Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos

Detalhes bibliográficos
Autor(a) principal: Scheidt, Tiago Bordignon
Data de Publicação: 2017
Tipo de documento: Dissertação
Idioma: por
Título da fonte: Manancial - Repositório Digital da UFSM
dARK ID: ark:/26339/0013000005fr4
Texto Completo: http://repositorio.ufsm.br/handle/1/14580
Resumo: to environmental requirements, new producing routes have been pursued and the butanol dehydration reaction is one of the most promising. HZSM-5 zeolites and -alumina acid catalysts were synthesized at different conditions to investigate the effects of their acid properties on catalyst activity in this reaction. The catalytic tests were carried out following a complete factorial design. The results evinced that there is a great influence of feeding rate on butanol conversion, exhibiting a characteristic profile of chemical reaction with order lower than 1. The conversion obtained with the zeolites were always higher than the ones obtained with the aluminas at all reaction temperatures, even though less catalyst mass was employed, which indicates a higher activity of this catalyst. Selectivity to 2-butene was higher than the primary olefin selectivity for the HZSM-5; while, the aluminas almost did not isomerized 1- butene, with selectivity of approximately 98% in all tests. The SAR of the HZSM-5 presents impact on the activity of this material, the lower the SAR is, more active is the catalyst. The zeolites with SAR 30 and 40 presented high conversions of butanol and concentrations of isomerization product than SAR 50. For the aluminas, the highest catalytic activity was observed for the sample calcined at 600 °C. After calculating the molar fraction of the products at the reactor outlet, parameter estimation of the proposed kinetic models was performed. The results from the models confirmed the higher activity of the HZSM-5 and also validated the effect of the zeolite SAR and the calcination temperature of the aluminas on the reaction selectivity. Heterogeneous models fitted better the experimental data than pseudohomogeneous models. Comparing different kinetic models, it was observed that the butanol adsorption is the only significant hypothesis in model fitting to the experimental data. The adsorption of other molecules, such as 2-butene, isobutene and water, could be disconsidered in the best model formulation.
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spelling Cinética da produção de butenos a partir de butanol empregando catalisadores ácidosKinetics of butene production from butanol using acid catalystsDesidrataçãoButanolButenosHZSM-5AluminaModelagem cinéticaDehydrationButanolButenesHZSM-5AluminaKinetic modelingCNPQ::ENGENHARIAS::ENGENHARIA QUIMICAto environmental requirements, new producing routes have been pursued and the butanol dehydration reaction is one of the most promising. HZSM-5 zeolites and -alumina acid catalysts were synthesized at different conditions to investigate the effects of their acid properties on catalyst activity in this reaction. The catalytic tests were carried out following a complete factorial design. The results evinced that there is a great influence of feeding rate on butanol conversion, exhibiting a characteristic profile of chemical reaction with order lower than 1. The conversion obtained with the zeolites were always higher than the ones obtained with the aluminas at all reaction temperatures, even though less catalyst mass was employed, which indicates a higher activity of this catalyst. Selectivity to 2-butene was higher than the primary olefin selectivity for the HZSM-5; while, the aluminas almost did not isomerized 1- butene, with selectivity of approximately 98% in all tests. The SAR of the HZSM-5 presents impact on the activity of this material, the lower the SAR is, more active is the catalyst. The zeolites with SAR 30 and 40 presented high conversions of butanol and concentrations of isomerization product than SAR 50. For the aluminas, the highest catalytic activity was observed for the sample calcined at 600 °C. After calculating the molar fraction of the products at the reactor outlet, parameter estimation of the proposed kinetic models was performed. The results from the models confirmed the higher activity of the HZSM-5 and also validated the effect of the