Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO

Detalhes bibliográficos
Ano de defesa: 2008
Autor(a) principal: Silva, Edilene Deise da
Orientador(a): Urquieta-González, Ernesto Antonio
Banca de defesa: Não Informado pela instituição lattes
Tipo de documento: Dissertação
Tipo de acesso: Acesso aberto
Idioma: por
Instituição de defesa: Universidade Federal de São Carlos
Programa de Pós-Graduação: Programa de Pós-Graduação em Engenharia Química - PPGEQ
Departamento: Não Informado pela instituição
País: BR
Palavras-chave em Português:
Área do conhecimento CNPq:
Link de acesso: https://repositorio.ufscar.br/handle/20.500.14289/3997
Resumo: The emissions of the nitrogen oxides (NOx) must be hardly reduced in the next years. The catalytic reduction of NO with CO is one of the possible processes with potential to be able to transform those oxides in N2. In that process, supported noble metals have been the most used, however, their low stability in the presence of water steam or SO2, have led to develop studies to overcome those limitations. Perovkites type catalysts or transition metal oxides supported in a variety of support show activity in this reaction. Nevertheless, no adequate information about the activity of metal oxides supported on zeolites is found in the literature. In this context, the present work was focused to prepare and evaluate between 150°C and 500°C, Cu, Co or Fe containing catalysts dispersed on USY (Si/Al=3,4) or ZSM-5 (Si/Al=12,8) zeolites in the reduction of NO with CO and in the oxidation of CO to CO2. The oxide activity was also compared with that of the respective metal cations located in charge compensation sites. The catalysts were prepared by ion exchange or impregnation and characterized by AAS, XRD, DRS-UV and H2-TPR. Conversion data of NO to N2 on USY and ZSM-5 zeolites containing predominantly Cu2+ or Co2+ cations in exchangeable sites were more active when located on ZSM-5 zeolite (MFI structure), with the Cu2+ cations being more active. On the other hand, Cu, Co or Fe oxides supported on USY or ZSM-5 were more active than cations of considered metals in exchangeable sites, with conversion being dependent on the type and metal content and the type of zeolite. Among the studied metal oxides, the Fe one was the most active and selective. However the presence of O2 or water steam in the feed inhibited the NO reduction with CO on Fe oxide, which was attributed to the deactivation of the active sites by the water steam and the CO direct oxidation by O2 occurring preferentially than CO oxidation via NO reduction. This result gives evidence of the water steam leads to the deactivation of the metallic active sites and O2 favors the direct oxidation of CO to CO2 in detriment of its oxidation by NO reduction. The NO conversion was not significantly affected by the presence of SO2 in the feed (40 ppm).
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spelling Silva, Edilene Deise daUrquieta-González, Ernesto Antoniohttp://lattes.cnpq.br/2389975677904655http://lattes.cnpq.br/3672771633840838e6ca62ac-31f3-472c-bd8d-6f2191b5bfa82016-06-02T19:56:31Z2008-06-242016-06-02T19:56:31Z2008-04-08SILVA, Edilene Deise da. Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO. 2008. 125 f. Dissertação (Mestrado em Ciências Exatas e da Terra) - Universidade Federal de São Carlos, São Carlos, 2008.https://repositorio.ufscar.br/handle/20.500.14289/3997The emissions of the nitrogen oxides (NOx) must be hardly reduced in the next years. The catalytic reduction of NO with CO is one of the possible processes with potential to be able to transform those oxides in N2. In that process, supported noble metals have been the most used, however, their low stability in the presence of water steam or SO2, have led to develop studies to overcome those limitations. Perovkites type catalysts or transition metal oxides supported in a variety of support show activity in this reaction. Nevertheless, no adequate information about the activity of metal oxides supported on zeolites is found in the literature. In this context, the present work was focused to prepare and evaluate between 150°C and 500°C, Cu, Co or Fe containing catalysts dispersed on USY (Si/Al=3,4) or ZSM-5 (Si/Al=12,8) zeolites in the reduction of NO with CO and in the oxidation of CO to CO2. The oxide activity was also compared with that of