Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol
Autor(a) principal: | |
---|---|
Data de Publicação: | 2015 |
Tipo de documento: | Dissertação |
Idioma: | por |
Título da fonte: | Repositório Institucional da UFSCAR |
Texto Completo: | https://repositorio.ufscar.br/handle/ufscar/7476 |
Resumo: | In intense search best environmental conditions, it is necessary to invest in renewable fuels, affordable and low polluting. With the aim to participate in this effort, this work was undertaken to study the steam reforming of ethanol. Cobalt catalysts supported on SiO2 were studied using mass loading of lanthanum 10, 20 and 30% mass content, and 0,5% platinum as additives in order to check their influences on the initial catalyst to reduce carbon formation on the catalyst surface, enhancing the activity, stability and selectivity for H2. All catalysts were prepared by impregnation method. Were characterized by temperature programmed reduction in H2, Hydrogen Chemisorption, surface area by BET, X ray diffraction method, thermo gravimetric analysis and chemical analysis. Subsequently, the reaction RVE catalysts, which was analyzed in conversion and selectivity were applied. The TPR and XRD analyzes observed the formation of Co3O4 which espinélia phase is reduced to CoO and Co°, respectively. Subsequently, the catalysts were used for ethanol steam reforming reaction, where the conversion, selectivity, and stability was analyzed. In XRD analysis and RTP observed the formation of Co3O4 that espinélia phase and reduces CoO and Co°, respectively. Also, it was identified diffraction peaks relating to La2O3 and La(OH)3; platinum, and a broad peak was assigned to the SiO2 structure, which has low crystallinity. There was a decrease in coking catalysts, effect obtained by forming lanthanum oxicarbonate, which was also identified by XRD. The increased lanthanum loading also influence the decrease in particle size, thereby increasing the dispersion of the catalysts. During the 24-hour stability test, the catalyst is not desactivated. It was identified that the impregnation method used and the utilized treating conditions were adequate to obtain the desired compounds for reform to ethanol vapor. The CoLa2SiO2 catalyst showed promise for ethanol steam reforming, with better selectivity to hydrogen, with little formation of undesirable products. The addition of 0.5% by mass Pt content in the cobalt catalyst has not led to a significant increase in product formation and conversion. The monometallic Pt catalyst (0.5% w / w) proved active and with good hydrogen selectivity even with a small amount of active phase. This behavior can be related to the presence of highly dispersed platinum metal on the surface. The best performing catalysts did not show the formation of CO, which can be related to the addition of lanthanum. |
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Baldoino, Marília Gabriela BranquinhoAssaf, José Mansurhttp://lattes.cnpq.br/9563312407691130http://lattes.cnpq.br/0292961252771980c05a715a-a032-453e-ae0d-1f6621ab599c2016-09-26T20:50:28Z2016-09-26T20:50:28Z2015-03-24BALDOINO, Marília Gabriela Branquinho. Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol. 2015. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2015. Disponível em: https://repositorio.ufscar.br/handle/ufscar/7476.https://repositorio.ufscar.br/handle/ufscar/7476In intense search best environmental conditions, it is necessary to invest in renewable fuels, affordable and low polluting. With the aim to participate in this effort, this work was undertaken to study the steam reforming of ethanol. Cobalt catalysts supported on SiO2 were studied using mass loading of lanthanum 10, 20 and 30% mass content, and 0,5% platinum as additives in order to check their influences on the initial catalyst to reduce carbon formation on the catalyst surface, enhancing the activity, stability and selectivity for H2. All catalysts were prepared by impregnation method. Were characterized by temperature programmed reduction in H2, Hydrogen Chemisorption, surface area by BET, X ray diffraction method, thermo gravimetric analysis and chemical analysis. Subsequently, the reaction RVE catalysts, which was analyzed in conversion and selectivity were applied. The TPR and XRD analyzes observed the formation of Co3O4 which espinélia phase is reduced to CoO and Co°, respectively. Subsequently, the catalysts were used for ethanol steam reforming reaction, where the conversion, selectivity, and stability was analyzed. In XRD analysis and RTP observed the formation of Co3O4 that espinélia phase and reduces CoO and Co°, respectively. Also, it was identified diffraction peaks relating to La2O3 and La(OH)3; platinum, and a broad peak was assigned to the SiO2 structure, which has low crystallinity. There was a decrease in coking catalysts, effect obtained by forming lanthanum oxicarbonate, which was also identified by XRD. The increased lanthanum loading also influence the decrease in particle size, thereby increasing the dispersion of the catalysts. During the 24-hour stability test, the catalyst is not desactivated. It was identified that the impregnation method used and the utilized treating conditions were