Precursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano.
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Data de Publicação: | 2016 |
Tipo de documento: | Trabalho de conclusão de curso |
Idioma: | por |
Título da fonte: | Repositório Institucional da UFRN |
Texto Completo: | https://repositorio.ufrn.br/handle/123456789/38348 |
Resumo: | The energy generation in the face of growing energy demand is a challenge to maintain the social welfare, especially if we take into account the strong presence of oil in the energy matrix. Added to this, there is the link between oil and climate changes due to carbon dioxide (CO2) emissions. In an attempt to cease such problems, hydrogen (H2) stands out as an energy source due to its high conversion and efficiency. With the increase of environmental awareness, the Methane Dry Reforming, MDR, is highlighted due to the use of CO2 in synthesis gas generation (H2 and CO). Nickel catalysts are widely studied because of its low cost and stability. As a catalyst, nickel can be obtained from the perovskite LaNiO3 because of perovskite’s good stability. Perovskite compounds have low surface area, limiting their use. The use of supports with high surface area, such as MCM-41, increases the surface area of the catalyst. One of the problems in supporting perovskites on MCM-41 is the high temperature required to form them, which would destabilize the MCM-41 structure. The present work aims to put together MCM-41 and perovskite proprieties preparing LaNiO3 and La2NiO4 in situ by wet impregnation as precursors of Ni0/La2O3 supported on MCM-41. The calcination temperature (700°C) was chosen because it was intermediate to that of perovskite formation and destabilization of the MCM-41 structure. The XRD results show a mixture of NiO, La2O3, LaNiO3 and La2NiO4, whereas the post-TPR XRD show Ni0 and La2O3. MDR results in fixed-bed reactor show CH4 and CO2 conversion rates around 88.8 and 88.1%, respectively, for a ten-hour analysis, as well as H2/CO> 1 ratio, indicating good results for hydrogen generation. |
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Agostinho, Lenilton VidalRodolfo Luiz Bezerra de Araújo MedeirosVitor Sobrinho, EledirMelo, Dulce Maria de Araújo2017-01-30T12:13:56Z2021-09-27T11:47:57Z2017-01-30T12:13:56Z2021-09-27T11:47:57Z2016-12-162011024354ABBAS, H.F.; WAN DAUD, W.M.A. Hydrogen production by methane decomposition: A review. International Journal of Hydrogen Energy, v. 35, p. 1160–1190, 2010. http://dx.doi.org/10.1016/j.ijhydene.2009.11.036 Agência Nacional do Petróleo, Gás Natural e Biocombustíveis – ANP. Anuário estatístico brasileiro do petróleo, gás natural e biocombustíveis: 2015. Disponível em: <http://www.anp.gov.br/?dw=78135> Acesso em: 29 de agosto de 2016. ALIPOUR, Z.; REZAEI, M.; MESHKANI, F. Effect of alkaline earth promoters (MgO, CaO, and BaO) on the activity and coke formation of Ni catalysts supported on nanocrystalline Al2O3 in dry reforming of methane. 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Added to this, there is the link between oil and climate changes due to carbon dioxide (CO2) emissions. In an attempt to cease such problems, hydrogen (H2) stands out as an energy source due to its high conversion and efficiency. With the increase of environmental awareness, the Methane Dry Reforming, MDR, is highlighted due to the use of CO2 in synthesis gas generation (H2 and CO). Nickel catalysts are widely studied because of its low cost and stability. As a catalyst, nickel can be obtained from the perovskite LaNiO3 because of perovskite’s good stability. Perovskite compounds have low surface area, limiting their use. The use of supports with high surface area, such as MCM-41, increases the surface area of the catalyst. One of the