the respective metal cations located in charge compensation sites. The catalysts were prepared by ion exchange or impregnation and characterized by AAS, XRD, DRS-UV and H2-TPR. Conversion data of NO to N2 on USY and ZSM-5 zeolites containing predominantly Cu2+ or Co2+ cations in exchangeable sites were more active when located on ZSM-5 zeolite (MFI structure), with the Cu2+ cations being more active. On the other hand, Cu, Co or Fe oxides supported on USY or ZSM-5 were more active than cations of considered metals in exchangeable sites, with conversion being dependent on the type and metal content and the type of zeolite. Among the studied metal oxides, the Fe one was the most active and selective. However the presence of O2 or water steam in the feed inhibited the NO reduction with CO on Fe oxide, which was attributed to the deactivation of the active sites by the water steam and the CO direct oxidation by O2 occurring preferentially than CO oxidation via NO reduction. This result gives evidence of the water steam leads to the deactivation of the metallic active sites and O2 favors the direct oxidation of CO to CO2 in detriment of its oxidation by NO reduction. The NO conversion was not significantly affected by the presence of SO2 in the feed (40 ppm).A emissão de óxidos de nitrogênio (NOx) deverá ser no curto prazo reduzida drasticamente. Dentre os processos com potencial para a conversão desses óxidos a N2 tem-se a redução catalítica de NO com CO. Nesse processo, metais nobres suportados têm sido os mais empregados, entretanto, sua baixa estabilidade na presença de vapor de água e de SO2, levam à necessidade de se realizar estudos que superem essas limitações. Catalisadores tipo perovskita ou de óxidos de metais de transição depositados sobre diversos suportes apresentam atividade nessa reação. Entretanto, pouca informação encontra-se disponível relacionada à atividade desses óxidos suportados em zeólitas. Dentro desse contexto, este trabalho teve como objetivo preparar catalisadores à base de Cu, Co ou Fe dispersos em zeólita USY (Si/Al=3,4) ou ZSM-5 (Si/Al=12,8) e avaliá-los na redução de NO a N2 e oxidação de CO a CO2 no intervalo entre 150°C e 500°C. A atividade desses óxidos foi comparada com cátions dos respectivos metais em sítios de compensação de carga. Os catalisadores foram preparados por troca iônica ou impregnação e caracterizados por EAA, DRX, ERD-UV e RTP-H2. Os resultados de conversão de NO a N2 sobre as zeólitas USY ou ZSM-5 com predominância de cátions Cu2+ e Co2+ compensando carga, mostraram que essas espécies foram mais ativas quando presentes na zeólita ZSM-5 (estrutura MFI), sendo os cátions de Cu mais ativos. Por outro lado, óxidos de Cu, Co ou Fe depositados sobre a USY ou ZSM-5 mostraramse mais ativos que cátions desses metais em sítios de compensação, com a conversão sendo dependente do tipo e do teor de metal e do tipo de zeólita. Dentre os óxidos estudados, o óxido de Fe foi o mais ativo e seletivo a N2, porém a presença de O2 ou vapor de água inibiram fortemente a redução de NO com CO sobre óxido de Fe. Esse resultado evidencia que o vapor de água desativa os sítios metálicos ativos e o O2 favorece a oxidação direta do CO a CO2 em detrimento da sua oxidação via redução de NO. A conversão de NO não foi afetada significantemente na presença de SO2 (40 ppm).Universidade Federal de Sao Carlosapplication/pdfporUniversidade Federal de São CarlosPrograma de Pós-Graduação em Engenharia Química - PPGEQUFSCarBRCatáliseZeólita FAURedução de NOENGENHARIAS::ENGENHARIA QUIMICACatalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com COinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesis-1-10fecd90c-2648-4551-9f5a-7b6c106679b1info:eu-repo/semantics/openAccessreponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARTEXT1834.pdf.txt1834.pdf.txtExtracted texttext/plain103450https://repositorio.ufscar.br/bitstreams/7390916b-9757-4834-b3f3-dc9a3cb0ce98/download6a35805ded4d2acf84582ab281b02da9MD53falseAnonymousREADORIGINAL1834.pdfapplication/pdf2502250https://repositorio.ufscar.br/bitstreams/a45b2743-22a3-4337-8ef2-309ef7e2743a/downloadb7141cbd006fe2ef074f6b3f3c48dfd2MD51trueAnonymousREADTHUMBNAIL1834.pdf.jpg1834.pdf.jpgIM Thumbnailimage/jpeg7299https://repositorio.ufscar.br/bitstreams/bce8c685-197d-451b-a90f-97171e8b3c12/download16612f76a5d3497b0026c4d700e3d015MD52falseAnonymousREAD20.500.14289/39972025-02-05 15:34:28.352open.accessoai:repositorio.ufscar.br:20.500.14289/3997https://repositorio.ufscar.brRepositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestrepositorio.sibi@ufscar.bropendoar:43222025-02-05T18:34:28Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false