adequate to obtain the desired compounds for reform to ethanol vapor. The CoLa2SiO2 catalyst showed promise for ethanol steam reforming, with better selectivity to hydrogen, with little formation of undesirable products. The addition of 0.5% by mass Pt content in the cobalt catalyst has not led to a significant increase in product formation and conversion. The monometallic Pt catalyst (0.5% w / w) proved active and with good hydrogen selectivity even with a small amount of active phase. This behavior can be related to the presence of highly dispersed platinum metal on the surface. The best performing catalysts did not show the formation of CO, which can be related to the addition of lanthanum.Na intensa busca por melhores condições ambientais, é necessário investir em combustíveis renováveis, acessíveis economicamente e pouco poluentes. Visando participar deste esforço, este trabalho está inserido num conjunto de estudos do processo de reforma a vapor do etanol (RVE). Foram estudados catalisadores de cobalto suportados em SiO2, utilizando carga mássica de lantânio em 10, 20 e 30% e teor mássico 0,5% de platina como aditivos, a fim de se verificar as influências destes promotores sobre o catalisador inicial de Co/SiO2: diminuição da formação de carbono sobre a superfície dos catalisadores e melhora da atividade, estabilidade e seletividade a H2. Todos os experimentos foram preparados pelo método de impregnação por via úmida e caracterizados por redução à temperatura programada de H2, quimissorção de hidrogênio, a área superficial pelo método B.E.T., difração de raios X, análise termogravimétrica e análise química. Os catalisadores foram testados na reação reforma a vapor do etanol, onde foi analisada a conversão, seletividade e estabilidade. Nas análises de DRX e RTP observou-se a formação da fase tipo espinélio de Co3O4 que se reduz a CoO e Co°, progressivamente. Também identificaram picos de difração referentes ao La2O3 e La(OH)3; à platina metálica, Pt°, e um largo pico que foi atribuída à estrutura de SiO2, que apresenta baixa cristalinidade. Houve a diminuição de coque nos catalisadores, efeito obtido através da formação de oxicarbonato de lantânio, que também foi identificado através do DRX. O aumento da carga de lantânio influenciou a diminuição do tamanho das partículas, aumentando assim a dispersão dos catalisadores. Durante os testes de estabilidade de 24 horas, nenhum catalisador se desativou. Identificou-se que o método de impregnação utilizado e as condições de tratamento das amostras foram adequados para obtenção dos compostos desejados para a reforma à vapor do etanol. O catalisador de CoSiO2 com teor mássico de 20% de lantânio mostrou-se promissor para a reforma a vapor de etanol, apresentando melhor seletividade a hidrogênio, com pouca formação de produtos indesejáveis. A adição de 0,5% em teor mássico de Pt no catalisador de cobalto não levou a um aumento significativo na formação de produtos e na conversão. O catalisador monometálico de Pt (0,5% m/m) mostrou-se ativo e com boa seletividade a hidrogênio, mesmo com pequena quantidade de fase ativa. Este comportamento pode ser relacionado com a presença de platina metálica altamente dispersa na superfície. Os catalisadores com melhores desempenhos não apresentaram formação de CO, o que pode ser relacionado à adição de lantânio.Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)porUniversidade Federal de São CarlosCâmpus São CarlosPrograma de Pós-Graduação em Engenharia Química - PPGEQUFSCarEtanolReforma a vaporHidrogênioCatalisadoresENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICAENGENHARIAS::ENGENHARIA QUIMICACatalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanolinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisOnline600600d348d7f1-5523-40f0-9d08-b82dac73a6d8info:eu-repo/semantics/openAccessreponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINALDissMGBB.pdfDissMGBB.pdfapplication/pdf3813643https://repositorio.ufscar.br/bitstream/ufscar/7476/1/DissMGBB.pdf80f77b5bb8ccd773369afd7f536bae1eMD51LICENSElicense.txtlicense.txttext/plain; charset=utf-81957https://repositorio.ufscar.br/bitstream/ufscar/7476/2/license.txtae0398b6f8b235e40ad82cba6c50031dMD52TEXTDissMGBB.pdf.txtDissMGBB.pdf.txtExtracted texttext/plain171404https://repositorio.ufscar.br/bitstream/ufscar/7476/3/DissMGBB.pdf.txt263df0dad9aca3328ad15bd8f4bf808dMD53THUMBNAILDissMGBB.pdf.jpgDissMGBB.pdf.jpgIM Thumbnailimage/jpeg7957https://repositorio.ufscar.br/bitstream/ufscar/7476/4/DissMGBB.pdf.jpg472130fb5115afe1f417ee7957bef664MD54ufscar/74762023-09-18 18:30:52.976oai:repositorio.ufscar.br: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Repositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestopendoar:43222023-09-18T18:30:52Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false |
dc.title.por.fl_str_mv |
Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol |
title |
Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol |
spellingShingle |
Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol Baldoino, Marília Gabriela Branquinho Etanol Reforma a vapor Hidrogênio Catalisadores ENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA QUIMICA |
title_short |
Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol |
title_full |
Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol |
title_fullStr |
Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol |
title_full_unstemmed |
Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol |
title_sort |
Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol |
author |
Baldoino, Marília Gabriela Branquinho |
author_facet |
Baldoino, Marília Gabriela Branquinho |
author_role |
author |
dc.contributor.authorlattes.por.fl_str_mv |
http://lattes.cnpq.br/0292961252771980 |
dc.contributor.author.fl_str_mv |
Baldoino, Marília Gabriela Branquinho |
dc.contributor.advisor1.fl_str_mv |
Assaf, José Mansur |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/9563312407691130 |
dc.contributor.authorID.fl_str_mv |
c05a715a-a032-453e-ae0d-1f6621ab599c |
contributor_str_mv |
Assaf, José Mansur |
dc.subject.por.fl_str_mv |
Etanol Reforma a vapor Hidrogênio Catalisadores |
topic |
Etanol Reforma a vapor Hidrogênio Catalisadores ENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA QUIMICA |
dc.subject.cnpq.fl_str_mv |
ENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA QUIMICA |
description |
In intense search best environmental conditions, it is necessary to invest in renewable fuels, affordable and low polluting. With the aim to participate in this effort, this work was undertaken to study the steam reforming of ethanol. Cobalt catalysts supported on SiO2 were studied using mass loading of lanthanum 10, 20 and 30% mass content, and 0,5% platinum as additives in order to check their influences on the initial catalyst to reduce carbon formation on the catalyst surface, enhancing the activity, stability and selectivity for H2. All catalysts were prepared by impregnation method. Were characterized by temperature programmed reduction in H2, Hydrogen Chemisorption, surface area by BET, X ray diffraction method, thermo gravimetric analysis and chemical analysis. Subsequently, the reaction RVE catalysts, which was analyzed in conversion and selectivity were applied. The TPR and XRD analyzes observed the formation of Co3O4 which espinélia phase is reduced to CoO and Co°, respectively. Subsequently, the catalysts were used for ethanol steam reforming reaction, where the conversion, selectivity, and stability was analyzed. In XRD analysis and RTP observed the formation of Co3O4 that espinélia phase and reduces CoO and Co°, respectively. Also, it was identified diffraction peaks relating to La2O3 and La(OH)3; platinum, and a broad peak was assigned to the SiO2 structure, which has low crystallinity. There was a decrease in coking catalysts, effect obtained by forming lanthanum oxicarbonate, which was also identified by XRD. The increased lanthanum loading also influence the decrease in particle size, thereby increasing the dispersion of the catalysts. During the 24-hour stability test, the catalyst is not desactivated. It was identified that the impregnation method used and the utilized treating conditions were adequate to obtain the desired compounds for reform to ethanol vapor. The CoLa2SiO2 catalyst showed promise for ethanol steam reforming, with better selectivity to hydrogen, with little formation of undesirable products. The addition of 0.5% by mass Pt content in the cobalt catalyst has not led to a significant increase in product formation and conversion. The monometallic Pt catalyst (0.5% w / w) proved active and with good hydrogen selectivity even with a small amount of active phase. This behavior can be related to the presence of highly dispersed platinum metal on the surface. The best performing catalysts did not show the formation of CO, which can be related to the addition of lanthanum. |
publishDate |
2015 |
dc.date.issued.fl_str_mv |
2015-03-24 |
dc.date.accessioned.fl_str_mv |
2016-09-26T20:50:28Z |
dc.date.available.fl_str_mv |
2016-09-26T20:50:28Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/masterThesis |
format |
masterThesis |
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publishedVersion |
dc.identifier.citation.fl_str_mv |
BALDOINO, Marília Gabriela Branquinho. Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol. 2015. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2015. Disponível em: https://repositorio.ufscar.br/handle/ufscar/7476. |
dc.identifier.uri.fl_str_mv |
https://repositorio.ufscar.br/handle/ufscar/7476 |
identifier_str_mv |
BALDOINO, Marília Gabriela Branquinho. Catalisadores de Co e Pt suportados em La2O3 e SiO2 aplicados na reforma a vapor do etanol. 2015. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2015. Disponível em: https://repositorio.ufscar.br/handle/ufscar/7476. |
url |
https://repositorio.ufscar.br/handle/ufscar/7476 |
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openAccess |
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Universidade Federal de São Carlos Câmpus São Carlos |
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Programa de Pós-Graduação em Engenharia Química - PPGEQ |
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UFSCar |
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Universidade Federal de São Carlos Câmpus São Carlos |
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