problems in supporting perovskites on MCM-41 is the high temperature required to form them, which would destabilize the MCM-41 structure. The present work aims to put together MCM-41 and perovskite proprieties preparing LaNiO3 and La2NiO4 in situ by wet impregnation as precursors of Ni0/La2O3 supported on MCM-41. The calcination temperature (700°C) was chosen because it was intermediate to that of perovskite formation and destabilization of the MCM-41 structure. The XRD results show a mixture of NiO, La2O3, LaNiO3 and La2NiO4, whereas the post-TPR XRD show Ni0 and La2O3. MDR results in fixed-bed reactor show CH4 and CO2 conversion rates around 88.8 and 88.1%, respectively, for a ten-hour analysis, as well as H2/CO> 1 ratio, indicating good results for hydrogen generation.A geração de energia frente ao crescimento da demanda energética é um desafio para manutenção do bem-estar social, principalmente se levarmos em conta a forte presença do petróleo na matriz energética. Soma-se a isso, a ligação entre petróleo e mudanças climáticas devido às emissões de dióxido de carbono (CO2). Na tentativa de driblar tais problemas, o hidrogênio (H2) se destaca como fonte de energia devido à sua alta conversão e eficiência. Com a conscientização ambiental, a Reforma a Seco do Metano, RSM, ganha destaque devido à utilização de CO2 na geração de gás de síntese (H2 e CO). Catalisadores de níquel são largamente estudados devido ao baixo custo e estabilidade. Como catalisador, o níquel, Ni, pode ser obtido a partir da perovskita LaNiO3 em função de sua boa estabilidade. Tal composto tem uma baixa área superficial, limitando sua utilização. A utilização de suportes com alta área superficial, como o MCM-41, aumenta a área superficial do catalisador. Um dos problemas em suportar perovskitas em MCM-41 é a alta temperatura requerida na formação das mesmas, o que desestabilizaria a estrutura do MCM-41. O presente trabalho objetiva unir propriedades do MCM-41 e da perovskita, preparando LaNiO3 e La2NiO4 in situ por impregnação úmida como precursores de Ni0/La2O3 suportados em MCM-41. A temperatura de calcinação (700ºC) foi escolhida por ser intermediária à de formação das perovskitas e destruição da desestabilização do MCM-41. Os resultados de DRX mostram uma mistura de NiO, La2O3, LaNiO3 e La2NiO4, enquanto que os pós-RTP mostram Ni0 e La2O3. Os resultados de RSM realizados em reator de leito fixo mostram taxas de conversão de CH4 e CO2 em torno de 88,8 e 88,1%, respectivamente, para 10 horas de reação, além de razão H2/CO > 1, indicando bons resultados para a produção de hidrogênio.Universidade Federal do Rio Grande do NorteUFRNBrasilQuímica do PetróleoHidrogênio.MCM-41.Perovskita.Reforma a Seco do Metano.Methane Dry Reforming.Hydrogen.CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICAPrecursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano.info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/bachelorThesisinfo:eu-repo/semantics/openAccessporreponame:Repositório Institucional da UFRNinstname:Universidade Federal do Rio Grande do Norte (UFRN)instacron:UFRNTEXTPrecursoresLaNiO3-La2NiO4_Agostinho_2016.pdf.txtExtracted texttext/plain85755https://repositorio.ufrn.br/bitstream/123456789/38348/1/PrecursoresLaNiO3-La2NiO4_Agostinho_2016.pdf.txte4939b8b4c5a102597fc027155b2c505MD51LICENSElicense.txttext/plain756https://repositorio.ufrn.br/bitstream/123456789/38348/2/license.txta80a9cda2756d355b388cc443c3d8a43MD52ORIGINALPrecursoresLaNiO3-La2NiO4_Agostinho_2016.pdfapplication/pdf1496879https://repositorio.ufrn.br/bitstream/123456789/38348/3/PrecursoresLaNiO3-La2NiO4_Agostinho_2016.pdf1776b87810eb3b301bf7f32283f9d389MD53123456789/383482023-05-12 13:46:06.71oai:https://repositorio.ufrn.br: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ório de PublicaçõesPUBhttp://repositorio.ufrn.br/oai/opendoar:2023-05-12T16:46:06Repositório Institucional da UFRN - Universidade Federal do Rio Grande do Norte (UFRN)false |