dc.title.por.fl_str_mv Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO
title Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO
spellingShingle Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO
Silva, Edilene Deise da
Catálise
Zeólita FAU
Redução de NO
ENGENHARIAS::ENGENHARIA QUIMICA
title_short Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO
title_full Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO
title_fullStr Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO
title_full_unstemmed Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO
title_sort Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO
author Silva, Edilene Deise da
author_facet Silva, Edilene Deise da
author_role author
dc.contributor.authorlattes.por.fl_str_mv http://lattes.cnpq.br/3672771633840838
dc.contributor.author.fl_str_mv Silva, Edilene Deise da
dc.contributor.advisor1.fl_str_mv Urquieta-González, Ernesto Antonio
dc.contributor.referee1Lattes.fl_str_mv http://lattes.cnpq.br/2389975677904655
dc.contributor.authorID.fl_str_mv e6ca62ac-31f3-472c-bd8d-6f2191b5bfa8
contributor_str_mv Urquieta-González, Ernesto Antonio
dc.subject.por.fl_str_mv Catálise
Zeólita FAU
Redução de NO
topic Catálise
Zeólita FAU
Redução de NO
ENGENHARIAS::ENGENHARIA QUIMICA
dc.subject.cnpq.fl_str_mv ENGENHARIAS::ENGENHARIA QUIMICA
description The emissions of the nitrogen oxides (NOx) must be hardly reduced in the next years. The catalytic reduction of NO with CO is one of the possible processes with potential to be able to transform those oxides in N2. In that process, supported noble metals have been the most used, however, their low stability in the presence of water steam or SO2, have led to develop studies to overcome those limitations. Perovkites type catalysts or transition metal oxides supported in a variety of support show activity in this reaction. Nevertheless, no adequate information about the activity of metal oxides supported on zeolites is found in the literature. In this context, the present work was focused to prepare and evaluate between 150°C and 500°C, Cu, Co or Fe containing catalysts dispersed on USY (Si/Al=3,4) or ZSM-5 (Si/Al=12,8) zeolites in the reduction of NO with CO and in the oxidation of CO to CO2. The oxide activity was also compared with that of the respective metal cations located in charge compensation sites. The catalysts were prepared by ion exchange or impregnation and characterized by AAS, XRD, DRS-UV and H2-TPR. Conversion data of NO to N2 on USY and ZSM-5 zeolites containing predominantly Cu2+ or Co2+ cations in exchangeable sites were more active when located on ZSM-5 zeolite (MFI structure), with the Cu2+ cations being more active. On the other hand, Cu, Co or Fe oxides supported on USY or ZSM-5 were more active than cations of considered metals in exchangeable sites, with conversion being dependent on the type and metal content and the type of zeolite. Among the studied metal oxides, the Fe one was the most active and selective. However the presence of O2 or water steam in the feed inhibited the NO reduction with CO on Fe oxide, which was attributed to the deactivation of the active sites by the water steam and the CO direct oxidation by O2 occurring preferentially than CO oxidation via NO reduction. This result gives evidence of the water steam leads to the deactivation of the metallic active sites and O2 favors the direct oxidation of CO to CO2 in detriment of its oxidation by NO reduction. The NO conversion was not significantly affected by the presence of SO2 in the feed (40 ppm).
publishDate 2008
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2016-06-02T19:56:31Z
dc.date.issued.fl_str_mv 2008-04-08
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identifier_str_mv SILVA, Edilene Deise da. Catalisadores à base de Cu, Co ou Fe trocados ou suportados em zeólita USY avaliação na redução de NO com CO. 2008. 125 f. Dissertação (Mestrado em Ciências Exatas e da Terra) - Universidade Federal de São Carlos, São Carlos, 2008.
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