Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo

Detalhes bibliográficos
Ano de defesa: 2015
Autor(a) principal: Araújo, Camila Pacelly Brandão de
Orientador(a): Não Informado pela instituição
Banca de defesa: Não Informado pela instituição
Tipo de documento: Dissertação
Tipo de acesso: Acesso aberto
Idioma: por
Instituição de defesa: Universidade Federal do Rio Grande do Norte
Brasil
UFRN
PÓS-GRADUAÇÃO EM ENGENHARIA QUÍMICA
Programa de Pós-Graduação: Não Informado pela instituição
Departamento: Não Informado pela instituição
País: Não Informado pela instituição
Palavras-chave em Português:
Link de acesso: https://repositorio.ufrn.br/jspui/handle/123456789/19690
Resumo: Sulfur compounds emissions have been, on the late years, subject to more severe environmental laws due to its impact on the environment (causing the acid rain phenomena) and on human health. It has also been object of much attention from the refiners worldwide due to its relationship with equipment’s life, which is decreased by corrosion, and also with products’ quality, as the later may have its color, smell and stability altered by the presence of such compounds. Sulfur removal can be carried out by hydrotreating (HDT) which is a catalytic process. Catalysts for HDS are traditionally based on Co(Ni)-Mo(W)/Al2O3. However, in face of the increased contaminants’ content on crude oil, and stricter legislation on emissions, the development of new, more active and efficient catalysts is pressing. Carbides of refractory material have been identified as potential materials for this use. The addition of a second metal to carbides may enhance catalytic activities by increasing the density of active sites. In the present thesis Mo2C with Co addition was produced in a fixed bed reactor via gas-solid reaction of CH4 (5%) and H2(95%) with a precursor made of a mix of ammonium heptamolybdate [(NH4)6[Mo7O24].4H2O] and cobalt nitrate[Co(NO3)2.6H2O] at stoichiometric amounts. Precursors’ where analyzed by XRF, XRD, SEM and TG/DTA. Carboreduction reactions were carried out at 700 and 750°C with two cobalt compositions (2,5 and 5%). Reaction’s products were characterized by XRF, XRD, SEM, TOC, BET and laser granulometry. It was possible to obtain Mo2C with 2,5 and 5% cobalt addition as a single phase at 750°C with nanoscale crystallite sizes. At 700°C, however, both MoO2 and Mo2C phases were found by XRD. No Co containing phases were found by XRD. XRF, however, confirmed the intended Co content added. SEM images confirmed XRD data. The increase on Co content promoted a more severe agglomeration of the produced powder. The same effect was noted when the reaction temperature was increased. The powder synthesized at 750°C with 2,5% Co addition TOC analysis indicated the complete conversion from oxide material to carbide, with a 8,9% free carbon production. The powder produced at this temperature with 5% Co addition was only partially converted (86%)
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spelling Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixoCarbeto de molibdênioCobaltoReator de leito fixoDopagemCNPQ::ENGENHARIAS::ENGENHARIA QUIMICASulfur compounds emissions have been, on the late years, subject to more severe environmental laws due to its impact on the environment (causing the acid rain phenomena) and on human health. It has also been object of much attention from the refiners worldwide due to its relationship with equipment’s life, which is decreased by corrosion, and also with products’ quality, as the later may have its color, smell and stability altered by the presence of such compounds. Sulfur removal can be carried out by hydrotreating (HDT) which is a catalytic process. Catalysts for HDS are traditionally based on Co(Ni)-Mo(W)/Al2O3. However, in face of the increased contaminants’ content on crude oil, and stricter legislation on emissions, the development of new, more active and efficient catalysts is pressing. Carbides of refractory material have been identified as potential materials for this use. The addition of a second metal to carbides may enhance catalytic activities by increasing the density of active sites. In the present thesis Mo2C with Co addition was produced in a fixed bed reactor via gas-solid reaction of CH4 (5%) and H2(95%) with a precursor made of a mix of ammonium heptamolybdate [(NH4)6[Mo7O24].4H2O] and cobalt nitrate[Co(NO3)2.6H2O] at stoichiometric amounts. Precursors’ where analyzed by XRF, XRD, SEM and TG/DTA. Carboreduction reactions were carried out at 700 and 750°C with two cobalt compositions (2,5 and 5%). Reaction’s products were characterized by XRF, XRD, SEM, TOC, BET and laser granulometry. It was possible to obtain Mo2C with 2,5 and 5% cobalt addition as a single phase at 750°C with nanoscale crystallite