Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas
Autor(a) principal: | |
---|---|
Data de Publicação: | 2017 |
Tipo de documento: | Dissertação |
Idioma: | por |
Título da fonte: | Repositório Institucional da UFSCAR |
Texto Completo: | https://repositorio.ufscar.br/handle/ufscar/9849 |
Resumo: | The effect of iron incorporation on the catalytic properties of Ni / MgAl2O4 for the Ethanol Steam Reforming (ESR) was studied. Samples of different Fe/Ni molar ratios were prepared by wet impregnation of MgAl2O4, synthesized by the sol-gel method. The catalysts were characterized by X-ray diffraction (XRD), temperature programmed reduction (TPR), temperature programmed desorption of ethanol, near-edge X-ray absorption spectroscopy (XANES), and photoelectric spectroscopy of X-rays. The formation of the MgAl2O4 spinel was confirmed by XDR and the NiO, Fe2O3 and NiFe2O4 phases were identified in the monometallic nickel, iron and bimetallic catalysts, respectively. In TPR it was verified that the presence of nickel altered the iron properties in the bimetallic catalysts. The catalytic tests were carried out under an atmosphere of water:ethanol and water:ethanol:H2 in the temperature range of 250 to 650 °C. Changing the drag from He to hydrogen, reduced the degree of oxidation of the samples at low temperatures and, consequently, increased the activity. The higher the iron content, the lower the activity at low temperatures. The results of XANES indicated that a restructuring of the Ni-Fe particles occurs during the RVE. After the reduction, Ni-Fe alloy formation is obtained, with increasing temperature Fe migrates to the surface and is oxidized to FeO. The intensity of this reconstruction depends on the Fe/Ni ratio and the composition of the reactants, being more intense in the reaction without H2. Among the catalysts analyzed, 8Ni-5Fe was the most stable and selective to hydrogen gas during the ESR, presenting a lower carbon formation |
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Lara, Thais Paula NogueiraBueno, José Maria Corrêahttp://lattes.cnpq.br/0157452280626031http://lattes.cnpq.br/988921461204832522f1b10b-9811-41cd-ad03-5d413c90a6992018-05-02T18:32:30Z2018-05-02T18:32:30Z2017-03-02LARA, Thais Paula Nogueira. Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas. 2017. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2017. Disponível em: https://repositorio.ufscar.br/handle/ufscar/9849.https://repositorio.ufscar.br/handle/ufscar/9849The effect of iron incorporation on the catalytic properties of Ni / MgAl2O4 for the Ethanol Steam Reforming (ESR) was studied. Samples of different Fe/Ni molar ratios were prepared by wet impregnation of MgAl2O4, synthesized by the sol-gel method. The catalysts were characterized by X-ray diffraction (XRD), temperature programmed reduction (TPR), temperature programmed desorption of ethanol, near-edge X-ray absorption spectroscopy (XANES), and photoelectric spectroscopy of X-rays. The formation of the MgAl2O4 spinel was confirmed by XDR and the NiO, Fe2O3 and NiFe2O4 phases were identified in the monometallic nickel, iron and bimetallic catalysts, respectively. In TPR it was verified that the presence of nickel altered the iron properties in the bimetallic catalysts. The catalytic tests were carried out under an atmosphere of water:ethanol and water:ethanol:H2 in the temperature range of 250 to 650 °C. Changing the drag from He to hydrogen, reduced the degree of oxidation of the samples at low temperatures and, consequently, increased the activity. The higher the iron content, the lower the activity at low temperatures. The results of XANES indicated that a restructuring of the Ni-Fe particles occurs during the RVE. After the reduction, Ni-Fe alloy formation is obtained, with increasing temperature Fe migrates to the surface and is oxidized to FeO. The intensity of this reconstruction depends on the Fe/Ni ratio and