Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno

Detalhes bibliográficos
Autor(a) principal: Soares, João Carlos Serpa
Data de Publicação: 2014
Tipo de documento: Dissertação
Idioma: por
Título da fonte: Biblioteca Digital de Teses e Dissertações da UERJ
Texto Completo: http://www.bdtd.uerj.br/handle/1/12052
Resumo: Benzene has been associated with an increase in diseases such as leukemia and it can also cause irreversible chromosomal modifications and damage to life. The cyclohexene is an intermediate for nylon and other fine chemical products and it can be generated through partial benzene hydrogenation, which is an alternative application for this toxic compound. However, from the thermodynamic point of view, the total benzene hydrogenation to cyclohexane is much more favorable than its partial hydrogenation to cyclohexene. Based in this context, this work aims at the preparation, characterization and evaluation of Ru/xZnO-Al2O3 catalysts in the partial benzene hydrogenation reaction using a batch reactor. The ZnAl mixed oxides were synthesized by co-precipitation of their respective salts. The catalysts were prepared by dry impregnation of RuCl3.6H2O and the samples received the following nomenclatures: RuAl, Ru5ZnAl, Ru10ZnAl, Ru20ZnAl, Ru50ZnAl, Ru90ZnAl and RuZn. Textural analysis, X-ray fluorescence, X-ray diffraction, X-ray phoelectron, temperature programmed reduction and H2 chemisorption techniques were used to characterize the catalysts. Partial benzene hydrogenation was carried out in a PARR reactor Instruments. The order of activity for the reaction with pure benzene was as follows: Ru10ZnAl >>> Ru5ZnAl > Ru20ZnAl > RuAl >> Ru90ZnAl = Ru50ZnAl = RuZn. Over the studied catalysts, Ru10ZnAl presented lower particle size (8 nm) and higher surface area (297 m².g-1) and these factors most likely have favoured ruthenium high dispersion on the catalyst surface. In addition, through the TPR analysis, there was a partial ZnO reduction on this catalyst. Tests conducted with addition of solvents using Ru10ZnAl catalyst showed lower activities than the ones containing only benzene
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spelling Zotin, Fatima Maria Zanon://lattes.cnpq.br/2398224913573093Araujo, Lucia Regina Raddi dehttp://lattes.cnpq.br/1592062469734844Gaspar, Alexandre Barroshttp://lattes.cnpq.br/1049735133222758Silva, Mônica Antunes Pereira dahttp://lattes.cnpq.br/3911383035330556Zonetti, Priscila da Costahttp://lattes.cnpq.br/7522580132803695Santos, Luz Amparo Palaciohttp://lattes.cnpq.br/2277031732030434http://lattes.cnpq.br/3708838349183919Soares, João Carlos Serpa2021-01-06T19:37:53Z2018-05-082014-10-24SOARES, João Carlos Serpa. Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno. 2014. 98 f. Dissertação (Mestrado em Processos Químicos e Meio Ambiente) - Universidade do Estado do Rio de Janeiro, Rio de Janeiro, 2014.http://www.bdtd.uerj.br/handle/1/12052Benzene has been associated with an increase in diseases such as leukemia and it can also cause irreversible chromosomal modifications and damage to life. The cyclohexene is an intermediate for nylon and other fine chemical products and it can be generated through partial benzene hydrogenation, which is an alternative application for this toxic compound. However, from the thermodynamic point of view, the total benzene hydrogenation to cyclohexane is much more favorable than its partial hydrogenation to cyclohexene. Based in this context, this work aims at the preparation, characterization and evaluation of Ru/xZnO-Al2O3 catalysts in the partial benzene hydrogenation reaction using a batch reactor. The ZnAl mixed oxides were synthesized by co-precipitation of their respective salts. The catalysts were prepared by dry impregnation of RuCl3.6H2O and the samples received the following nomenclatures: RuAl, Ru5ZnAl, Ru10ZnAl, Ru20ZnAl, Ru50ZnAl, Ru90ZnAl and RuZn. Textural analysis, X-ray fluorescence, X-ray diffraction, X-ray phoelectron, temperature programmed reduction and H2 chemisorption techniques were used to characterize the catalysts. Partial benzene hydrogenation was carried out in a PARR reactor Instruments. The order of activity for the reaction with pure benzene was as follows: Ru10ZnAl >>> Ru5ZnAl > Ru20ZnAl > RuAl >> Ru90ZnAl = Ru50ZnAl = RuZn. Over the studied catalysts, Ru10ZnAl presented lower particle size (8 nm) and higher surface area (297 m².g-1) and these factors most likely have favoured ruthenium high