Obtenção de Mo2C com adição de Co por reação gás-sólido em reator de leito fixo
| Ano de defesa: | 2015 |
|---|---|
| Autor(a) principal: | |
| Orientador(a): | |
| Banca de defesa: | |
| 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%) |
| id |
UFRN_0c4dd0f6cb67b1ed8607de5fbaad839b |
|---|---|
| oai_identifier_str |
oai:repositorio.ufrn.br:123456789/19690 |
| network_acronym_str |
UFRN |
| network_name_str |
Repositório Institucional da UFRN |
| repository_id_str |
|
| 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 |
| dc.language.iso.fl_str_mv |
por |
| 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) instacron:UFRN |
| instname_str |
Universidade Federal do Rio Grande do Norte (UFRN) |
| instacron_str |
UFRN |
| institution |
UFRN |
| 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) |
| repository.mail.fl_str_mv |
repositorio@bczm.ufrn.br |
| _version_ |
1855758814043701248 |