Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustion

The objective of this work was to determine the kinetic parameters for reduction and oxidation reactions of a highly reactive Fe-based oxygen carrier for use in chemical looping combustion (CLC) of gaseous fuels containing CH4, CO and/or H2, e.g. natural gas, syngas and PSA-off gas. The oxygen carri...

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Autores: Cabello Flores, Arturo, Abad Secades, Alberto, García Labiano, Francisco, Gayán Sanz, Pilar, Diego Poza, Luis F. de, Adánez Elorza, Juan
Formato: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2014
País:España
Recursos:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/137809
Acesso em linha:http://hdl.handle.net/10261/137809
Access Level:acceso abierto
Palavra-chave:CO2 capture
Chemical looping combustion
Oxygen carrier
Iron
Reaction kinetic
Impregnated
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spelling Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustionCabello Flores, ArturoAbad Secades, AlbertoGarcía Labiano, FranciscoGayán Sanz, PilarDiego Poza, Luis F. deAdánez Elorza, JuanCO2 captureChemical looping combustionOxygen carrierIronReaction kineticImpregnatedThe objective of this work was to determine the kinetic parameters for reduction and oxidation reactions of a highly reactive Fe-based oxygen carrier for use in chemical looping combustion (CLC) of gaseous fuels containing CH4, CO and/or H2, e.g. natural gas, syngas and PSA-off gas. The oxygen carrier was prepared by impregnation of iron on alumina. The effect of both the temperature and gas concentration was analysed in a thermogravimetric analyser (TGA). The grain model with uniform conversion in the particle and reaction in grains following the shrinking core model (SCM) was used for kinetics determination. It was assumed that the reduction reactions were controlled by two different resistances: the reaction rate was controlled by chemical reaction in a first step, whereas the mechanism that controlled the reactions at higher conversion values was diffusion through the product layer around the grains. Furthermore, it was found that the reduction reaction mechanism was based on the interaction of Fe2O3 with Al2O3 in presence of the reacting gases to form FeAl2O4 as the only stable Fe-based phase. The reaction order values found for the reducing gases were 0.25, 0.3 and 0.6 for CH4, H2 and CO, respectively, and the activation energy took values of between 8 kJ mol-1 (for H2) and 66 kJ mol-1 (for CH4). With regard to oxidation kinetics, the reacting model assumed a reaction rate that was only controlled by chemical reaction. Values of 0.9 and 23 kJ mol-1 were found for reaction order and activation energy, respectively. Finally, the solids inventory needed in a CLC system was also estimated by considering kinetic parameters. The total solids inventory in the CLC unit took a minimum value of 150 kg MW-1 for CH4 combustion, which is a low value when compared to those of other Fe-based materials found in the literature.This paper is based on the work carried out within the framework of the SUCCESS project, funded by the European Commission under the seventh Framework Programme (Contract 608571). This research was supported by the Spanish Ministry of Science and Innovation (MICINN Project: ENE2011-26354) and by FEDER.Peer reviewedElsevierEuropean CommissionMinisterio de Ciencia e Innovación (España)Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]201620162014info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/137809reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/EC/FP7/608571http://dx.doi.org/10.1016/j.cej.2014.07.083Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/1378092026-05-22T06:33:51Z
dc.title.none.fl_str_mv Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustion
title Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustion
spellingShingle Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustion
Cabello Flores, Arturo
CO2 capture
Chemical looping combustion
Oxygen carrier
Iron
Reaction kinetic
Impregnated
title_short Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustion
title_full Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustion
title_fullStr Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustion
title_full_unstemmed Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustion
title_sort Kinetic determination of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for use in gas-fuelled chemical looping combustion
dc.creator.none.fl_str_mv Cabello Flores, Arturo
Abad Secades, Alberto
García Labiano, Francisco
Gayán Sanz, Pilar
Diego Poza, Luis F. de
Adánez Elorza, Juan
author Cabello Flores, Arturo
author_facet Cabello Flores, Arturo
Abad Secades, Alberto
García Labiano, Francisco
Gayán Sanz, Pilar
Diego Poza, Luis F. de
Adánez Elorza, Juan
author_role author
author2 Abad Secades, Alberto
García Labiano, Francisco
Gayán Sanz, Pilar
Diego Poza, Luis F. de
Adánez Elorza, Juan
author2_role author
author
author
author
author
dc.contributor.none.fl_str_mv European Commission
Ministerio de Ciencia e Innovación (España)
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv CO2 capture
Chemical looping combustion
Oxygen carrier
Iron
Reaction kinetic
Impregnated
topic CO2 capture
Chemical looping combustion
Oxygen carrier
Iron
Reaction kinetic
Impregnated
description The objective of this work was to determine the kinetic parameters for reduction and oxidation reactions of a highly reactive Fe-based oxygen carrier for use in chemical looping combustion (CLC) of gaseous fuels containing CH4, CO and/or H2, e.g. natural gas, syngas and PSA-off gas. The oxygen carrier was prepared by impregnation of iron on alumina. The effect of both the temperature and gas concentration was analysed in a thermogravimetric analyser (TGA). The grain model with uniform conversion in the particle and reaction in grains following the shrinking core model (SCM) was used for kinetics determination. It was assumed that the reduction reactions were controlled by two different resistances: the reaction rate was controlled by chemical reaction in a first step, whereas the mechanism that controlled the reactions at higher conversion values was diffusion through the product layer around the grains. Furthermore, it was found that the reduction reaction mechanism was based on the interaction of Fe2O3 with Al2O3 in presence of the reacting gases to form FeAl2O4 as the only stable Fe-based phase. The reaction order values found for the reducing gases were 0.25, 0.3 and 0.6 for CH4, H2 and CO, respectively, and the activation energy took values of between 8 kJ mol-1 (for H2) and 66 kJ mol-1 (for CH4). With regard to oxidation kinetics, the reacting model assumed a reaction rate that was only controlled by chemical reaction. Values of 0.9 and 23 kJ mol-1 were found for reaction order and activation energy, respectively. Finally, the solids inventory needed in a CLC system was also estimated by considering kinetic parameters. The total solids inventory in the CLC unit took a minimum value of 150 kg MW-1 for CH4 combustion, which is a low value when compared to those of other Fe-based materials found in the literature.
publishDate 2014
dc.date.none.fl_str_mv 2014
2016
2016
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Postprint
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/137809
url http://hdl.handle.net/10261/137809
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/EC/FP7/608571
http://dx.doi.org/10.1016/j.cej.2014.07.083
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.811543

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