dc.title.pr_BR.fl_str_mv |
Precursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano. |
title |
Precursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano. |
spellingShingle |
Precursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano. Agostinho, Lenilton Vidal Hidrogênio. MCM-41. Perovskita. Reforma a Seco do Metano. Methane Dry Reforming. Hydrogen. CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
title_short |
Precursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano. |
title_full |
Precursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano. |
title_fullStr |
Precursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano. |
title_full_unstemmed |
Precursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano. |
title_sort |
Precursores LaNiO3/La2NiO4 suportados em MCM-41 para obtenção de hidrogênio a partir da reforma a seco do metano. |
author |
Agostinho, Lenilton Vidal |
author_facet |
Agostinho, Lenilton Vidal |
author_role |
author |
dc.contributor.referees1.none.fl_str_mv |
Vitor Sobrinho, Eledir |
dc.contributor.author.fl_str_mv |
Agostinho, Lenilton Vidal |
dc.contributor.advisor-co1.fl_str_mv |
Rodolfo Luiz Bezerra de Araújo Medeiros |
dc.contributor.advisor1.fl_str_mv |
Melo, Dulce Maria de Araújo |
contributor_str_mv |
Rodolfo Luiz Bezerra de Araújo Medeiros Melo, Dulce Maria de Araújo |
dc.subject.pr_BR.fl_str_mv |
Hidrogênio. MCM-41. Perovskita. Reforma a Seco do Metano. Methane Dry Reforming. Hydrogen. |
topic |
Hidrogênio. MCM-41. Perovskita. Reforma a Seco do Metano. Methane Dry Reforming. Hydrogen. CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
dc.subject.cnpq.fl_str_mv |
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
description |
The energy generation in the face of growing energy demand is a challenge to maintain the social welfare, especially if we take into account the strong presence of oil in the energy matrix. Added to this, there is the link between oil and climate changes due to carbon dioxide (CO2) emissions. In an attempt to cease such problems, hydrogen (H2) stands out as an energy source due to its high conversion and efficiency. With the increase of environmental awareness, the Methane Dry Reforming, MDR, is highlighted due to the use of CO2 in synthesis gas generation (H2 and CO). Nickel catalysts are widely studied because of its low cost and stability. As a catalyst, nickel can be obtained from the perovskite LaNiO3 because of perovskite’s good stability. Perovskite compounds have low surface area, limiting their use. The use of supports with high surface area, such as MCM-41, increases the surface area of the catalyst. One of the problems in supporting perovskites on MCM-41 is the high temperature required to form them, which would destabilize the MCM-41 structure. The present work aims to put together MCM-41 and perovskite proprieties preparing LaNiO3 and La2NiO4 in situ by wet impregnation as precursors of Ni0/La2O3 supported on MCM-41. The calcination temperature (700°C) was chosen because it was intermediate to that of perovskite formation and destabilization of the MCM-41 structure. The XRD results show a mixture of NiO, La2O3, LaNiO3 and La2NiO4, whereas the post-TPR XRD show Ni0 and La2O3. MDR results in fixed-bed reactor show CH4 and CO2 conversion rates around 88.8 and 88.1%, respectively, for a ten-hour analysis, as well as H2/CO> 1 ratio, indicating good results for hydrogen generation. |
publishDate |
2016 |
dc.date.issued.fl_str_mv |
2016-12-16 |
dc.date.accessioned.fl_str_mv |
2017-01-30T12:13:56Z 2021-09-27T11:47:57Z |
