Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalysts

Partial oxidation of methane (POM) was studied over a series of Co/Mg-Al catalysts. Various commercial hydroxides with different Mg/Al ratios were used as precursors of the oxides employed as catalytic supports, as well as MgO prepared in the laboratory. The effects of Co loading, Mg content, and ca...

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Autores: Moral, A., Reyero, I., Llorca Piqué, Jordi|||0000-0002-7447-9582, Bimbela, F., Gandía, L. M.
Formato: artículo
Fecha de publicación:2018
País:España
Recursos:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/130912
Acesso em linha:https://hdl.handle.net/2117/130912
https://dx.doi.org/10.1016/j.cattod.2018.04.003
Access Level:acceso abierto
Palavra-chave:Cobalt catalysts
Methane
Synthesis gas
Coke formation
Mg-Al supports
Partial oxidation
Syngas
Cobalt
Metà
Àrees temàtiques de la UPC::Enginyeria química
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spelling Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalystsMoral, A.Reyero, I.Llorca Piqué, Jordi|||0000-0002-7447-9582Bimbela, F.Gandía, L. M.Cobalt catalystsMethaneSynthesis gasCobalt catalystsCoke formationMethaneMg-Al supportsPartial oxidationSyngasCobaltMetàÀrees temàtiques de la UPC::Enginyeria químicaPartial oxidation of methane (POM) was studied over a series of Co/Mg-Al catalysts. Various commercial hydroxides with different Mg/Al ratios were used as precursors of the oxides employed as catalytic supports, as well as MgO prepared in the laboratory. The effects of Co loading, Mg content, and calcination temperature (400–750¿°C) were studied on the POM reaction. The catalytic performance was evaluated at 800¿°C in a fixed-bed tubular quartz reactor under a high space velocity of 300¿L N CH4/(gcat¿h) and a O2/CH4 molar ratio of 0.5. A very high activity was obtained during 4¿h on-stream with a 20¿wt. % Co catalyst prepared with a Mg-Al mixed oxide support having a MgO content of 63¿wt. %. This catalyst gave CH4 conversions (91.3%) very close to the maximum corresponding to the thermodynamic equilibrium. Such notable performance could be attained with the catalyst precursor subjected to calcination at 500¿°C for 6¿h and subsequent in situ reduction under H2 flow at 800¿°C for 2¿h. Two main types of deactivation mechanisms were generally observed in most of the samples that suffered either a very rapid cobalt re-oxidation upon their exposure to the POM reaction atmosphere or significant deposition of carbonaceous deposits of different kinds. The characterization of the spent samples by transmission electron microscopy (TEM) revealed the presence of carbon deposits of different nature in the Mg/Al samples having a high MgO content, including filamentous carbon (whiskers), onion-shell like sheets and/or amorphous encapsulating layers. Conversely, no carbon deposits were observed in the spent Co/MgO catalyst, which underwent oxidation of the relatively less dispersed surface Co sites to form clearly defined crystals of Co oxides with particle diameters typically ranging between 25 and 100¿nm.Peer Reviewed20182018-04-0320192019-03-27journal articlehttp://purl.org/coar/resource_type/c_6501AMhttp://purl.org/coar/version/c_ab4af688f83e57aainfo:eu-repo/semantics/articleapplication/pdfapplication/pdfhttps://hdl.handle.net/2117/130912https://dx.doi.org/10.1016/j.cattod.2018.04.003reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)InglésengMinisterio de Economía y Competitividad http://doi.org/10.13039/501100003329 ENE2015-63969-C3-1-R MICROREACTORES CON TECNOLOGIA DE IMPRESION 3D PARA LA GENERACION CATALITICA Y FOTOCATALITICA DE HIDROGENOopen accesshttp://purl.org/coar/access_right/c_abf2Attribution-NonCommercial-NoDerivs 3.0 Spainhttp://creativecommons.org/licenses/by-nc-nd/3.0/es/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/1309122026-05-27T15:37:01Z
dc.title.none.fl_str_mv Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalysts
title Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalysts
spellingShingle Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalysts
Moral, A.