zeolite SAR and the calcination temperature of the aluminas on the reaction selectivity. Heterogeneous models fitted better the experimental data than pseudohomogeneous models. Comparing different kinetic models, it was observed that the butanol adsorption is the only significant hypothesis in model fitting to the experimental data. The adsorption of other molecules, such as 2-butene, isobutene and water, could be disconsidered in the best model formulation.Butenos são olefinas produzidas a partir de derivados do petróleo para diversos fins industriais. Devido às exigências ambientais, novas rotas de produção estão sendo buscadas, e a reação de desidratação do butanol é uma das mais promissoras. Catalisadores ácidos do tipo zeólita HZSM-5 e -alumina foram sintetizados sob diferentes condições, para investigação do efeito das suas propriedades ácidas na atividade dos catalisadores nesta reação. Os testes catalíticos foram realizados seguindo um planejamento experimental fatorial completo. Os resultados indicaram que há uma grande influência da vazão de alimentação na conversão do butanol, exibindo um perfil característico de reações químicas com ordem menor do que 1. As conversões obtidas com as zeólitas foram sempre superiores às obtidas para as aluminas em todas temperaturas de reação, mesmo com menor massa de catalisador empregada, o que indica maior atividade desse catalisador. A seletividade a 2-buteno foi superior à seletividade a olefina primária, 1-buteno, para as HZSM-5; enquanto, as aluminas quase não isomerizaram o 1-buteno, com seletividades de cerca de 98% em todos os testes. A SAR das HZSM-5 apresenta impacto na atividade deste material, sendo que quanto menor a SAR, mais ativo é o catalisador. As zeólitas com SAR 30 e 40 apresentaram maiores conversões de butanol e concentrações de produtos de isomerização do que a SAR 50. Para as aluminas, a maior atividade catalítica foi observada para a amostra calcinada a 600 °C. Após o cálculo das frações molares dos produtos na saída do reator, foi realizada a estimação de parâmetros dos modelos cinéticos propostos. Os resultados obtidos pelos modelos confirmaram a maior atividade das HZSM-5, além de validarem o efeito da SAR das zeólitas e da temperatura de calcinação das aluminas sobre a seletividade da reação. Os modelos heterogêneos ajustaram melhor os dados experimentais que os modelos pseudo-homogêneos. Comparando os diferentes modelos cinéticos, observou-se que a adsorção do butanol é a única hipótese significativa no ajuste dos modelos aos dados experimentais. A adsorção das demais moléculas, como 2-buteno, isobuteno e água, puderam ser desconsideradas na formulação do melhor modelo.Universidade Federal de Santa MariaBrasilEngenharia QuímicaUFSMPrograma de Pós-Graduação em Engenharia QuímicaCentro de TecnologiaSalau, Nina Paula Gonçalveshttp://lattes.cnpq.br/4234840503539989Coutinho, Elisa Barbosahttp://lattes.cnpq.br/0551304679934048Schwaab, Marciohttp://lattes.cnpq.br/7572439258027513Varela, Maria do Carmo Rangel Santoshttp://lattes.cnpq.br/0023950321397451Scheidt, Tiago Bordignon2018-10-17T17:40:46Z2018-10-17T17:40:46Z2017-12-01info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisapplication/pdfhttp://repositorio.ufsm.br/handle/1/14580ark:/26339/0013000005fr4porAttribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessreponame:Manancial - Repositório Digital da UFSMinstname:Universidade Federal de Santa Maria (UFSM)instacron:UFSM2018-10-17T17:40:46Zoai:repositorio.ufsm.br:1/14580Biblioteca Digital de Teses e Dissertaçõeshttps://repositorio.ufsm.br/ONGhttps://repositorio.ufsm.br/oai/requestatendimento.sib@ufsm.br||tedebc@gmail.comopendoar:2018-10-17T17:40:46Manancial - Repositório Digital da UFSM - Universidade Federal de Santa Maria (UFSM)false
dc.title.none.fl_str_mv Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos
Kinetics of butene production from butanol using acid catalysts
title Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos
spellingShingle Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos
Scheidt, Tiago Bordignon
Desidratação
Butanol
Butenos
HZSM-5
Alumina
Modelagem cinética
Dehydration
Butanol
Butenes
HZSM-5
Alumina
Kinetic modeling
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
title_short Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos
title_full Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos
title_fullStr Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos
title_full_unstemmed Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos
title_sort Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos
author Scheidt, Tiago Bordignon
author_facet Scheidt, Tiago Bordignon
author_role author
dc.contributor.none.fl_str_mv Salau, Nina Paula Gonçalves
http://lattes.cnpq.br/4234840503539989
Coutinho, Elisa Barbosa
http://lattes.cnpq.br/0551304679934048
Schwaab, Marcio
http://lattes.cnpq.br/7572439258027513
Varela, Maria do Carmo Rangel Santos
http://lattes.cnpq.br/0023950321397451
dc.contributor.author.fl_str_mv Scheidt, Tiago Bordignon
dc.subject.por.fl_str_mv Desidratação
Butanol
Butenos
HZSM-5
Alumina
Modelagem cinética
Dehydration
Butanol
Butenes
HZSM-5
Alumina
Kinetic modeling
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
topic Desidratação
Butanol
Butenos
HZSM-5
Alumina
Modelagem cinética
Dehydration
Butanol
Butenes
HZSM-5
Alumina
Kinetic modeling
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
description to environmental requirements, new producing routes have been pursued and the butanol dehydration reaction is one of the most promising. HZSM-5 zeolites and -alumina acid catalysts were synthesized at different conditions to investigate the effects of their acid properties on catalyst activity in this reaction. The catalytic tests were carried out following a complete factorial design. The results evinced that there is a great influence of feeding rate on butanol conversion, exhibiting a characteristic profile of chemical reaction with order lower than 1. The conversion obtained with the zeolites were always higher than the ones obtained with the aluminas at all reaction temperatures, even though less catalyst mass was employed, which indicates a higher activity of this catalyst. Selectivity to 2-butene was higher than the primary olefin selectivity for the HZSM-5; while, the aluminas almost did not isomerized 1- butene, with selectivity of approximately 98% in all tests. The SAR of the HZSM-5 presents impact on the activity of this material, the lower the SAR is, more active is the catalyst. The zeolites with SAR 30 and 40 presented high conversions of butanol and concentrations of isomerization product than SAR 50. For the aluminas, the highest catalytic activity was observed for the sample calcined at 600 °C. After calculating the molar fraction of the products at the reactor outlet, parameter estimation of the proposed kinetic models was performed. The results from the models confirmed the higher activity of the HZSM-5 and also validated the effect of the zeolite SAR and the calcination temperature of the aluminas on the reaction selectivity. Heterogeneous models fitted better the experimental data than pseudohomogeneous models. Comparing different kinetic models, it was observed that the butanol adsorption is the only significant hypothesis in model fitting to the experimental data. The adsorption of other molecules, such as 2-butene, isobutene and water, could be disconsidered in the best model formulation.
publishDate 2017
dc.date.none.fl_str_mv 2017-12-01
2018-10-17T17:40:46Z
2018-10-17T17:40:46Z
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/1/14580
dc.identifier.dark.fl_str_mv ark:/26339/0013000005fr4
url http://repositorio.ufsm.br/handle/1/14580
identifier_str_mv ark:/26339/0013000005fr4
dc.language.iso.fl_str_mv por
language por
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.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Universidade Federal de Santa Maria
Brasil
Engenharia Química
UFSM
Programa de Pós-Graduação em Engenharia Química
Centro de Tecnologia
publisher.none.fl_str_mv Universidade Federal de Santa Maria
Brasil
Engenharia Química
UFSM
Programa de Pós-Graduação em Engenharia Química
Centro de Tecnologia
dc.source.none.fl_str_mv reponame:Manancial - Repositório Digital da 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 Manancial - Repositório Digital da UFSM
collection Manancial - Repositório Digital da UFSM
repository.name.fl_str_mv Manancial - Repositório Digital da UFSM - Universidade Federal de Santa Maria (UFSM)
repository.mail.fl_str_mv atendimento.sib@ufsm.br||tedebc@gmail.com
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