Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.

Detalhes bibliográficos
Autor(a) principal: Gonçalves, Marli Lansoni
Data de Publicação: 2006
Tipo de documento: Dissertação
Idioma: por
Título da fonte: Repositório Institucional da UFSCAR
Texto Completo: https://repositorio.ufscar.br/handle/ufscar/3976
Resumo: In the transformation of bulky molecules, the necessity of catalysts that allow the diffusion to and from the active sites located in the interior of the porous system has become of higher interest. The restriction for the diffusion of this type of molecule in zeolites has led the community to study routes that can make possible to obtain solids that allow the diffusion in mesoporous and simultaneously possess the intrinsic properties of microporous zeolites. In this context, the objective of this work was the synthesis of micro-mesostructured Zeolite ZSM-5/MCM-41 Molecular Sieve type solids. These solids were prepared under hydrothermal conditions in two stages. Initially was prepared a gel of ZSM-5 seeds, which was subsequently crystallized in the presence of cetyltrimetylammonium bromide (CTABr), used as structure directing agent in the synthesis of the MCM-41. The influence of the Si/Al ratio in the seeding gel and the effect of both the time and temperature used in the preparation of such gel and during crystallization were evaluated. X-ray diffraction in the low and wide angle region, nitrogen adsorption/desorption, FTIR spectroscopy and scanning and transmission electron microscopy data evidenced the formation of micro-mesostructured ZSM-5/MCM-41 materials. It is suggested that the formation of the microporous structure occurs by an intraparticle "solid-to-solid" process through the transformation of the walls of the mesoporous into crystalline structure. During the growth of the crystals, the surfactant micelles are dislocated, causing loss of the symmetry of the mesoporous arrangement. However, the micelles remain unchanged in a random array, generating after calcination irregularly arranged mesoporous, but possessing uniform diameters. The cristallinity of the formed ZSM-5 crystals, the volume of the mesoporous and the specific surface area of the final solid were influenced by the Si/Al ratio in the seeding gel and by the time and temperature used in the aging and during the stage of mesostructuration/crystallization. The optimization of this set of variables will allow the control of the ratio between the obtained microporous and mesoporous phases, thus making possible the preparation of tailor-made adsorbents and catalysts for the separation and transformation of bulky molecules.
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spelling Gonçalves, Marli LansoniUrquieta-González, Ernesto Antoniohttp://lattes.cnpq.br/2389975677904655http://buscatextual.cnpq.br/buscatextual/index.jsp2016-06-02T19:56:28Z2007-08-202016-06-02T19:56:28Z2006-08-16GONÇALVES, Marli Lansoni. Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.. 2006. 130 f. Dissertação (Mestrado em Ciências Exatas e da Terra) - Universidade Federal de São Carlos, São Carlos, 2006.https://repositorio.ufscar.br/handle/ufscar/3976In the transformation of bulky molecules, the necessity of catalysts that allow the diffusion to and from the active sites located in the interior of the porous system has become of higher interest. The restriction for the diffusion of this type of molecule in zeolites has led the community to study routes that can make possible to obtain solids that allow the diffusion in mesoporous and simultaneously possess the intrinsic properties of microporous zeolites. In this context, the objective of this work was the synthesis of micro-mesostructured Zeolite ZSM-5/MCM-41 Molecular Sieve type solids. These solids were prepared under hydrothermal conditions in two stages. Initially was prepared a gel of ZSM-5 seeds, which was subsequently crystallized in the presence of cetyltrimetylammonium bromide (CTABr), used as structure directing agent in the synthesis of the MCM-41. The influence of the Si/Al ratio in the seeding gel and the effect of both the time and temperature used in the preparation of such gel and during crystallization were evaluated. X-ray diffraction in the low and wide angle region, nitrogen adsorption/desorption, FTIR spectroscopy and scanning and transmission electron microscopy data evidenced the formation of micro-mesostructured ZSM-5/MCM-41 materials. It is suggested that the formation of the microporous structure occurs by an intraparticle "solid-to-solid" process through the transformation of the walls of the mesoporous into crystalline structure. During the growth of the crystals, the surfactant micelles are dislocated, causing loss of the symmetry of the mesoporous arrangement. However, the micelles remain unchanged in a random array, generating after calcination irregularly arranged mesoporous, but possessing uniform diameters. The cristallinity of the formed ZSM-5 crystals, the volume of the mesoporous and the specific surface area of the final solid were influenced by the Si/Al ratio in the seeding gel and by the time and temperature used in the aging and during the stage of mesostructuration/crystallization. The optimization of this set of variables will allow the control of the ratio between the obtained microporous and mesoporous phases, thus making possible the preparation of tailor-made adsorbents and catalysts for the separation and transformation of bulky molecules.No processamento de moléculas volumosas, é cada vez maior a necessidade de dispor-se de catalisadores que permitam a difusão para os sítios ativos localizados no interior do sistema poroso. A restrição à difusão desse tipo de molécula em zeólitas tem levado a comunidade a estudar rotas que tornem possível a obtenção de um sólido que permita a difusão nos mesoporos e que, ao mesmo tempo, possua as propriedades intrínsecas das zeólitas microporosas. Nesse contexto, este trabalho teve como objetivo a síntese de sólidos micro-mesoestruturados do tipo Zeólita ZSM-5/Peneira Molecular MCM-41. Estes sólidos foram preparados sob condições hidrotérmicas em duas etapas. Inicialmente preparou-se um gel de sementes da zeólita ZSM-5, sendo estas posteriormente cristalizadas na presença de brometo de cetiltrimetilamônio (CTABr), agente mesoestruturante utilizado na síntese da peneira molecular MCM-41. Nessas sínteses, foram avaliadas as influências da relação Si/Al no gel de síntese e o efeito do tempo e da temperatura utilizados na etapa de preparação do gel e na de cristalização. Dados de difração de raios-X em pequenos e altos ângulos, adsorção/dessorção de nitrogênio, espectroscopia no infravermelho e microscopia eletrônica de varredura e de transmissão evidenciaram a formação de materiais micro-mesoestruturados ZSM-5/MCM-41 a partir de géis de sementes , cristalizadas na presença do surfactante catiônico CTA+. Sugere-se que a formação da estrutura microporosa ocorre via um processo sólidosólido intrapartícula, com a transformação das paredes dos mesoporos em estrutura cristalina. Durante o crescimento dos cristais, as micelas do surfactante ocluídas nas partículas são deslocadas, ocasionando perda de simetria do arranjo mesoporoso. Entretanto, as micelas permanecem inalteradas num arranjo aleatório, gerando após a calcinação mesoporos num arranjo irregular, mas possuindo diâmetros uniformes. A cristalinidade da fase ZSM-5 formada, o volume de mesoporos e a área superficial específica do sólido final dependem da relação Si/Al no gel de sementes, do tempo e da temperatura usados durante o envelhecimento e na etapa de mesoestruturação/cristalização. A otimização desse conjunto de varáveis permitirá o controle da proporção entre as fases micro e mesoporosas possibilitando a preparação, sob medida, de novos adsorventes e catalisadores, para a separação e transformação de moléculas volumosas.Universidade Federal de Sao Carlosapplication/pdfporUniversidade Federal de São CarlosPrograma de Pós-Graduação em Engenharia Química - PPGEQUFSCarBRCatáliseCompósitosZeólitaZSM-5Peneira molecularENGENHARIAS::ENGENHARIA QUIMICASólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisinfo:eu-repo/semantics/openAccessreponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINALDissMLG.pdfapplication/pdf4644860https://{{ getenv "DSPACE_HOST" "repositorio.ufscar.br" }}/bitstream/ufscar/3976/1/DissMLG.pdf745bf2fba935eb4bb3fc032321ab36e7MD51THUMBNAILDissMLG.pdf.jpgDissMLG.pdf.jpgIM Thumbnailimage/jpeg8022https://{{ getenv "DSPACE_HOST" "repositorio.ufscar.br" }}/bitstream/ufscar/3976/2/DissMLG.pdf.jpg8443d41dd580a1a82bad09fd3c4671daMD52ufscar/39762019-09-11 02:30:31.458oai:repositorio.ufscar.br:ufscar/3976Repositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestopendoar:43222019-09-11T02:30:31Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false
dc.title.por.fl_str_mv Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.
title Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.
spellingShingle Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.
