Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese
Autor(a) principal: | |
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Data de Publicação: | 2016 |
Tipo de documento: | Dissertação |
Idioma: | por |
Título da fonte: | Repositório Institucional da UFSCAR |
Texto Completo: | https://repositorio.ufscar.br/handle/ufscar/8769 |
Resumo: | Dry reforming of methane (DRM) is a promising process in syngas generation with low molar H2/CO ratio. Syngas production is of great interest for many processes, such as obtaining liquid fuels by Fischer-Tropsch. The main problem in DRM is the large formation of carbon depositions over the catalyst. Catalyst with pyrochlore structure, A2B2O7, presents uniform distribution of active metals into the lattice, resulting in a dispersed metal with good interaction with surface, reducing metal sintering and deactivation by carbon deposition. In this work, Zr was partially substituted by Ni, Co and Ru on the B site of La2Zr2O7 and Ni was added on the B site of La2Ce2O7 and La2Sn2O7. All the catalysts were prepared by a modified Pechini method. These catalysts were characterized by X-ray diffraction, temperature programmed reduction with H2, fluorescence X-ray, thermogravimetric analysis and scanning electron microscopy coupled to energy dispersive spectroscopic. The catalytic activity was tested in temperatures from 500 to 800°C, at intervals of 50°C. The catalysts containing Ce and Sn in the B site were not active in the dry reforming of methane, neither the catalyst containing Co and Zr in the B site. During stability runs, it was observed that LaZrNi was not stable, presenting rapid deactivation. The containing Ru catalysts were most active that the Ni ones. The results in this study indicate that oxides with pyrochlore structure are promising to catalyze dry (CO2) reforming of methane, they proved to be active even with Ni and Ru content very low at the catalyst surface. |
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Ramon, Adriana PaulaAssaf, José Mansurhttp://lattes.cnpq.br/9563312407691130http://lattes.cnpq.br/663873296438511291279b5f-9223-4c7d-baf6-8161ec0df4b52017-05-23T19:27:31Z2017-05-23T19:27:31Z2016-03-31RAMON, Adriana Paula. Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese. 2016. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2016. Disponível em: https://repositorio.ufscar.br/handle/ufscar/8769.https://repositorio.ufscar.br/handle/ufscar/8769Dry reforming of methane (DRM) is a promising process in syngas generation with low molar H2/CO ratio. Syngas production is of great interest for many processes, such as obtaining liquid fuels by Fischer-Tropsch. The main problem in DRM is the large formation of carbon depositions over the catalyst. Catalyst with pyrochlore structure, A2B2O7, presents uniform distribution of active metals into the lattice, resulting in a dispersed metal with good interaction with surface, reducing metal sintering and deactivation by carbon deposition. In this work, Zr was partially substituted by Ni, Co and Ru on the B site of La2Zr2O7 and Ni was added on the B site of La2Ce2O7 and La2Sn2O7. All the catalysts were prepared by a modified Pechini method. These catalysts were characterized by X-ray diffraction, temperature programmed reduction with H2, fluorescence X-ray, thermogravimetric analysis and scanning electron microscopy coupled to energy dispersive spectroscopic. The catalytic activity was tested in temperatures from 500 to 800°C, at intervals of 50°C. The catalysts containing Ce and Sn in the B site were not active in the dry reforming of methane, neither the catalyst containing Co and Zr in the B site. During stability runs, it was observed that LaZrNi was not stable, presenting rapid deactivation. The containing Ru catalysts were most active that the Ni ones. The results in this study indicate that oxides with pyrochlore structure are promising to catalyze dry (CO2) reforming of methane, they proved to be active even with Ni and Ru content very low at the catalyst surface.A reforma seca do metano (RSM) é um processo promissor na geração de gás de síntese com baixas razões molares entre H2 e CO. O gás de síntese apresenta grande interesse industrial em diversos processos, como na obtenção de combustíveis líquidos por Fischer-Tropsch. O maior problema da RSM é a grande formação de depósitos de carbono sobre o catalisador. Catalisadores do tipo pirocloro, A2B2O7, apresentam distribuição uniforme dos metais ativos na estrutura cristalina, o que resulta em um metal disperso ligado na estrutura cristalina, reduzindo a sinterização do metal e também a desativação por deposição de carbono. Neste trabalho foram sintetizados catalisadores La2Zr2O7 com substituição parcial de Zr por Ni, Co e Ru, e catalisadores La2Ce2O7 e La2Sn2O7 com substituição parcial de Ce e Sn, respectivamente, por Ni através do método de Pechini modificado. Esses foram caracterizados por difração de raios X, redução a temperatura programada com H2, fluorescência de raios X, análise termogravimétrica e microscopia eletrônica de varredura acoplada a espectroscopia dispersiva de raios X. A atividade catalítica dos materiais foi testada em temperaturas entre 500 a 800°C, em intervalos de 50°C. Os catalisadores contendo Ce e Sn no sítio B não se mostraram ativos na reação de reforma seca do metano, assim como o catalisador contendo Co e Zr no sítio B. Durante o teste de estabilidade observou-se que o catalisador LaZrNi desativou-se rapidamente. O catalisador contendo Ru foi sempre mais ativo que os contendo Ni como metal ativo. Os resultados obtidos neste trabalho indicam que estruturas óxidas do tipo pirocloro são promissoras para catalisar reações de reforma de metano com CO2, pois mostraram-se ativas mesmo com teores de Ni e Ru na superfície muito baixos.