the composition of the reactants, being more intense in the reaction without H2. Among the catalysts analyzed, 8Ni-5Fe was the most stable and selective to hydrogen gas during the ESR, presenting a lower carbon formationEstudou-se o efeito da incorporação de ferro nas propriedades catalíticas do Ni/MgAl2O4 para a Reforma a Vapor do Etanol (RVE). Foram preparadas amostras de diferentes razões molares Fe/Ni pela impregnação úmida do MgAl2O4, sintetizado pelo método sol-gel. Os catalisadores foram caracterizados através de difração de raios X (DRX), redução à temperatura programa (TPR), dessorção de etanol a temperatura programada, espectroscopia de absorção de raios X próximo da borda (XANES), e espectroscopia fotoelétrica de raios X. Pelo DRX confirmou-se a formação do espinélio MgAl2O4 e identificou-se a presença das fases NiO, Fe2O3 e NiFe2O4 nos catalisadores monometálicos de níquel, de ferro e bimetálicos, respectivamente. No TPR verificou-se que a presença do ferro alterou as propriedades do níquel nos catalisadores bimetálicos. Os testes catalíticos foram realizados em atmosfera água:etanol e água:etanol:H2 no intervalo de temperatura de 250 a 650 °C. A troca do arraste de He para hidrogênio, reduziu o grau de oxidação das amostras em baixas temperaturas, e consequentemente, aumentou a atividade. Os resultados de XANES indicaram que ocorre uma reestruturação das partículas Ni-Fe durante a RVE. Após a redução, tem-se a formação da liga Ni-Fe, com o aumento da temperatura durante a RVE o Fe migra para superfície e é oxidado a FeO. A intensidade dessa reconstrução depende da razão Fe/Ni e da composição dos reagentes, sendo mais intensa no meio sem H2. Dentre os catalisadores analisados, 8Ni-5Fe foi o mais estável e seletivo a gás hidrogênio durante a RVE, apresentando menor formação de carbono.Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)CNPq: 132147/2015-7porUniversidade Federal de São CarlosCâmpus São CarlosPrograma de Pós-Graduação em Engenharia Química - PPGEQUFSCarCatalisador de Ni/FeAtividade catalíticaFormação de ligaInfluência do meio reacionalENGENHARIAS::ENGENHARIA QUIMICA::OPERACOES INDUSTRIAIS E EQUIPAMENTOS PARA ENGENHARIA QUIMICAENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICAENGENHARIAS::ENGENHARIA QUIMICA::TECNOLOGIA QUIMICACatalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticasinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisOnline6006003b275236-acc5-4218-a33b-8f802e7f5a18info:eu-repo/semantics/openAccessreponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINALDissertação Thais Lara.pdfDissertação Thais Lara.pdfDissertação finalapplication/pdf2953232https://repositorio.ufscar.br/bitstream/ufscar/9849/2/Disserta%c3%a7%c3%a3o%20Thais%20Lara.pdf798754a681079a76a19fcb091994d39cMD52Carta Orientador.pdfCarta Orientador.pdfCarta Comprovanteapplication/pdf320920https://repositorio.ufscar.br/bitstream/ufscar/9849/1/Carta%20Orientador.pdf918476c1fc4da19aada7616e5e7ec169MD51LICENSElicense.txtlicense.txttext/plain; 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dc.title.por.fl_str_mv |
Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas |
title |
Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas |
spellingShingle |
Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas Lara, Thais Paula Nogueira Catalisador de Ni/Fe Atividade catalítica Formação de liga Influência do meio reacional ENGENHARIAS::ENGENHARIA QUIMICA::OPERACOES INDUSTRIAIS E EQUIPAMENTOS PARA ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA QUIMICA::TECNOLOGIA QUIMICA |
title_short |
Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas |
title_full |
Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas |
title_fullStr |
Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas |
title_full_unstemmed |
Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas |
title_sort |
Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas |
author |
Lara, Thais Paula Nogueira |
author_facet |
Lara, Thais Paula Nogueira |
author_role |
author |
dc.contributor.authorlattes.por.fl_str_mv |
http://lattes.cnpq.br/9889214612048325 |
dc.contributor.author.fl_str_mv |
Lara, Thais Paula Nogueira |
dc.contributor.advisor1.fl_str_mv |
Bueno, José Maria Corrêa |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/0157452280626031 |
dc.contributor.authorID.fl_str_mv |
22f1b10b-9811-41cd-ad03-5d413c90a699 |
contributor_str_mv |
Bueno, José Maria Corrêa |
dc.subject.por.fl_str_mv |
Catalisador de Ni/Fe Atividade catalítica Formação de liga Influência do meio reacional |
topic |
Catalisador de Ni/Fe Atividade catalítica Formação de liga Influência do meio reacional ENGENHARIAS::ENGENHARIA QUIMICA::OPERACOES INDUSTRIAIS E EQUIPAMENTOS PARA ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA QUIMICA::TECNOLOGIA QUIMICA |
dc.subject.cnpq.fl_str_mv |
ENGENHARIAS::ENGENHARIA QUIMICA::OPERACOES INDUSTRIAIS E EQUIPAMENTOS PARA ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA QUIMICA::TECNOLOGIA QUIMICA |
description |
The effect of iron incorporation on the catalytic properties of Ni / MgAl2O4 for the Ethanol Steam Reforming (ESR) was studied. Samples of different Fe/Ni molar ratios were prepared by wet impregnation of MgAl2O4, synthesized by the sol-gel method. The catalysts were characterized by X-ray diffraction (XRD), temperature programmed reduction (TPR), temperature programmed desorption of ethanol, near-edge X-ray absorption spectroscopy (XANES), and photoelectric spectroscopy of X-rays. The formation of the MgAl2O4 spinel was confirmed by XDR and the NiO, Fe2O3 and NiFe2O4 phases were identified in the monometallic nickel, iron and bimetallic catalysts, respectively. In TPR it was verified that the presence of nickel altered the iron properties in the bimetallic catalysts. The catalytic tests were carried out under an atmosphere of water:ethanol and water:ethanol:H2 in the temperature range of 250 to 650 °C. Changing the drag from He to hydrogen, reduced the degree of oxidation of the samples at low temperatures and, consequently, increased the activity. The higher the iron content, the lower the activity at low temperatures. The results of XANES indicated that a restructuring of the Ni-Fe particles occurs during the RVE. After the reduction, Ni-Fe alloy formation is obtained, with increasing temperature Fe migrates to the surface and is oxidized to FeO. The intensity of this reconstruction depends on the Fe/Ni ratio and the composition of the reactants, being more intense in the reaction without H2. Among the catalysts analyzed, 8Ni-5Fe was the most stable and selective to hydrogen gas during the ESR, presenting a lower carbon formation |
publishDate |
2017 |
dc.date.issued.fl_str_mv |
2017-03-02 |
dc.date.accessioned.fl_str_mv |
2018-05-02T18:32:30Z |
dc.date.available.fl_str_mv |
2018-05-02T18:32:30Z |
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.citation.fl_str_mv |
LARA, Thais Paula Nogueira. Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas. 2017. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2017. Disponível em: https://repositorio.ufscar.br/handle/ufscar/9849. |
dc.identifier.uri.fl_str_mv |
https://repositorio.ufscar.br/handle/ufscar/9849 |
identifier_str_mv |
LARA, Thais Paula Nogueira. Catalisadores Ni-Fe/MgAl2O4 na reforma a vapor do etanol: influência da razão molar Ni/Fe nas propriedades catalíticas. 2017. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2017. Disponível em: https://repositorio.ufscar.br/handle/ufscar/9849. |
url |
https://repositorio.ufscar.br/handle/ufscar/9849 |
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info:eu-repo/semantics/openAccess |
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openAccess |
dc.publisher.none.fl_str_mv |
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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