In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature

Studies with a series of metal/ceria(111) (metal=Co, Ni, Cu; ceria=CeO2) surfaces indicate that metal–oxide interactions can play a very important role for the activation of methane and its reforming with CO2 at relatively low temperatures (600–700 K). Among the systems examined, Co/CeO2(111) exhibi...

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Authors: Liu, Zongyuan, Lustemberg, Pablo G., Gutiérrez, Ramón A., Carey, John J., Palomino, Robert M., Vorokhta, Mykhailo, Grinter, David C., Ramírez, Pedro J., Matolín, Vladimír, Nolan, Michael, Ganduglia-Pirovano, M. V., Senanayake, S.D., Rodriguez, J.A.
Format: article
Status:Versión aceptada para publicación
Publication Date:2017
Country:España
Institution:Consejo Superior de Investigaciones Científicas (CSIC)
Repository:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/377028
Online Access:http://hdl.handle.net/10261/377028
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85028945531&doi=10.1002%2fanie.201707538&partnerID=40&md5=0e20615b2ed61247730ed7017376d639
Access Level:Open access
Keyword:ceria
cobalt
density functional theory
methane dissociation
XPS
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spelling In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low TemperatureLiu, ZongyuanLustemberg, Pablo G.Gutiérrez, Ramón A.Carey, John J.Palomino, Robert M.Vorokhta, MykhailoGrinter, David C.Ramírez, Pedro J.Matolín, VladimírNolan, MichaelGanduglia-Pirovano, M. V.Senanayake, S.D.Rodriguez, J.A.ceriacobaltdensity functional theorymethane dissociationXPSStudies with a series of metal/ceria(111) (metal=Co, Ni, Cu; ceria=CeO2) surfaces indicate that metal–oxide interactions can play a very important role for the activation of methane and its reforming with CO2 at relatively low temperatures (600–700 K). Among the systems examined, Co/CeO2(111) exhibits the best performance and Cu/CeO2(111) has negligible activity. Experiments using ambient pressure X-ray photoelectron spectroscopy indicate that methane dissociates on Co/CeO2(111) at temperatures as low as 300 K—generating CHx and COx species on the catalyst surface. The results of density functional calculations show a reduction in the methane activation barrier from 1.07 eV on Co(0001) to 0.87 eV on Co2+/CeO2(111), and to only 0.05 eV on Co0/CeO2−x(111). At 700 K, under methane dry reforming conditions, CO2 dissociates on the oxide surface and a catalytic cycle is established without coke deposition. A significant part of the CHx formed on the Co0/CeO2−x(111) catalyst recombines to yield ethane or ethylene. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, WeinheimThe work carried out at Brookhaven National Laboratory was supported by the US Department of Energy (Chemical Sciences Division, DE-SC0012704). The theoretical work was supported by the MINECO-Spain (CTQ2015-78823-R) and the European Commission Framework 7 project BIOGO (Grant no. 604296). The COST action CM1104 is gratefully acknowledged. Computer time provided by the SGAI-CSIC, CESGA, BIFI-ZCAM, RES, SNCAD (Sistema Nacional de Computaciln de Alto DesempeÇo, Arg), ICHEC, and the DECI resources BEM based in Poland at WCSS and Archer at EPCC with support from the PRACE aislb, is acknowledged. M.V. thanks the Ministry of Education, Youth and Sports of the Czech Republic for financial support under project LH15277.Peer reviewedJohn Wiley & SonsConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252017info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/377028https://www.scopus.com/inward/record.uri?eid=2-s2.0-85028945531&doi=10.1002%2fanie.201707538&partnerID=40&md5=0e20615b2ed61247730ed7017376d639reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)InglésAngewandte Chemie - International Editionhttps://doi.org/10.1002/anie.201707538Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3770282026-05-22T06:33:51Z
dc.title.none.fl_str_mv In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature
title In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature
spellingShingle In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature
Liu, Zongyuan
ceria
cobalt
density functional theory
methane dissociation
XPS
title_short In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature
title_full In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature
title_fullStr In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature
title_full_unstemmed In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature
title_sort In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature
dc.creator.none.fl_str_mv Liu, Zongyuan
Lustemberg, Pablo G.
Gutiérrez, Ramón A.
Carey, John J.
Palomino, Robert M.
Vorokhta, Mykhailo
Grinter, David C.
Ramírez, Pedro J.
Matolín, Vladimír
Nolan, Michael
Ganduglia-Pirovano, M. V.
Senanayake, S.D.
Rodriguez, J.A.
author Liu, Zongyuan
author_facet Liu, Zongyuan
Lustemberg, Pablo G.
Gutiérrez, Ramón A.
Carey, John J.
Palomino, Robert M.
Vorokhta, Mykhailo
Grinter, David C.
Ramírez, Pedro J.
Matolín, Vladimír
Nolan, Michael
Ganduglia-Pirovano, M. V.
Senanayake, S.D.
Rodriguez, J.A.
author_role author
author2 Lustemberg, Pablo G.
Gutiérrez, Ramón A.
Carey, John J.
Palomino, Robert M.
Vorokhta, Mykhailo
Grinter, David C.
Ramírez, Pedro J.
Matolín, Vladimír
Nolan, Michael
Ganduglia-Pirovano, M. V.
Senanayake, S.D.
Rodriguez, J.A.
author2_role author
author
author
author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv ceria
cobalt
density functional theory
methane dissociation
XPS
topic ceria
cobalt
density functional theory
methane dissociation
XPS
description Studies with a series of metal/ceria(111) (metal=Co, Ni, Cu; ceria=CeO2) surfaces indicate that metal–oxide interactions can play a very important role for the activation of methane and its reforming with CO2 at relatively low temperatures (600–700 K). Among the systems examined, Co/CeO2(111) exhibits the best performance and Cu/CeO2(111) has negligible activity. Experiments using ambient pressure X-ray photoelectron spectroscopy indicate that methane dissociates on Co/CeO2(111) at temperatures as low as 300 K—generating CHx and COx species on the catalyst surface. The results of density functional calculations show a reduction in the methane activation barrier from 1.07 eV on Co(0001) to 0.87 eV on Co2+/CeO2(111), and to only 0.05 eV on Co0/CeO2−x(111). At 700 K, under methane dry reforming conditions, CO2 dissociates on the oxide surface and a catalytic cycle is established without coke deposition. A significant part of the CHx formed on the Co0/CeO2−x(111) catalyst recombines to yield ethane or ethylene. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
publishDate 2017
dc.date.none.fl_str_mv 2017
2025
2025
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/10261/377028
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85028945531&doi=10.1002%2fanie.201707538&partnerID=40&md5=0e20615b2ed61247730ed7017376d639
url http://hdl.handle.net/10261/377028
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85028945531&doi=10.1002%2fanie.201707538&partnerID=40&md5=0e20615b2ed61247730ed7017376d639
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Angewandte Chemie - International Edition
https://doi.org/10.1002/anie.201707538
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv John Wiley & Sons
publisher.none.fl_str_mv John Wiley & Sons
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 15,81155

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