Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysis
Ceria-supported Ni-Ru bimetallic catalysts with different metal loadings have been prepared by co-impregnation, characterized and tested in the production of hydrogen from the catalytic decomposition of ammonia. The bimetallic catalysts showed an excellent catalytic performance in long-term stabilit...
| Autores: | , , , , , |
|---|---|
| Tipo de documento: | artigo |
| Data de publicação: | 2021 |
| País: | España |
| Recursos: | Universitat Politècnica de Catalunya (UPC) |
| Repositório: | UPCommons. Portal del coneixement obert de la UPC |
| Idioma: | inglês |
| OAI Identifier: | oai:upcommons.upc.edu:2117/364129 |
| Acesso em linha: | https://hdl.handle.net/2117/364129 https://dx.doi.org/10.1016/j.apcatb.2021.119896 |
| Access Level: | Acceso aberto |
| Palavra-chave: | Catalysis Ammonia Ammonia decomposition Bimetallic catalysts Nickel-ruthenium Ceria catalysts Kinetics Catàlisi Amoníac Àrees temàtiques de la UPC::Física |
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Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysisLucentini, Ilaria|||0000-0003-1311-9062García Colli, GermánLuzi, Carlos DanielSerrano Carreño, M. Isabel|||0000-0002-4996-9280Martínez, Osvaldo MiguelLlorca Piqué, Jordi|||0000-0002-7447-9582CatalysisAmmoniaAmmonia decompositionBimetallic catalystsNickel-rutheniumCeria catalystsKineticsCatàlisiAmoníacÀrees temàtiques de la UPC::FísicaCeria-supported Ni-Ru bimetallic catalysts with different metal loadings have been prepared by co-impregnation, characterized and tested in the production of hydrogen from the catalytic decomposition of ammonia. The bimetallic catalysts showed an excellent catalytic performance in long-term stability tests with respect to monometallic Ru/CeO2 and Ni/CeO2 and in multicycle tests under pure ammonia. The best catalytic performance has been obtained over catalysts with 2.4-5 wt.% Ni, 0.4-0.6 wt.% Ru, and a Ni/Ru wt.% ratio of ca. 7. TOFH2 values exceeding 2 s-1 have been obtained, which are among the highest reported for ammonia decomposition at 400 °C. Raman spectroscopy, XRD, HRTEM, XPS, TPR and H2 chemisorption have revealed the existence of an intimate contact between Ni and Ru and CeO2, which is considered the reason of the excellent catalytic activity and stability observed. A kinetic model has been developed using the Langmuir-Hinshelwood-Hougen-Watson approach for the decomposition of ammonia in a fixed bed reactor. The reaction rate expression of the ammonia decomposition on Ni-Ru bimetallics supported on ceria suggests that the dehydrogenation of the ammonia adsorbed on the surface of the catalyst is the limiting step of the reaction and that ammonia decomposition is inhibited by the presence of H2.Peer ReviewedElsevier20212021-06-0520222022-03-15journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/2117/364129https://dx.doi.org/10.1016/j.apcatb.2021.119896reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution 4.0 International (CC BY 4.0)https://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/3641292026-05-27T15:37:01Z |
| dc.title.none.fl_str_mv |
Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysis |
| title |
Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysis |
| spellingShingle |
Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysis Lucentini, Ilaria|||0000-0003-1311-9062 Catalysis Ammonia Ammonia decomposition Bimetallic catalysts Nickel-ruthenium Ceria catalysts Kinetics Catàlisi Amoníac Àrees temàtiques de la UPC::Física |
| title_short |
Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysis |
| title_full |
Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysis |
| title_fullStr |
Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysis |
| title_full_unstemmed |
Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysis |
| title_sort |
Catalytic ammonia decomposition over Ni-Ru supported on CeO2 for hydrogen production: Effect of metal loading and kinetic analysis |
