caldeira dehttp://lattes.cnpq.br/1107181432483018Mendonça, Thayane Regine Dantas de2019-07-25T15:08:46Z2019-07-022019-07-25T15:08:46Z2019-01-29info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisapplication/pdfMENDONÇA, Thayane Regine Dantas de. Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas. 2019. 93 f. Tese (Doutorado em Materiais) – Centro de Tecnologia, Programa de Pós-Graduação em Materiais, Universidade Federal de Alagoas, Maceió, 2019.http://www.repositorio.ufal.br/handle/riufal/5551porinfo:eu-repo/semantics/openAccessreponame:Repositório Institucional da Universidade Federal de Alagoas (UFAL)instname:Universidade Federal de Alagoas (UFAL)instacron:UFAL2019-07-25T15:08:46Zoai:www.repositorio.ufal.br:riufal/5551Repositório InstitucionalPUBhttp://www.repositorio.ufal.br/oai/requestri@sibi.ufal.bropendoar:2019-07-25T15:08:46Repositório Institucional da Universidade Federal de Alagoas (UFAL) - Universidade Federal de Alagoas (UFAL)false |
dc.title.none.fl_str_mv |
Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas |
title |
Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas |
spellingShingle |
Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas Mendonça, Thayane Regine Dantas de ZSM-5 (Zeolitas) Sílica Aminas Etanol Microscopia eletrônica de varredura Cristalização Zeólitos sintéticos ZSM-5 (Zeolites) Amines Ethanol Scanning electron microscopy Crystallization Synthetic Zeolites CNPQ::ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA |
title_short |
Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas |
title_full |
Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas |
title_fullStr |
Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas |
title_full_unstemmed |
Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas |
title_sort |
Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas |
author |
Mendonça, Thayane Regine Dantas de |
author_facet |
Mendonça, Thayane Regine Dantas de |
author_role |
author |
dc.contributor.none.fl_str_mv |
Silva, Antonio Osimar Sousa da http://lattes.cnpq.br/5289388662589522 Galdino, Fabiane Caxico de Abreu http://lattes.cnpq.br/4203326795155880 Meili, Lucas http://lattes.cnpq.br/3802018064427795 Santos, Jailma Barros dos http://lattes.cnpq.br/4737558086696037 Souza, Felipe Thiago Caldeira de http://lattes.cnpq.br/1107181432483018 |
dc.contributor.author.fl_str_mv |
Mendonça, Thayane Regine Dantas de |
dc.subject.por.fl_str_mv |
ZSM-5 (Zeolitas) Sílica Aminas Etanol Microscopia eletrônica de varredura Cristalização Zeólitos sintéticos ZSM-5 (Zeolites) Amines Ethanol Scanning electron microscopy Crystallization Synthetic Zeolites CNPQ::ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA |
topic |
ZSM-5 (Zeolitas) Sílica Aminas Etanol Microscopia eletrônica de varredura Cristalização Zeólitos sintéticos ZSM-5 (Zeolites) Amines Ethanol Scanning electron microscopy Crystallization Synthetic Zeolites CNPQ::ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA |
description |
In this study, it was evaluated the crystallization of ZSM-5 with high Si/Al ratio (100 and 150) through combined use of crystallization seeds and addition of organic compounds which are not conventional templates of ZSM-5 (ethanol, methylamine, ethylamine, propylamine, butylamine, isopropylamine and diethylamine), intending to establish a route of synthesis with less environmental impact and low cost. In the first stage, it was verified the effect of ethanol and amines added to the synthesis gel, as well as the time of hydrothermal and ratios codirecting/silica and OH/silica in static crystallization conditions. In the second stage, it was analyzed the influence of agitation during the crystallization upon the ZSM-5’s proprieties obtained in optimized conditions on static experiments from the past stage. The zeolites formed were analyzed by X-ray diffractometry to comprehend the effects of template types and further studied parameters about this material’s formation, whilst for the most crystalline samples were realized additional characterizations for: desorption at the programmed temperature, nitrogen adsorption, scanning electronic microscopy, dispersive X-Ray energy spectroscopy and thermogravimetric analysis. Through these data, it was observed that the crystallinity decreased, due to the formation of the magadiite phase with increasement of the synthesis time. It was verified that the magadiite phase is thermally instable, disappearing after the stage of calcination at 550 °C. On synthesis under agitation, it was observed ZSM-5/magadiite/cristobalita composites. The cristobalite phase occurred due to prolonged times of hydrothermal treatment and the system agitation, making necessaire to adjust the synthesis parameters to establish a methodology able to produce the ZSM-5 with high crystallinity. This procedure was successfully obtained to the synthesis of ZSM-5, using propylamine as template agent of alternative structure, under static conditions. The material formed through this method showed a superior crystallinity rate over the standard commercial sample and average crystal size between 23 and 24 nm. Its superficial specific area was superior to 300 m2.g-1, and the microporous volume reached 0,09 cm3.g-1. The biggest accessibility to the catalyzer porous with propylamine led to superior catalytic results over further evaluated material, with low ratio of coke formation, showing high stability on n-hexane cracking. |
publishDate |
2019 |
dc.date.none.fl_str_mv |
2019-07-25T15:08:46Z 2019-07-02 2019-07-25T15:08:46Z 2019-01-29 |
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.uri.fl_str_mv |
MENDONÇA, Thayane Regine Dantas de. Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas. 2019. 93 f. Tese (Doutorado em Materiais) – Centro de Tecnologia, Programa de Pós-Graduação em Materiais, Universidade Federal de Alagoas, Maceió, 2019. http://www.repositorio.ufal.br/handle/riufal/5551 |
identifier_str_mv |
MENDONÇA, Thayane Regine Dantas de. Síntese da ZSM-5 de alto teor de sílica com sementes na presença de etanol e aminas. 2019. 93 f. Tese (Doutorado em Materiais) – Centro de Tecnologia, Programa de Pós-Graduação em Materiais, Universidade Federal de Alagoas, Maceió, 2019. |
url |
http://www.repositorio.ufal.br/handle/riufal/5551 |
dc.language.iso.fl_str_mv |
por |
language |
por |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
application/pdf |
dc.publisher.none.fl_str_mv |
Universidade Federal de Alagoas Brasil Programa de Pós-Graduação em Materiais UFAL |
publisher.none.fl_str_mv |
Universidade Federal de Alagoas Brasil Programa de Pós-Graduação em Materiais UFAL |
dc.source.none.fl_str_mv |
reponame:Repositório Institucional da Universidade Federal de Alagoas (UFAL) instname:Universidade Federal de Alagoas (UFAL) instacron:UFAL |
instname_str |
Universidade Federal de Alagoas (UFAL) |
instacron_str |
UFAL |
institution |
UFAL |
reponame_str |
Repositório Institucional da Universidade Federal de Alagoas (UFAL) |
collection |
Repositório Institucional da Universidade Federal de Alagoas (UFAL) |
repository.name.fl_str_mv |
Repositório Institucional da Universidade Federal de Alagoas (UFAL) - Universidade Federal de Alagoas (UFAL) |
repository.mail.fl_str_mv |
ri@sibi.ufal.br |
_version_ |
1748233747233243136 |