Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos
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/9475 |
Resumo: | New sources of clean energy have been studied, such as hydrogen (H2). Carbon monoxide, a subproduct of its production, poisons the fuel cell. To reach concentrations below 10 ppm, the addition of preferential CO oxidation reaction (PROX-CO) is required. This work is based on the study of behavior of gold and iron catalysts for PROX-CO. Studies point to high activity and good selectivity in PROX-CO with the combination of Au and Fe in catalysts, especially at low temperatures, although there are effects of the iron-gold interaction to be clarified. M. Haruta, H. Kung and I. Green have proposed mechanisms of reaction where the support plays an important role in PROX-CO, either by its O2 vacancies at the interface with the Au NPs or by taking part in the adsorption of CO molecules. Iron oxides become interesting as they are known for their oxygen vacancies and have high oxygen mobility in their network that varies according to the phase of this metal oxide. Results with Au and/or Fe catalysts supported on γ-Al2O3 showed that varying the synthesis, interaction and oxidation state of Au and Fe were modified. Catalysis tests for PROX-CO with previously reduced samples were more active possibly due to the formation of Au+/Au0 ions essentials for the activation and oxidation of CO. AuFeAl sample reduced at 400°C was shown to be most promising for PROX-CO of the samples tested, due both conversion and selectivity. Subsequently, gold catalysts were supported in the phases hematite, goethite and magnetite of iron oxide obtained from different preparation methods with different thermal treatments. These catalysts presented very different performance for PROX-CO. The performance for hematite-supported Au catalysts was higher. The AuHSG catalyst, which at around 110°C, showed a 33% CO conversion with acceptable CO2 selectivity (above 1:1 CO and O2 conversions respectively). |
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Franke, Karen NiégePalhares, Adriana Paula Ferreirahttp://lattes.cnpq.br/5736423072715628http://lattes.cnpq.br/35723895396008486b7f5411-1311-420d-a850-81eac81cbb2f2018-02-21T19:48:35Z2018-02-21T19:48:35Z2017-04-07FRANKE, Karen Niége. Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos. 2017. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2017. Disponível em: https://repositorio.ufscar.br/handle/ufscar/9475.https://repositorio.ufscar.br/handle/ufscar/9475New sources of clean energy have been studied, such as hydrogen (H2). Carbon monoxide, a subproduct of its production, poisons the fuel cell. To reach concentrations below 10 ppm, the addition of preferential CO oxidation reaction (PROX-CO) is required. This work is based on the study of behavior of gold and iron catalysts for PROX-CO. Studies point to high activity and good selectivity in PROX-CO with the combination of Au and Fe in catalysts, especially at low temperatures, although there are effects of the iron-gold interaction to be clarified. M. Haruta, H. Kung and I. Green have proposed mechanisms of reaction where the support plays an important role in PROX-CO, either by its O2 vacancies at the interface with the Au NPs or by taking part in the adsorption of CO molecules. Iron oxides become interesting as they are known for their oxygen vacancies and have high oxygen mobility in their network that varies according to the phase of this metal oxide. Results with Au and/or Fe catalysts supported on γ-Al2O3 showed that varying the synthesis, interaction and oxidation state of Au and Fe were modified. Catalysis tests for PROX-CO with previously reduced samples were more active possibly due to the formation of Au+/Au0 ions essentials for the activation and oxidation of CO. AuFeAl sample reduced at 400°C was shown to be most promising for PROX-CO of the samples tested, due both conversion and selectivity. Subsequently, gold catalysts were supported in the phases hematite, goethite and magnetite of iron oxide obtained from different preparation methods with different thermal treatments. These catalysts presented very different performance for PROX-CO. The performance for hematite-supported Au catalysts was higher. The