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)porUniversidade Federal de São CarlosCâmpus São CarlosPrograma de Pós-Graduação em Engenharia Química - PPGEQUFSCarSínteseCatalisadoresProdução de gásENGENHARIAS::ENGENHARIA QUIMICASíntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de sínteseinfo: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:UFSCARORIGINALDissAPR.pdfDissAPR.pdfapplication/pdf4828740https://repositorio.ufscar.br/bitstream/ufscar/8769/1/DissAPR.pdf6ac3a929eaf1ea3cdc41065c4ccd0cc5MD51LICENSElicense.txtlicense.txttext/plain; charset=utf-81957https://repositorio.ufscar.br/bitstream/ufscar/8769/2/license.txtae0398b6f8b235e40ad82cba6c50031dMD52TEXTDissAPR.pdf.txtDissAPR.pdf.txtExtracted texttext/plain111269https://repositorio.ufscar.br/bitstream/ufscar/8769/3/DissAPR.pdf.txtddb91fdac9c09fa60f97638d458b9055MD53THUMBNAILDissAPR.pdf.jpgDissAPR.pdf.jpgIM Thumbnailimage/jpeg5943https://repositorio.ufscar.br/bitstream/ufscar/8769/4/DissAPR.pdf.jpg305653d426bf5624253cb02ea30764e5MD54ufscar/87692023-09-18 18:31:24.095oai:repositorio.ufscar.br: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Repositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestopendoar:43222023-09-18T18:31:24Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false |
dc.title.por.fl_str_mv |
Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese |
title |
Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese |
spellingShingle |
Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese Ramon, Adriana Paula Síntese Catalisadores Produção de gás ENGENHARIAS::ENGENHARIA QUIMICA |
title_short |
Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese |
title_full |
Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese |
title_fullStr |
Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese |
title_full_unstemmed |
Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese |
title_sort |
Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese |
author |
Ramon, Adriana Paula |
author_facet |
Ramon, Adriana Paula |
author_role |
author |
dc.contributor.authorlattes.por.fl_str_mv |
http://lattes.cnpq.br/6638732964385112 |
dc.contributor.author.fl_str_mv |
Ramon, Adriana Paula |
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 |
91279b5f-9223-4c7d-baf6-8161ec0df4b5 |
contributor_str_mv |
Assaf, José Mansur |
dc.subject.por.fl_str_mv |
Síntese Catalisadores Produção de gás |
topic |
Síntese Catalisadores Produção de gás ENGENHARIAS::ENGENHARIA QUIMICA |
dc.subject.cnpq.fl_str_mv |
ENGENHARIAS::ENGENHARIA QUIMICA |
description |
Dry reforming of methane (DRM) is a promising process in syngas generation with low molar H2/CO ratio. Syngas production is of great interest for many processes, such as obtaining liquid fuels by Fischer-Tropsch. The main problem in DRM is the large formation of carbon depositions over the catalyst. Catalyst with pyrochlore structure, A2B2O7, presents uniform distribution of active metals into the lattice, resulting in a dispersed metal with good interaction with surface, reducing metal sintering and deactivation by carbon deposition. In this work, Zr was partially substituted by Ni, Co and Ru on the B site of La2Zr2O7 and Ni was added on the B site of La2Ce2O7 and La2Sn2O7. All the catalysts were prepared by a modified Pechini method. These catalysts were characterized by X-ray diffraction, temperature programmed reduction with H2, fluorescence X-ray, thermogravimetric analysis and scanning electron microscopy coupled to energy dispersive spectroscopic. The catalytic activity was tested in temperatures from 500 to 800°C, at intervals of 50°C. The catalysts containing Ce and Sn in the B site were not active in the dry reforming of methane, neither the catalyst containing Co and Zr in the B site. During stability runs, it was observed that LaZrNi was not stable, presenting rapid deactivation. The containing Ru catalysts were most active that the Ni ones. The results in this study indicate that oxides with pyrochlore structure are promising to catalyze dry (CO2) reforming of methane, they proved to be active even with Ni and Ru content very low at the catalyst surface. |
publishDate |
2016 |
dc.date.issued.fl_str_mv |
2016-03-31 |
dc.date.accessioned.fl_str_mv |
2017-05-23T19:27:31Z |
dc.date.available.fl_str_mv |
2017-05-23T19:27:31Z |
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 |
RAMON, Adriana Paula. Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese. 2016. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2016. Disponível em: https://repositorio.ufscar.br/handle/ufscar/8769. |
dc.identifier.uri.fl_str_mv |
https://repositorio.ufscar.br/handle/ufscar/8769 |
identifier_str_mv |
RAMON, Adriana Paula. Síntese e desempenho de catalisadores com estrutura do tipo pirocloro para produção de gás de síntese. 2016. Dissertação (Mestrado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2016. Disponível em: https://repositorio.ufscar.br/handle/ufscar/8769. |
url |
https://repositorio.ufscar.br/handle/ufscar/8769 |
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por |
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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 |
dc.publisher.program.fl_str_mv |
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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