sizes. At 700°C, however, both MoO2 and Mo2C phases were found by XRD. No Co containing phases were found by XRD. XRF, however, confirmed the intended Co content added. SEM images confirmed XRD data. The increase on Co content promoted a more severe agglomeration of the produced powder. The same effect was noted when the reaction temperature was increased. The powder synthesized at 750°C with 2,5% Co addition TOC analysis indicated the complete conversion from oxide material to carbide, with a 8,9% free carbon production. The powder produced at this temperature with 5% Co addition was only partially converted (86%)Conselho Nacional de Desenvolvimento Científico e Tecnológico - CNPqAs emissões de compostos sulfurados pela indústria do refino de petróleo vêm sendo sujeitas a legislações cada vez mais restritivas devido aos impactos ambientais e na saúde humana. A remoção de compostos de enxofre pode ocorrer através de reações de hidrotratamento (HDT) as quais são catalisadas por sólidos, geralmente óxidos ou sulfetos metálicos normalmente suportados em alumina. Para a remoção de enxofre (HDS) catalisadores de Co(Ni)-Mo(W)/Al2O3 são os mais utilizados, porém novos materiais vem sendo desenvolvidos para esse fim. Carbetos de metais refratários foram identificados como potenciais candidatos para essa aplicação, a dopagem destes pode ser uma alternativa para a catálise dessa reação. Os precursores para obtenção de Mo2C foram heptamolibdato de molibdênio [(NH4)6[Mo7O24].4H2O] e nitrato de cobalto [Co(NO3)2.6H2O] e foram cominuídos manualmente em proporções estequiométricas anteriormente à reação. Os precursores foram caracterizados por TG/DTA, MEV, FRX e DRX. Os carbetos de molibdênio com adição de cobalto foram obtidos através de reação gás-sólido com atmosfera de metano (CH4) e hidrogênio (H2) utilizando reator de leito fixo. Foi utilizada vazão total da mistura gasosa de 15L/h com 5% de CH4 e taxa de aquecimento de 5°C/min até a temperatura de reação (700 ou 750°C). Dois percentuais de cobalto foram empregados: 2,5 e 5%. Foi notada a presença de fase CoMoO4 e MoO3 nos percursores calcinados, o que indica o íntimo contato entre os metais. Para os produtos da reação de carbonetação a 700°C, independentemente do teor de cobalto adicionado, foi formado Mo2C-ortorrômbica e MoO2- monoclínica. A 750°C somente Mo2C foi detectada por DRX. Não foi possível a identificação de fase contendo Co pelos difratogramas em nenhuma das condições. Nessa temperatura, a análise de TOC indicou a completa conversão dos óxidos a carbeto, com formação de 8,9% de carbono livre para a amostra com 2,5% de Co, para a amostra com 5% a conversão foi incompleta (86%). Os produtos de reação foram caracterizados por FRX, DRX, MEV, TOC, BET e granulometria a laserUniversidade Federal do Rio Grande do NorteBrasilUFRNPÓS-GRADUAÇÃO EM ENGENHARIA QUÍMICASouza, Carlson Pereira dehttp://lattes.cnpq.br/4474516366734941http://lattes.cnpq.br/1030834608582624Fontes, Francisco de Assis Oliveirahttp://lattes.cnpq.br/9043538628554844Silva, Gilson Garcia dahttp://lattes.cnpq.br/8681275097040450Araújo, Camila Pacelly Brandão de2016-01-29T17:12:23Z2016-01-29T17:12:23Z2015-01-30info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisapplication/pdfARAÚJO, Camila Pacelly Brandão de. Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo. 2015. 87f. Dissertação (Mestrado em Engenharia Química) - Centro de Tecnologia, Universidade Federal do Rio Grande do Norte, Natal, 2015.https://repositorio.ufrn.br/jspui/handle/123456789/19690porinfo:eu-repo/semantics/openAccessreponame:Repositório Institucional da UFRNinstname:Universidade Federal do Rio Grande do Norte (UFRN)instacron:UFRN2017-11-02T15:11:48Zoai:repositorio.ufrn.br:123456789/19690Repositório InstitucionalPUBhttp://repositorio.ufrn.br/oai/repositorio@bczm.ufrn.bropendoar:2017-11-02T15:11:48Repositório Institucional da UFRN - Universidade Federal do Rio Grande do Norte (UFRN)false
dc.title.none.fl_str_mv Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo
title Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo
spellingShingle Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo
Araújo, Camila Pacelly Brandão de
Carbeto de molibdênio
Cobalto
Reator de leito fixo
Dopagem
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
title_short Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo
title_full Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo
title_fullStr Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo
title_full_unstemmed Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo
title_sort Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo
author Araújo, Camila Pacelly Brandão de
author_facet Araújo, Camila Pacelly Brandão de
author_role author
dc.contributor.none.fl_str_mv Souza, Carlson Pereira de

