Cinética da produção de butenos a partir de butanol empregando catalisadores ácidos
Autor(a) principal: | |
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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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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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1815172287558582272 |