dispersion on the catalyst surface. In addition, through the TPR analysis, there was a partial ZnO reduction on this catalyst. Tests conducted with addition of solvents using Ru10ZnAl catalyst showed lower activities than the ones containing only benzeneO benzeno tem sido associado ao aumento de doenças como leucemia, podendo provocar também alterações cromossômicas e danos irreversíveis à vida. O cicloexeno é um intermediário na obtenção de nylon e outros produtos da química fina e sua obtenção via hidrogenação parcial de benzeno constitui uma aplicação alternativa para este composto tóxico. No entanto, do ponto de vista termodinâmico, a hidrogenação total do benzeno a cicloexano é muito mais favorável do que a hidrogenação parcial deste a cicloexeno. Inserido neste contexto, este trabalho tem como objetivo a preparação, caracterização e avaliação de catalisadores Ru/xZnO-Al2O3 na reação de hidrogenação parcial de benzeno em reator batelada.Os óxidos mistos de ZnAl foram sintetizados por co-precipitação dos seus respectivos sais. Os catalisadores foram preparados por impregnação ao ponto úmido a partir do sal RuCl3.6H2O e receberam a seguinte nomenclatura: RuAl, Ru5ZnAl, Ru10ZnAl, Ru20ZnAl, Ru50ZnAl, Ru90ZnAl e RuZn. Para a caracterização dos catalisadores foram utilizadas técnicas de análise textural, fluorescência de raios X, difração de raios X, espectroscopia fotoeletrônica de raios X, redução à temperatura programada e quimissorção de H2. A hidrogenação parcial de benzeno foi realizada num reator PARR Instruments. A ordem de atividade para a reação com benzeno puro foi: Ru10ZnAl >>> Ru5ZnAl > Ru20ZnAl > RuAl >> Ru90ZnAl = Ru50ZnAl = RuZn. Dos catalisadores estudados, o Ru10ZnAl, apresentou menor tamanho de partícula (8 nm) e maior área específica (297 m².g-1) , fatores estes que provavelmente favoreceram a maior dispersão do rutênio sobre a superfície do catalisador. Além disso, observou-se redução parcial do suporte ZnO neste catalisador, verificado pela análise de DRX. Os testes realizados com o catalisador Ru10ZnAl com adição de solventes (água e cicloexano) apresentaram atividade inferior a do sistema contendo apenas benzenoSubmitted by Boris Flegr (boris@uerj.br) on 2021-01-06T19:37:53Z No. of bitstreams: 1 Joao Carlos Serpa Soares.pdf: 1724387 bytes, checksum: 0b59557913e4ca10c8683f1053928985 (MD5)Made available in DSpace on 2021-01-06T19:37:53Z (GMT). No. of bitstreams: 1 Joao Carlos Serpa Soares.pdf: 1724387 bytes, checksum: 0b59557913e4ca10c8683f1053928985 (MD5) Previous issue date: 2014-10-24application/pdfporUniversidade do Estado do Rio de JaneiroPrograma de Pós-Graduação em Engenharia QuímicaUERJBRCentro de Tecnologia e Ciências::Instituto de QuímicaRutheniumhydrogenationcyclohexenezincRutêniohidrogenaçãocicloexenozincoCNPQ::ENGENHARIAS::ENGENHARIA QUIMICACatalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzenoCatalysts Ru / xZnO-Al2O3 in the partial hydrogenation of benzeneinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisinfo:eu-repo/semantics/openAccessreponame:Biblioteca Digital de Teses e Dissertações da UERJinstname:Universidade do Estado do Rio de Janeiro (UERJ)instacron:UERJORIGINALJoao Carlos Serpa Soares.pdfapplication/pdf1724387http://www.bdtd.uerj.br/bitstream/1/12052/1/Joao+Carlos+Serpa+Soares.pdf0b59557913e4ca10c8683f1053928985MD511/120522024-02-27 15:36:08.885oai:www.bdtd.uerj.br:1/12052Biblioteca Digital de Teses e Dissertaçõeshttp://www.bdtd.uerj.br/PUBhttps://www.bdtd.uerj.br:8443/oai/requestbdtd.suporte@uerj.bropendoar:29032024-02-27T18:36:08Biblioteca Digital de Teses e Dissertações da UERJ - Universidade do Estado do Rio de Janeiro (UERJ)false
dc.title.por.fl_str_mv Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno
dc.title.alternative.eng.fl_str_mv Catalysts Ru / xZnO-Al2O3 in the partial hydrogenation of benzene
title Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno
spellingShingle Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno
Soares, João Carlos Serpa
Ruthenium
hydrogenation
cyclohexene
zinc
Rutênio
hidrogenação
cicloexeno
zinco
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
title_short Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno
title_full Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno
title_fullStr Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno
title_full_unstemmed Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno
title_sort Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno
author Soares, João Carlos Serpa
author_facet Soares, João Carlos Serpa
author_role author
dc.contributor.advisor1.fl_str_mv Zotin, Fatima Maria Zanon
dc.contributor.advisor1Lattes.fl_str_mv ://lattes.cnpq.br/2398224913573093
dc.contributor.advisor-co1.fl_str_mv Araujo, Lucia Regina Raddi de
dc.contributor.advisor-co1Lattes.fl_str_mv http://lattes.cnpq.br/1592062469734844
dc.contributor.referee1.fl_str_mv Gaspar, Alexandre Barros
dc.contributor.referee1Lattes.fl_str_mv http://lattes.cnpq.br/1049735133222758
dc.contributor.referee2.fl_str_mv Silva, Mônica Antunes Pereira da
dc.contributor.referee2Lattes.fl_str_mv http://lattes.cnpq.br/3911383035330556
dc.contributor.referee3.fl_str_mv Zonetti, Priscila da Costa
dc.contributor.referee3Lattes.fl_str_mv http://lattes.cnpq.br/7522580132803695
dc.contributor.referee4.fl_str_mv Santos, Luz Amparo Palacio
dc.contributor.referee4Lattes.fl_str_mv http://lattes.cnpq.br/2277031732030434
dc.contributor.authorLattes.fl_str_mv http://lattes.cnpq.br/3708838349183919
dc.contributor.author.fl_str_mv Soares, João Carlos Serpa
contributor_str_mv Zotin, Fatima Maria Zanon
Araujo, Lucia Regina Raddi de
Gaspar, Alexandre Barros
Silva, Mônica Antunes Pereira da
Zonetti, Priscila da Costa
Santos, Luz Amparo Palacio
dc.subject.eng.fl_str_mv Ruthenium
hydrogenation
cyclohexene
zinc
topic Ruthenium
hydrogenation
cyclohexene
zinc
Rutênio
hidrogenação
cicloexeno
zinco
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
dc.subject.por.fl_str_mv Rutênio
hidrogenação
cicloexeno
zinco
dc.subject.cnpq.fl_str_mv CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
description Benzene has been associated with an increase in diseases such as leukemia and it can also cause irreversible chromosomal modifications and damage to life. The cyclohexene is an intermediate for nylon and other fine chemical products and it can be generated through partial benzene hydrogenation, which is an alternative application for this toxic compound. However, from the thermodynamic point of view, the total benzene hydrogenation to cyclohexane is much more favorable than its partial hydrogenation to cyclohexene. Based in this context, this work aims at the preparation, characterization and evaluation of Ru/xZnO-Al2O3 catalysts in the partial benzene hydrogenation reaction using a batch reactor. The ZnAl mixed oxides were synthesized by co-precipitation of their respective salts. The catalysts were prepared by dry impregnation of RuCl3.6H2O and the samples received the following nomenclatures: RuAl, Ru5ZnAl, Ru10ZnAl, Ru20ZnAl, Ru50ZnAl, Ru90ZnAl and RuZn. Textural analysis, X-ray fluorescence, X-ray diffraction, X-ray phoelectron, temperature programmed reduction and H2 chemisorption techniques were used to characterize the catalysts. Partial benzene hydrogenation was carried out in a PARR reactor Instruments. The order of activity for the reaction with pure benzene was as follows: Ru10ZnAl >>> Ru5ZnAl > Ru20ZnAl > RuAl >> Ru90ZnAl = Ru50ZnAl = RuZn. Over the studied catalysts, Ru10ZnAl presented lower particle size (8 nm) and higher surface area (297 m².g-1) and these factors most likely have favoured ruthenium high dispersion on the catalyst surface. In addition, through the TPR analysis, there was a partial ZnO reduction on this catalyst. Tests conducted with addition of solvents using Ru10ZnAl catalyst showed lower activities than the ones containing only benzene
publishDate 2014
dc.date.issued.fl_str_mv 2014-10-24
dc.date.available.fl_str_mv 2018-05-08
dc.date.accessioned.fl_str_mv 2021-01-06T19:37:53Z
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/masterThesis
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dc.identifier.citation.fl_str_mv SOARES, João Carlos Serpa. Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno. 2014. 98 f. Dissertação (Mestrado em Processos Químicos e Meio Ambiente) - Universidade do Estado do Rio de Janeiro, Rio de Janeiro, 2014.
dc.identifier.uri.fl_str_mv http://www.bdtd.uerj.br/handle/1/12052
identifier_str_mv SOARES, João Carlos Serpa. Catalisadores Ru/xZnO-Al2O3 na hidrogenação parcial do benzeno. 2014. 98 f. Dissertação (Mestrado em Processos Químicos e Meio Ambiente) - Universidade do Estado do Rio de Janeiro, Rio de Janeiro, 2014.
url http://www.bdtd.uerj.br/handle/1/12052
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dc.publisher.department.fl_str_mv Centro de Tecnologia e Ciências::Instituto de Química
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