| dc.creator.none.fl_str_mv |
Lucentini, Ilaria|||0000-0003-1311-9062 García Colli, Germán Luzi, Carlos Daniel Serrano Carreño, M. Isabel|||0000-0002-4996-9280 Martínez, Osvaldo Miguel Llorca Piqué, Jordi|||0000-0002-7447-9582 |
| author |
Lucentini, Ilaria|||0000-0003-1311-9062 |
| author_facet |
Lucentini, Ilaria|||0000-0003-1311-9062 García Colli, Germán Luzi, Carlos Daniel Serrano Carreño, M. Isabel|||0000-0002-4996-9280 Martínez, Osvaldo Miguel Llorca Piqué, Jordi|||0000-0002-7447-9582 |
| author_role |
author |
| author2 |
García Colli, Germán Luzi, Carlos Daniel Serrano Carreño, M. Isabel|||0000-0002-4996-9280 Martínez, Osvaldo Miguel Llorca Piqué, Jordi|||0000-0002-7447-9582 |
| author2_role |
author author author author author |
| dc.subject.none.fl_str_mv |
Catalysis Ammonia Ammonia decomposition Bimetallic catalysts Nickel-ruthenium Ceria catalysts Kinetics Catàlisi Amoníac Àrees temàtiques de la UPC::Física |
| topic |
Catalysis Ammonia Ammonia decomposition Bimetallic catalysts Nickel-ruthenium Ceria catalysts Kinetics Catàlisi Amoníac Àrees temàtiques de la UPC::Física |
| description |
Ceria-supported Ni-Ru bimetallic catalysts with different metal loadings have been prepared by co-impregnation, characterized and tested in the production of hydrogen from the catalytic decomposition of ammonia. The bimetallic catalysts showed an excellent catalytic performance in long-term stability tests with respect to monometallic Ru/CeO2 and Ni/CeO2 and in multicycle tests under pure ammonia. The best catalytic performance has been obtained over catalysts with 2.4-5 wt.% Ni, 0.4-0.6 wt.% Ru, and a Ni/Ru wt.% ratio of ca. 7. TOFH2 values exceeding 2 s-1 have been obtained, which are among the highest reported for ammonia decomposition at 400 °C. Raman spectroscopy, XRD, HRTEM, XPS, TPR and H2 chemisorption have revealed the existence of an intimate contact between Ni and Ru and CeO2, which is considered the reason of the excellent catalytic activity and stability observed. A kinetic model has been developed using the Langmuir-Hinshelwood-Hougen-Watson approach for the decomposition of ammonia in a fixed bed reactor. The reaction rate expression of the ammonia decomposition on Ni-Ru bimetallics supported on ceria suggests that the dehydrogenation of the ammonia adsorbed on the surface of the catalyst is the limiting step of the reaction and that ammonia decomposition is inhibited by the presence of H2. |
| publishDate |
2021 |
| dc.date.none.fl_str_mv |
2021 2021-06-05 2022 2022-03-15 |
| dc.type.none.fl_str_mv |
journal article http://purl.org/coar/resource_type/c_6501 VoR http://purl.org/coar/version/c_970fb48d4fbd8a85 |
| dc.type.openaire.fl_str_mv |
info:eu-repo/semantics/article |
| format |
article |
| dc.identifier.none.fl_str_mv |
https://hdl.handle.net/2117/364129 https://dx.doi.org/10.1016/j.apcatb.2021.119896 |
| url |
https://hdl.handle.net/2117/364129 https://dx.doi.org/10.1016/j.apcatb.2021.119896 |
| dc.language.none.fl_str_mv |
Inglés eng |
| language_invalid_str_mv |
Inglés |
| language |
eng |
| dc.rights.none.fl_str_mv |
open access http://purl.org/coar/access_right/c_abf2 Attribution 4.0 International (CC BY 4.0) https://creativecommons.org/licenses/by/4.0/ |
| 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 4.0 International (CC BY 4.0) https://creativecommons.org/licenses/by/4.0/ |
| eu_rights_str_mv |
openAccess |
| 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:UPCommons. Portal del coneixement obert de la UPC instname:Universitat Politècnica de Catalunya (UPC) |
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Universitat Politècnica de Catalunya (UPC) |
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UPCommons. Portal del coneixement obert de la UPC |
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UPCommons. Portal del coneixement obert de la UPC |
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