Catalisadores de Au suportados aplicados à oxidação preferencial do CO : influência da interação entre Au e Fe nos sítios ativos

Detalhes bibliográficos
Autor(a) principal: Franke, Karen Niége
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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spelling 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:ufscar/9475TElDRU7Dh0EgREUgRElTVFJJQlVJw4fDg08gTsODTy1FWENMVVNJVkEKCkNvbSBhIGFwcmVzZW50YcOnw6NvIGRlc3RhIGxpY2Vuw6dhLCB2b2PDqiAobyBhdXRvciAoZXMpIG91IG8gdGl0dWxhciBkb3MgZGlyZWl0b3MgZGUgYXV0b3IpIGNvbmNlZGUgw6AgVW5pdmVyc2lkYWRlCkZlZGVyYWwgZGUgU8OjbyBDYXJsb3MgbyBkaXJlaXRvIG7Do28tZXhjbHVzaXZvIGRlIHJlcHJvZHV6aXIsICB0cmFkdXppciAoY29uZm9ybWUgZGVmaW5pZG8gYWJhaXhvKSwgZS9vdQpkaXN0cmlidWlyIGEgc3VhIHRlc2Ugb3UgZGlzc2VydGHDp8OjbyAoaW5jbHVpbmRvIG8gcmVzdW1vKSBwb3IgdG9kbyBvIG11bmRvIG5vIGZvcm1hdG8gaW1wcmVzc28gZSBlbGV0csO0bmljbyBlCmVtIHF1YWxxdWVyIG1laW8sIGluY2x1aW5kbyBvcyBmb3JtYXRvcyDDoXVkaW8gb3UgdsOtZGVvLgoKVm9jw6ogY29uY29yZGEgcXVlIGEgVUZTQ2FyIHBvZGUsIHNlbSBhbHRlcmFyIG8gY29udGXDumRvLCB0cmFuc3BvciBhIHN1YSB0ZXNlIG91IGRpc3NlcnRhw6fDo28KcGFyYSBxdWFscXVlciBtZWlvIG91IGZvcm1hdG8gcGFyYSBmaW5zIGRlIHByZXNlcnZhw6fDo28uCgpWb2PDqiB0YW1iw6ltIGNvbmNvcmRhIHF1ZSBhIFVGU0NhciBwb2RlIG1hbnRlciBtYWlzIGRlIHVtYSBjw7NwaWEgYSBzdWEgdGVzZSBvdQpkaXNzZXJ0YcOnw6NvIHBhcmEgZmlucyBkZSBzZWd1cmFuw6dhLCBiYWNrLXVwIGUgcHJlc2VydmHDp8Ojby4KClZvY8OqIGRlY2xhcmEgcXVlIGEgc3VhIHRlc2Ugb3UgZGlzc2VydGHDp8OjbyDDqSBvcmlnaW5hbCBlIHF1ZSB2b2PDqiB0ZW0gbyBwb2RlciBkZSBjb25jZWRlciBvcyBkaXJlaXRvcyBjb250aWRvcwpuZXN0YSBsaWNlbsOnYS4gVm9jw6ogdGFtYsOpbSBkZWNsYXJhIHF1ZSBvIGRlcMOzc2l0byBkYSBzdWEgdGVzZSBvdSBkaXNzZXJ0YcOnw6NvIG7Do28sIHF1ZSBzZWphIGRlIHNldQpjb25oZWNpbWVudG8sIGluZnJpbmdlIGRpcmVpdG9zIGF1dG9yYWlzIGRlIG5pbmd1w6ltLgoKQ2FzbyBhIHN1YSB0ZXNlIG91IGRpc3NlcnRhw6fDo28gY29udGVuaGEgbWF0ZXJpYWwgcXVlIHZvY8OqIG7Do28gcG9zc3VpIGEgdGl0dWxhcmlkYWRlIGRvcyBkaXJlaXRvcyBhdXRvcmFpcywgdm9jw6oKZGVjbGFyYSBxdWUgb2J0ZXZlIGEgcGVybWlzc8OjbyBpcnJlc3RyaXRhIGRvIGRldGVudG9yIGRvcyBkaXJlaXRvcyBhdXRvcmFpcyBwYXJhIGNvbmNlZGVyIMOgIFVGU0NhcgpvcyBkaXJlaXRvcyBhcHJlc2VudGFkb3MgbmVzdGEgbGljZW7Dp2EsIGUgcXVlIGVzc2UgbWF0ZXJpYWwgZGUgcHJvcHJpZWRhZGUgZGUgdGVyY2Vpcm9zIGVzdMOhIGNsYXJhbWVudGUKaWRlbnRpZmljYWRvIGUgcmVjb25oZWNpZG8gbm8gdGV4dG8gb3Ugbm8gY29udGXDumRvIGRhIHRlc2Ugb3UgZGlzc2VydGHDp8OjbyBvcmEgZGVwb3NpdGFkYS4KCkNBU08gQSBURVNFIE9VIERJU1NFUlRBw4fDg08gT1JBIERFUE9TSVRBREEgVEVOSEEgU0lETyBSRVNVTFRBRE8gREUgVU0gUEFUUk9Dw41OSU8gT1UKQVBPSU8gREUgVU1BIEFHw4pOQ0lBIERFIEZPTUVOVE8gT1UgT1VUUk8gT1JHQU5JU01PIFFVRSBOw4NPIFNFSkEgQSBVRlNDYXIsClZPQ8OKIERFQ0xBUkEgUVVFIFJFU1BFSVRPVSBUT0RPUyBFIFFVQUlTUVVFUiBESVJFSVRPUyBERSBSRVZJU8ODTyBDT01PClRBTULDiU0gQVMgREVNQUlTIE9CUklHQcOHw5VFUyBFWElHSURBUyBQT1IgQ09OVFJBVE8gT1UgQUNPUkRPLgoKQSBVRlNDYXIgc2UgY29tcHJvbWV0ZSBhIGlkZW50aWZpY2FyIGNsYXJhbWVudGUgbyBzZXUgbm9tZSAocykgb3UgbyhzKSBub21lKHMpIGRvKHMpCmRldGVudG9yKGVzKSBkb3MgZGlyZWl0b3MgYXV0b3JhaXMgZGEgdGVzZSBvdSBkaXNzZXJ0YcOnw6NvLCBlIG7Do28gZmFyw6EgcXVhbHF1ZXIgYWx0ZXJhw6fDo28sIGFsw6ltIGRhcXVlbGFzCmNvbmNlZGlkYXMgcG9yIGVzdGEgbGljZW7Dp2EuCg==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
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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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dc.rights.driver.fl_str_mv info:eu-repo/semantics/openAccess
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dc.publisher.none.fl_str_mv Universidade Federal de São Carlos
Câmpus São Carlos
dc.publisher.program.fl_str_mv Programa de Pós-Graduação em Engenharia Química - PPGEQ
dc.publisher.initials.fl_str_mv UFSCar
publisher.none.fl_str_mv Universidade Federal de São Carlos
Câmpus São Carlos
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reponame_str Repositório Institucional da UFSCAR
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