Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthane

[EN]The viability of a series of nickel aluminate-based spinel catalysts with varying Ni deficiency (corresponding to a Ni/Al molar ratio in the 0.13-0.50 range) was explored for the partial oxidation of methane under different operation conditions in terms of temperature, volume hourly space veloci...

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Autores: Gil Calvo, Miryam, Jiménez González, Cristina, De Rivas Martín, Beatriz, Gutiérrez Ortiz, José Ignacio, López Fonseca, Rubén
Tipo de recurso: artículo
Fecha de publicación:2017
País:España
Institución:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/71503
Acceso en línea:http://hdl.handle.net/10810/71503
Access Level:acceso abierto
Palabra clave:methane
partial oxidation
nickel aluminate
substoichiometric spin
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spelling Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthaneGil Calvo, MiryamJiménez González, CristinaDe Rivas Martín, BeatrizGutiérrez Ortiz, José IgnacioLópez Fonseca, Rubénmethanepartial oxidationnickel aluminatesubstoichiometric spin[EN]The viability of a series of nickel aluminate-based spinel catalysts with varying Ni deficiency (corresponding to a Ni/Al molar ratio in the 0.13-0.50 range) was explored for the partial oxidation of methane under different operation conditions in terms of temperature, volume hourly space velocity, O/C molar ratio and time on stream. Thus spinel-type catalysts with a Ni loading between 11 and 31wt.% were prepared by coprecipitation. A wide number of techniques including WDXRF, XRD, N2 physisorption, Raman spectroscopy, XPS, UV-visible-NIR DRS, H2-TPR, TEM and TGA-MS were used to characterise the calcined, reduced and post-run samples. With respect to the reference stoichiometric sample (Ni/Al=0.50) alumina excess in the precursor oxide provoked notable changes in the surface area, structural properties connected with the relative cation distribution between tetrahedral and octahedral coordination and reducibility of the resultant spinel phase. It was found that the catalytic performance of these non-stoichiometric samples could be optimised for a Ni/Al molar ratio of 0.25, which corresponded to a metal loading of 19wt.%Ni. The oxidation activity was associated with the remarkable intrinsic activity of nickel particles derived from Ni2+ cations with a preferential occupancy of octahedral sites in the lattice of the oxide. The promising catalytic behaviour of this sample was further proven by the notable activity and stability shown under severe reaction conditions with a reduced loss of yield of hydrogen with time on stream.The financial support for this work has been provided by the Spanish Ministry of Economy and Competitiveness (ENE2013-41187-R) and the Basque Country Government (PRE_2015_2_0114).Elsevier202520252017info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10810/71503reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoIngléshttps://doi.org/10.1016/j.apcatb.2017.02.063info:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by-nc-nd/3.0/es/© 2017 Elsevier under CC BY-NC-ND licenseoai:addi.ehu.eus:10810/715032026-06-18T09:23:17Z
dc.title.none.fl_str_mv Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthane
title Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthane
spellingShingle Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthane
Gil Calvo, Miryam
methane
partial oxidation
nickel aluminate
substoichiometric spin
title_short Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthane
title_full Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthane
title_fullStr Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthane
title_full_unstemmed Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthane
title_sort Effect of Ni/Al molar ratio on the performance of substoichiometric NiAl2O4 spinel-based catalysts for partial oxidation of metthane
dc.creator.none.fl_str_mv Gil Calvo, Miryam
Jiménez González, Cristina
De Rivas Martín, Beatriz
Gutiérrez Ortiz, José Ignacio
López Fonseca, Rubén
author Gil Calvo, Miryam
author_facet Gil Calvo, Miryam
Jiménez González, Cristina
De Rivas Martín, Beatriz
Gutiérrez Ortiz, José Ignacio
López Fonseca, Rubén
author_role author
author2 Jiménez González, Cristina
De Rivas Martín, Beatriz
Gutiérrez Ortiz, José Ignacio
López Fonseca, Rubén
author2_role author
author
author
author
dc.subject.none.fl_str_mv methane
partial oxidation
nickel aluminate
substoichiometric spin
topic methane
partial oxidation
nickel aluminate
substoichiometric spin
description [EN]The viability of a series of nickel aluminate-based spinel catalysts with varying Ni deficiency (corresponding to a Ni/Al molar ratio in the 0.13-0.50 range) was explored for the partial oxidation of methane under different operation conditions in terms of temperature, volume hourly space velocity, O/C molar ratio and time on stream. Thus spinel-type catalysts with a Ni loading between 11 and 31wt.% were prepared by coprecipitation. A wide number of techniques including WDXRF, XRD, N2 physisorption, Raman spectroscopy, XPS, UV-visible-NIR DRS, H2-TPR, TEM and TGA-MS were used to characterise the calcined, reduced and post-run samples. With respect to the reference stoichiometric sample (Ni/Al=0.50) alumina excess in the precursor oxide provoked notable changes in the surface area, structural properties connected with the relative cation distribution between tetrahedral and octahedral coordination and reducibility of the resultant spinel phase. It was found that the catalytic performance of these non-stoichiometric samples could be optimised for a Ni/Al molar ratio of 0.25, which corresponded to a metal loading of 19wt.%Ni. The oxidation activity was associated with the remarkable intrinsic activity of nickel particles derived from Ni2+ cations with a preferential occupancy of octahedral sites in the lattice of the oxide. The promising catalytic behaviour of this sample was further proven by the notable activity and stability shown under severe reaction conditions with a reduced loss of yield of hydrogen with time on stream.
publishDate 2017
dc.date.none.fl_str_mv 2017
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10810/71503
url http://hdl.handle.net/10810/71503
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv https://doi.org/10.1016/j.apcatb.2017.02.063
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
© 2017 Elsevier under CC BY-NC-ND license
eu_rights_str_mv openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by-nc-nd/3.0/es/
© 2017 Elsevier under CC BY-NC-ND license
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
dc.source.none.fl_str_mv reponame:Addi. Archivo Digital para la Docencia y la Investigación
instname:Universidad del País Vasco
instname_str Universidad del País Vasco
reponame_str Addi. Archivo Digital para la Docencia y la Investigación
collection Addi. Archivo Digital para la Docencia y la Investigación
repository.name.fl_str_mv
repository.mail.fl_str_mv
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