Cobalt catalysts
Methane
Synthesis gas
Cobalt catalysts
Coke formation
Methane
Mg-Al supports
Partial oxidation
Syngas
Cobalt
Metà
Àrees temàtiques de la UPC::Enginyeria química
title_short Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalysts
title_full Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalysts
title_fullStr Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalysts
title_full_unstemmed Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalysts
title_sort Partial oxidation of methane to syngas using Co/Mg and Co/Mg-Al oxide supported catalysts
dc.creator.none.fl_str_mv Moral, A.
Reyero, I.
Llorca Piqué, Jordi|||0000-0002-7447-9582
Bimbela, F.
Gandía, L. M.
author Moral, A.
author_facet Moral, A.
Reyero, I.
Llorca Piqué, Jordi|||0000-0002-7447-9582
Bimbela, F.
Gandía, L. M.
author_role author
author2 Reyero, I.
Llorca Piqué, Jordi|||0000-0002-7447-9582
Bimbela, F.
Gandía, L. M.
author2_role author
author
author
author
dc.subject.none.fl_str_mv Cobalt catalysts
Methane
Synthesis gas
Cobalt catalysts
Coke formation
Methane
Mg-Al supports
Partial oxidation
Syngas
Cobalt
Metà
Àrees temàtiques de la UPC::Enginyeria química
topic Cobalt catalysts
Methane
Synthesis gas
Cobalt catalysts
Coke formation
Methane
Mg-Al supports
Partial oxidation
Syngas
Cobalt
Metà
Àrees temàtiques de la UPC::Enginyeria química
description Partial oxidation of methane (POM) was studied over a series of Co/Mg-Al catalysts. Various commercial hydroxides with different Mg/Al ratios were used as precursors of the oxides employed as catalytic supports, as well as MgO prepared in the laboratory. The effects of Co loading, Mg content, and calcination temperature (400–750¿°C) were studied on the POM reaction. The catalytic performance was evaluated at 800¿°C in a fixed-bed tubular quartz reactor under a high space velocity of 300¿L N CH4/(gcat¿h) and a O2/CH4 molar ratio of 0.5. A very high activity was obtained during 4¿h on-stream with a 20¿wt. % Co catalyst prepared with a Mg-Al mixed oxide support having a MgO content of 63¿wt. %. This catalyst gave CH4 conversions (91.3%) very close to the maximum corresponding to the thermodynamic equilibrium. Such notable performance could be attained with the catalyst precursor subjected to calcination at 500¿°C for 6¿h and subsequent in situ reduction under H2 flow at 800¿°C for 2¿h. Two main types of deactivation mechanisms were generally observed in most of the samples that suffered either a very rapid cobalt re-oxidation upon their exposure to the POM reaction atmosphere or significant deposition of carbonaceous deposits of different kinds. The characterization of the spent samples by transmission electron microscopy (TEM) revealed the presence of carbon deposits of different nature in the Mg/Al samples having a high MgO content, including filamentous carbon (whiskers), onion-shell like sheets and/or amorphous encapsulating layers. Conversely, no carbon deposits were observed in the spent Co/MgO catalyst, which underwent oxidation of the relatively less dispersed surface Co sites to form clearly defined crystals of Co oxides with particle diameters typically ranging between 25 and 100¿nm.
publishDate 2018
dc.date.none.fl_str_mv 2018
2018-04-03
2019
2019-03-27
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
AM
http://purl.org/coar/version/c_ab4af688f83e57aa
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/2117/130912
https://dx.doi.org/10.1016/j.cattod.2018.04.003
url https://hdl.handle.net/2117/130912
https://dx.doi.org/10.1016/j.cattod.2018.04.003
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Ministerio de Economía y Competitividad http://doi.org/10.13039/501100003329 ENE2015-63969-C3-1-R MICROREACTORES CON TECNOLOGIA DE IMPRESION 3D PARA LA GENERACION CATALITICA Y FOTOCATALITICA DE HIDROGENO
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution-NonCommercial-NoDerivs 3.0 Spain
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution-NonCommercial-NoDerivs 3.0 Spain
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.source.none.fl_str_mv reponame:UPCommons. Portal del coneixement obert de la UPC
instname:Universitat Politècnica de Catalunya (UPC)
instname_str Universitat Politècnica de Catalunya (UPC)
reponame_str UPCommons. Portal del coneixement obert de la UPC
collection UPCommons. Portal del coneixement obert de la UPC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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