http://lattes.cnpq.br/4474516366734941

http://lattes.cnpq.br/1030834608582624
Fontes, Francisco de Assis Oliveira

http://lattes.cnpq.br/9043538628554844
Silva, Gilson Garcia da

http://lattes.cnpq.br/8681275097040450
dc.contributor.author.fl_str_mv Araújo, Camila Pacelly Brandão de
dc.subject.por.fl_str_mv Carbeto de molibdênio
Cobalto
Reator de leito fixo
Dopagem
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
topic Carbeto de molibdênio
Cobalto
Reator de leito fixo
Dopagem
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
description Sulfur compounds emissions have been, on the late years, subject to more severe environmental laws due to its impact on the environment (causing the acid rain phenomena) and on human health. It has also been object of much attention from the refiners worldwide due to its relationship with equipment’s life, which is decreased by corrosion, and also with products’ quality, as the later may have its color, smell and stability altered by the presence of such compounds. Sulfur removal can be carried out by hydrotreating (HDT) which is a catalytic process. Catalysts for HDS are traditionally based on Co(Ni)-Mo(W)/Al2O3. However, in face of the increased contaminants’ content on crude oil, and stricter legislation on emissions, the development of new, more active and efficient catalysts is pressing. Carbides of refractory material have been identified as potential materials for this use. The addition of a second metal to carbides may enhance catalytic activities by increasing the density of active sites. In the present thesis Mo2C with Co addition was produced in a fixed bed reactor via gas-solid reaction of CH4 (5%) and H2(95%) with a precursor made of a mix of ammonium heptamolybdate [(NH4)6[Mo7O24].4H2O] and cobalt nitrate[Co(NO3)2.6H2O] at stoichiometric amounts. Precursors’ where analyzed by XRF, XRD, SEM and TG/DTA. Carboreduction reactions were carried out at 700 and 750°C with two cobalt compositions (2,5 and 5%). Reaction’s products were characterized by XRF, XRD, SEM, TOC, BET and laser granulometry. It was possible to obtain Mo2C with 2,5 and 5% cobalt addition as a single phase at 750°C with nanoscale crystallite sizes. At 700°C, however, both MoO2 and Mo2C phases were found by XRD. No Co containing phases were found by XRD. XRF, however, confirmed the intended Co content added. SEM images confirmed XRD data. The increase on Co content promoted a more severe agglomeration of the produced powder. The same effect was noted when the reaction temperature was increased. The powder synthesized at 750°C with 2,5% Co addition TOC analysis indicated the complete conversion from oxide material to carbide, with a 8,9% free carbon production. The powder produced at this temperature with 5% Co addition was only partially converted (86%)
publishDate 2015
dc.date.none.fl_str_mv 2015-01-30
2016-01-29T17:12:23Z
2016-01-29T17:12:23Z
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.uri.fl_str_mv ARAÚJO, Camila Pacelly Brandão de. Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo. 2015. 87f. Dissertação (Mestrado em Engenharia Química) - Centro de Tecnologia, Universidade Federal do Rio Grande do Norte, Natal, 2015.
https://repositorio.ufrn.br/jspui/handle/123456789/19690
identifier_str_mv ARAÚJO, Camila Pacelly Brandão de. Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo. 2015. 87f. Dissertação (Mestrado em Engenharia Química) - Centro de Tecnologia, Universidade Federal do Rio Grande do Norte, Natal, 2015.
url https://repositorio.ufrn.br/jspui/handle/123456789/19690
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language por
dc.rights.driver.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Universidade Federal do Rio Grande do Norte
Brasil
UFRN
PÓS-GRADUAÇÃO EM ENGENHARIA QUÍMICA
publisher.none.fl_str_mv Universidade Federal do Rio Grande do Norte
Brasil
UFRN
PÓS-GRADUAÇÃO EM ENGENHARIA QUÍMICA
dc.source.none.fl_str_mv reponame:Repositório Institucional da UFRN
instname:Universidade Federal do Rio Grande do Norte (UFRN)
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instname_str Universidade Federal do Rio Grande do Norte (UFRN)
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reponame_str Repositório Institucional da UFRN
collection Repositório Institucional da UFRN
repository.name.fl_str_mv Repositório Institucional da UFRN - Universidade Federal do Rio Grande do Norte (UFRN)
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