AuHSG catalyst, which at around 110°C, showed a 33% CO conversion with acceptable CO2 selectivity (above 1:1 CO and O2 conversions respectively).Novas fontes de energia limpa têm sido estudadas, como o gás hidrogênio. Porém o monóxido de carbono, subproduto da sua produção, envenena a célula a combustível. Para atingir concentrações abaixo de 10 ppm, faz-se necessária a adição de uma etapa de reação de oxidação preferencial do CO (PROX-CO). Este trabalho se baseia no estudo do comportamento de catalisadores de ouro e ferro para a PROX-CO. Estudos apontam para uma elevada atividade e boa seletividade na PROX-CO com a combinação de Au e Fe em catalisadores, especialmente a baixas temperaturas, embora existam efeitos da interação ferro-ouro a serem esclarecidos. M. Haruta, H. Kung e I. Green propuseram mecanismos de reação onde o suporte desempenha um papel importante na PROX-CO, seja por suas vacâncias de O2 na interface com as NPs de Au ou participando da adsorção de moléculas de CO. Desta forma os óxidos de ferro se tornam interessantes, pois são conhecidos por suas vacâncias de oxigênio e possuem alta mobilidade de oxigênio na sua rede que varia de acordo com a fase deste óxido metálico. Resultados com catalisadores de Au e/ou Fe suportados em γ-Al2O3 mostraram que variando a síntese, a interação e o estado de oxidação do Au e do Fe foram modificados. Ensaios para a PROX-CO com amostras previamente reduzidas se mostraram mais ativas possivelmente devido a formação de íons Au+/Au0 essenciais para ativação e oxidação do CO. Dos catalisadores testados, a amostra AuFeAl reduzida a 400°C se demonstrou mais promissora para a PROX-CO tanto pela conversão como pela seletividade. Posteriormente, catalisadores de ouro foram suportados nas fases hematita, goethita e magnetita de óxido de ferro obtidos a partir de diferentes métodos de preparação com diferentes tratamentos térmicos. Estes catalisadores apresentaram desempenho para PROX-CO bem distintos. O desempenho para os catalisadores de Au suportados em hematita se mostrou superior. Destaca-se o catalisador AuHSG que em torno de 110°C apresentou conversão de CO de 33% com seletividade a CO2 aceitável (acima de 1:1 de conversões de CO e O2 respectivamente).Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)porUniversidade Federal de São CarlosCâmpus São CarlosPrograma de Pós-Graduação em Engenharia Química - PPGEQUFSCarCélula combustívelOxidação preferencial do monóxido de carbono (PROX-CO)OuroFerroFases de óxido de ferroFuel cellPreferential oxidation of carbon monoxide (PROX-CO)GoldIronIron oxide phasesENGENHARIAS::ENGENHARIA QUIMICACatalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativosinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisOnline6006003375b39f-fde0-4628-950c-0a09cc225fe5info:eu-repo/semantics/openAccessreponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINALDissKNF.pdfDissKNF.pdfapplication/pdf4995350https://repositorio.ufscar.br/bitstream/ufscar/9475/1/DissKNF.pdff4b3507a08ca4d99b7b0c2f50fcc60b4MD51LICENSElicense.txtlicense.txttext/plain; charset=utf-81957https://repositorio.ufscar.br/bitstream/ufscar/9475/2/license.txtae0398b6f8b235e40ad82cba6c50031dMD52TEXTDissKNF.pdf.txtDissKNF.pdf.txtExtracted texttext/plain249196https://repositorio.ufscar.br/bitstream/ufscar/9475/3/DissKNF.pdf.txt711e2bb6bfa8f5801c796efd18745691MD53THUMBNAILDissKNF.pdf.jpgDissKNF.pdf.jpgIM Thumbnailimage/jpeg7074https://repositorio.ufscar.br/bitstream/ufscar/9475/4/DissKNF.pdf.jpga3af1055d98a27987ed8ca8692ce8a09MD54ufscar/94752023-09-18 18:31:12.876oai:repositorio.ufscar.br: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Repositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestopendoar:43222023-09-18T18:31:12Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false |
dc.title.por.fl_str_mv |
Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos |
title |
Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos |
spellingShingle |
Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos Franke, Karen Niége Célula combustível Oxidação preferencial do monóxido de carbono (PROX-CO) Ouro Ferro Fases de óxido de ferro Fuel cell Preferential oxidation of carbon monoxide (PROX-CO) Gold Iron Iron oxide phases ENGENHARIAS::ENGENHARIA QUIMICA |
title_short |
Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos |
title_full |
Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos |
title_fullStr |
Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos |
title_full_unstemmed |
Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos |
title_sort |
Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos |
author |
Franke, Karen Niége |
author_facet |
Franke, Karen Niége |
author_role |
author |
dc.contributor.authorlattes.por.fl_str_mv |
http://lattes.cnpq.br/3572389539600848 |
dc.contributor.author.fl_str_mv |
Franke, Karen Niége |
dc.contributor.advisor1.fl_str_mv |
Palhares, Adriana Paula Ferreira |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/5736423072715628 |
dc.contributor.authorID.fl_str_mv |
6b7f5411-1311-420d-a850-81eac81cbb2f |
contributor_str_mv |
Palhares, Adriana Paula Ferreira |
dc.subject.por.fl_str_mv |
Célula combustível Oxidação preferencial do monóxido de carbono (PROX-CO) Ouro Ferro Fases de óxido de ferro |
topic |
Célula combustível Oxidação preferencial do monóxido de carbono (PROX-CO) Ouro Ferro Fases de óxido de ferro Fuel cell Preferential oxidation of carbon monoxide (PROX-CO) Gold Iron Iron oxide phases ENGENHARIAS::ENGENHARIA QUIMICA |
dc.subject.eng.fl_str_mv |
Fuel cell Preferential oxidation of carbon monoxide (PROX-CO) Gold Iron Iron oxide phases |
dc.subject.cnpq.fl_str_mv |
ENGENHARIAS::ENGENHARIA QUIMICA |
description |
New sources of clean energy have been studied, such as hydrogen (H2). Carbon monoxide, a subproduct of its production, poisons the fuel cell. To reach concentrations below 10 ppm, the addition of preferential CO oxidation reaction (PROX-CO) is required. This work is based on the study of behavior of gold and iron catalysts for PROX-CO. Studies point to high activity and good selectivity in PROX-CO with the combination of Au and Fe in catalysts, especially at low temperatures, although there are effects of the iron-gold interaction to be clarified. M. Haruta, H. Kung and I. Green have proposed mechanisms of reaction where the support plays an important role in PROX-CO, either by its O2 vacancies at the interface with the Au NPs or by taking part in the adsorption of CO molecules. Iron oxides become interesting as they are known for their oxygen vacancies and have high oxygen mobility in their network that varies according to the phase of this metal oxide. Results with Au and/or Fe catalysts supported on γ-Al2O3 showed that varying the synthesis, interaction and oxidation state of Au and Fe were modified. Catalysis tests for PROX-CO with previously reduced samples were more active possibly due to the formation of Au+/Au0 ions essentials for the activation and oxidation of CO. AuFeAl sample reduced at 400°C was shown to be most promising for PROX-CO of the samples tested, due both conversion and selectivity. Subsequently, gold catalysts were supported in the phases hematite, goethite and magnetite of iron oxide obtained from different preparation methods with different thermal treatments. These catalysts presented very different performance for PROX-CO. The performance for hematite-supported Au catalysts was higher. The AuHSG catalyst, which at around 110°C, showed a 33% CO conversion with acceptable CO2 selectivity (above 1:1 CO and O2 conversions respectively). |
publishDate |
2017 |
dc.date.issued.fl_str_mv |
2017-04-07 |
dc.date.accessioned.fl_str_mv |
2018-02-21T19:48:35Z |
dc.date.available.fl_str_mv |
2018-02-21T19:48:35Z |
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 |
FRANKE, Karen Niége. Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos. 2017. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2017. Disponível em: https://repositorio.ufscar.br/handle/ufscar/9475. |
dc.identifier.uri.fl_str_mv |
https://repositorio.ufscar.br/handle/ufscar/9475 |
identifier_str_mv |
FRANKE, Karen Niége. Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos. 2017. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2017. Disponível em: https://repositorio.ufscar.br/handle/ufscar/9475. |
url |
https://repositorio.ufscar.br/handle/ufscar/9475 |
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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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