Gonçalves, Marli Lansoni
Catálise
Compósitos
Zeólita
ZSM-5
Peneira molecular
ENGENHARIAS::ENGENHARIA QUIMICA
title_short Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.
title_full Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.
title_fullStr Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.
title_full_unstemmed Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.
title_sort Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.
author Gonçalves, Marli Lansoni
author_facet Gonçalves, Marli Lansoni
author_role author
dc.contributor.authorlattes.por.fl_str_mv http://buscatextual.cnpq.br/buscatextual/index.jsp
dc.contributor.author.fl_str_mv Gonçalves, Marli Lansoni
dc.contributor.advisor1.fl_str_mv Urquieta-González, Ernesto Antonio
dc.contributor.referee1Lattes.fl_str_mv http://lattes.cnpq.br/2389975677904655
contributor_str_mv Urquieta-González, Ernesto Antonio
dc.subject.por.fl_str_mv Catálise
Compósitos
Zeólita
ZSM-5
Peneira molecular
topic Catálise
Compósitos
Zeólita
ZSM-5
Peneira molecular
ENGENHARIAS::ENGENHARIA QUIMICA
dc.subject.cnpq.fl_str_mv ENGENHARIAS::ENGENHARIA QUIMICA
description In the transformation of bulky molecules, the necessity of catalysts that allow the diffusion to and from the active sites located in the interior of the porous system has become of higher interest. The restriction for the diffusion of this type of molecule in zeolites has led the community to study routes that can make possible to obtain solids that allow the diffusion in mesoporous and simultaneously possess the intrinsic properties of microporous zeolites. In this context, the objective of this work was the synthesis of micro-mesostructured Zeolite ZSM-5/MCM-41 Molecular Sieve type solids. These solids were prepared under hydrothermal conditions in two stages. Initially was prepared a gel of ZSM-5 seeds, which was subsequently crystallized in the presence of cetyltrimetylammonium bromide (CTABr), used as structure directing agent in the synthesis of the MCM-41. The influence of the Si/Al ratio in the seeding gel and the effect of both the time and temperature used in the preparation of such gel and during crystallization were evaluated. X-ray diffraction in the low and wide angle region, nitrogen adsorption/desorption, FTIR spectroscopy and scanning and transmission electron microscopy data evidenced the formation of micro-mesostructured ZSM-5/MCM-41 materials. It is suggested that the formation of the microporous structure occurs by an intraparticle "solid-to-solid" process through the transformation of the walls of the mesoporous into crystalline structure. During the growth of the crystals, the surfactant micelles are dislocated, causing loss of the symmetry of the mesoporous arrangement. However, the micelles remain unchanged in a random array, generating after calcination irregularly arranged mesoporous, but possessing uniform diameters. The cristallinity of the formed ZSM-5 crystals, the volume of the mesoporous and the specific surface area of the final solid were influenced by the Si/Al ratio in the seeding gel and by the time and temperature used in the aging and during the stage of mesostructuration/crystallization. The optimization of this set of variables will allow the control of the ratio between the obtained microporous and mesoporous phases, thus making possible the preparation of tailor-made adsorbents and catalysts for the separation and transformation of bulky molecules.
publishDate 2006
dc.date.issued.fl_str_mv 2006-08-16
dc.date.available.fl_str_mv 2007-08-20
2016-06-02T19:56:28Z
dc.date.accessioned.fl_str_mv 2016-06-02T19:56:28Z
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dc.type.driver.fl_str_mv info:eu-repo/semantics/masterThesis
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dc.identifier.citation.fl_str_mv GONÇALVES, Marli Lansoni. Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.. 2006. 130 f. Dissertação (Mestrado em Ciências Exatas e da Terra) - Universidade Federal de São Carlos, São Carlos, 2006.
dc.identifier.uri.fl_str_mv https://repositorio.ufscar.br/handle/ufscar/3976
identifier_str_mv GONÇALVES, Marli Lansoni. Sólidos micro-mesoestruturados tipo zeólita ZSM-5/peneira molecular MCM-41 - síntese e estudo de propriedades.. 2006. 130 f. Dissertação (Mestrado em Ciências Exatas e da Terra) - Universidade Federal de São Carlos, São Carlos, 2006.
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