dc.date.available.fl_str_mv |
2017-01-30T12:13:56Z 2021-09-27T11:47:57Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/bachelorThesis |
format |
bachelorThesis |
status_str |
publishedVersion |
dc.identifier.pr_BR.fl_str_mv |
2011024354 |
dc.identifier.citation.fl_str_mv |
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Catalysis Today, v. 107-108, p. 785-791, 2005. http://dx.doi.org/10.1016/j.cattod.2005.07.010 VALDERRAMA, G.; KIENNEMANN, A.; GOLDWASSER, M.R. La-Sr-Ni-Co-O based perovskite-type solid solutions as catalyst precursors in the CO2 reforming of methane. International Journal of Hydrogen Energy, v. 39, p. 4917-4925, 2014. http://dx.doi.org/10.1016/j.jpowsour.2009.10.004 WANG, N.; YU, X.; WANG, Y.; CHU, W.; LIU, M. A comparison study on methane dry reforming with carbon dioxide over LaNiO3 perovskite catalysts supported on mesoporous SBA-15, MCM-41 and silica carrier. Catalysis Today, v. 212, p. 98–107, 2013. http://dx.doi.org/10.1016/j.cattod.2012.07.022 WANG, Z.; CAO, X.M.; ZHU, J.; HU, P. Activity and coke formation of nickel and nickel carbide in dry reforming: a deactivation scheme from density functional theory. Journal of Catalysis, v. 311, p. 469-480, 2014. http://dx.doi.org/10.1016/j.jcat.2013.12.015 YI, N.; CAO, Y.; SU, Y.; DAI, W.-L.; HE, H.-Y.; FAN, K.-N. 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Effects of Fe partial substitution of La2NiO4/LaNiO3 catalyst precursors prepared by wet impregnation method for the dry reforming of methane. Applied Catalysis A: General, v. 526, p. 132–138, 2016. http://dx.doi.org/10.1016/j.apcata.2016.07.024 SUTTHIUMPORN, K.; MANEERUNG, T.; KATHIRASER, Y.; KAWI, S. CO2 dry-reforming of methane over La0.8Sr0.2Ni0.8M0.2O3 perovskite (M = Bi, Co, Cr, Cu, Fe): Roles of lattice oxygen on CeH activation and carbon suppression. International Journal of Hydrogen Energy, v. 37, p. 11195-11207, 2012. http://dx.doi.org/10.1016/j.ijhydene.2012.04.059 TSANG, S.C.; CLARIDGE, J.B.; GREEN, M.L.H. Recent advances in the conversion of methane to synthesis gas. Catalysis Today, v. 23, p. 3–15, 1995. http://dx.doi.org/10.1016/0920-5861(94)00080-L VALDERRAMA, G.; GOLDWASSER, M.R.; NAVARRO, C.U.; TATIBOUËT, J.M.; BARRAULT, J.; BATIOT-DUPEYRAT, C.; MARTÍNEZ, F. Dry reforming of methane over Ni perovskite type oxides. Catalysis Today, v. 107-108, p. 785-791, 2005. http://dx.doi.org/10.1016/j.cattod.2005.07.010 VALDERRAMA, G.; KIENNEMANN, A.; GOLDWASSER, M.R. La-Sr-Ni-Co-O based perovskite-type solid solutions as catalyst precursors in the CO2 reforming of methane. International Journal of Hydrogen Energy, v. 39, p. 4917-4925, 2014. http://dx.doi.org/10.1016/j.jpowsour.2009.10.004 WANG, N.; YU, X.; WANG, Y.; CHU, W.; LIU, M. A comparison study on methane dry reforming with carbon dioxide over LaNiO3 perovskite catalysts supported on mesoporous SBA-15, MCM-41 and silica carrier. Catalysis Today, v. 212, p. 98–107, 2013. http://dx.doi.org/10.1016/j.cattod.2012.07.022 WANG, Z.; CAO, X.M.; ZHU, J.; HU, P. Activity and coke formation of nickel and nickel carbide in dry reforming: a deactivation scheme from density functional theory. Journal of Catalysis, v. 311, p. 469-480, 2014. http://dx.doi.org/10.1016/j.jcat.2013.12.015 YI, N.; CAO, Y.; SU, Y.; DAI, W.-L.; HE, H.-Y.; FAN, K.-N. Nanocrystalline LaCoO3 perovskite particles confined in SBA-15 silica as a new efficient catalyst for hydrocarbon oxidation. Journal of Catalysis, v. 230, p. 249–253, 2005. http://dx.doi.org/10.1016/j.jcat.2004.11.042 ZHANG, Q.; LI, Z.; WANG, G.; LI, H. Study on the impacts of natural gas supply cost on gas flow and infrastructure deployment in China. Applied Energy, v. 162, p. 1385-1398, 2016. http://dx.doi.org/10.1016/j.apenergy.2015.06.058 |
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