The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalysts

Although nickel dispersed in mesoporous aluminosilicates are efficient catalysts for the oligomerization of ethylene, the nature of the active nickel sites still remains controversial. Here we applied in situ FTIR-CO spectroscopy during reaction with ethylene combined with reaction kinetics with onl...

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Autores: Moussa, Sara, Concepción, Patricia, Arribas, M.A, Martínez, Agustín
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2020
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:dnet:digitalcsic_::5976da95e569eba85c374778ef85f7a3
Acceso en línea:http://hdl.handle.net/10261/224951
Access Level:acceso abierto
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spelling The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalystsMoussa, SaraConcepción, PatriciaArribas, M.AMartínez, AgustínAlthough nickel dispersed in mesoporous aluminosilicates are efficient catalysts for the oligomerization of ethylene, the nature of the active nickel sites still remains controversial. Here we applied in situ FTIR-CO spectroscopy during reaction with ethylene combined with reaction kinetics with online MS analysis of reaction products to unravel the nature of the active nickel species in working mesoporous Ni-Al-MCM-41 catalysts. The results revealed that isolated ion-exchanged Ni cations are irreversibly blocked during the initial reaction stages leaving unsaturated Ni cations grafted on silanols and at the surface of small (confined) NiO nanoparticles as the active species in the pseudo-steady state. The low activity of these species in pure silica materials suggested a promotional role of aluminum in the Al-MCM-41 matrix on enhancing the activity of Ni sites, probably through a close interaction between Al species and nearby Ni sites, as inferred from quantitative Al MAS NMR and FTIR spectroscopies.This work has been financially supported by the Spanish government through the Severo Ochoa Program (SEV2016-0683) and RTI2018-102161 projects. The authors acknowledge the Microscopy Service of the Universitat Politècnica de València for its assistance in the characterization of materials by electron microscopy.Elsevier BVMinisterio de Economía y Competitividad (España)Ministerio de Ciencia, Innovación y Universidades (España)Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]2020202020202020info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/224951reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/SEV-2016-0683info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-102161http://dx.doi.org/10.1016/j.apcata.2020.117831Síinfo:eu-repo/semantics/openAccessoai:dnet:digitalcsic_::5976da95e569eba85c374778ef85f7a32026-05-22T06:33:51Z
dc.title.none.fl_str_mv The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalysts
title The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalysts
spellingShingle The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalysts
Moussa, Sara
title_short The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalysts
title_full The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalysts
title_fullStr The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalysts
title_full_unstemmed The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalysts
title_sort The nature of active Ni sites and the role of Al species in the oligomerization of ethylene on mesoporous Ni-Al-MCM-41 catalysts
dc.creator.none.fl_str_mv Moussa, Sara
Concepción, Patricia
Arribas, M.A
Martínez, Agustín
author Moussa, Sara
author_facet Moussa, Sara
Concepción, Patricia
Arribas, M.A
Martínez, Agustín
author_role author
author2 Concepción, Patricia
Arribas, M.A
Martínez, Agustín
author2_role author
author
author
dc.contributor.none.fl_str_mv Ministerio de Economía y Competitividad (España)
Ministerio de Ciencia, Innovación y Universidades (España)
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
description Although nickel dispersed in mesoporous aluminosilicates are efficient catalysts for the oligomerization of ethylene, the nature of the active nickel sites still remains controversial. Here we applied in situ FTIR-CO spectroscopy during reaction with ethylene combined with reaction kinetics with online MS analysis of reaction products to unravel the nature of the active nickel species in working mesoporous Ni-Al-MCM-41 catalysts. The results revealed that isolated ion-exchanged Ni cations are irreversibly blocked during the initial reaction stages leaving unsaturated Ni cations grafted on silanols and at the surface of small (confined) NiO nanoparticles as the active species in the pseudo-steady state. The low activity of these species in pure silica materials suggested a promotional role of aluminum in the Al-MCM-41 matrix on enhancing the activity of Ni sites, probably through a close interaction between Al species and nearby Ni sites, as inferred from quantitative Al MAS NMR and FTIR spectroscopies.
publishDate 2020
dc.date.none.fl_str_mv 2020
2020
2020
2020
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/10261/224951
url http://hdl.handle.net/10261/224951
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/SEV-2016-0683
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-102161
http://dx.doi.org/10.1016/j.apcata.2020.117831
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Elsevier BV
publisher.none.fl_str_mv Elsevier BV
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
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