Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage

Autores
Lustemberg, Pablo German; Ramírez, Pedro J.; Liu, Zongyuan; Gutiérrez, Ramón A.; Grinter, David G.; Carrasco, Javier; Senanayake, Sanjaya D.; Rodriguez, José A.; Ganduglia Pirovano, Maria Veronica
Año de publicación
2016
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The results of core-level photoemission indicate that Ni-CeO2(111) surfaces with small or medium coverages of nickel are able to activate methane at 300 K, producing adsorbed CHx and COx (x = 2, 3) groups. Calculations based on density functional theory predict a relatively low activation energy of 0.6-0.7 eV for the cleavage of the first C-H bond in the adsorbed methane molecule. Ni and O centers of ceria work in a cooperative way in the dissociation of the C-H bond at room temperature, where a low Ni loading is crucial for the catalyst activity and stability. The strong electronic perturbations in the Ni nanoparticles produced by the ceria supports of varying natures, such as stoichiometric and reduced, result in a drastic change in their chemical properties toward methane adsorption and dissociation as well as the dry reforming of methane reaction. The coverage of Ni has a drastic effect on the ability of the system to dissociate methane and catalyze the dry re-forming process.
Fil: Lustemberg, Pablo German. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Ramírez, Pedro J.. Universidad Central de Venezuela. Facultad de Ciencias; Venezuela
Fil: Liu, Zongyuan. State University of New York; Estados Unidos
Fil: Gutiérrez, Ramón A.. Universidad Central de Venezuela. Facultad de Ciencias; Venezuela
Fil: Grinter, David G.. State University of New York; Estados Unidos
Fil: Carrasco, Javier. CIC EnergiGUNE; España
Fil: Senanayake, Sanjaya D.. Brookhaven National Laboratory; Estados Unidos
Fil: Rodriguez, José A.. Brookhaven National Laboratory; Estados Unidos
Fil: Ganduglia Pirovano, Maria Veronica. Consejo Superior de Investigaciones Científicas. Instituto de Catálisis y Petroleoquímica; España
Materia
Ceria
Dft
Dry Re-Forming
Methane Activation
Nickel
Support Effect
Supported Catalysts
Xps
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/61045
Acceder
id CONICETDig_299078cde92f28db2e9fb182b1b188f1
oai_identifier_str oai:ri.conicet.gov.ar:11336/61045
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond CleavageLustemberg, Pablo GermanRamírez, Pedro J.Liu, ZongyuanGutiérrez, Ramón A.Grinter, David G.Carrasco, JavierSenanayake, Sanjaya D.Rodriguez, José A.Ganduglia Pirovano, Maria VeronicaCeriaDftDry Re-FormingMethane ActivationNickelSupport EffectSupported CatalystsXpshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1https://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1The results of core-level photoemission indicate that Ni-CeO2(111) surfaces with small or medium coverages of nickel are able to activate methane at 300 K, producing adsorbed CHx and COx (x = 2, 3) groups. Calculations based on density functional theory predict a relatively low activation energy of 0.6-0.7 eV for the cleavage of the first C-H bond in the adsorbed methane molecule. Ni and O centers of ceria work in a cooperative way in the dissociation of the C-H bond at room temperature, where a low Ni loading is crucial for the catalyst activity and stability. The strong electronic perturbations in the Ni nanoparticles produced by the ceria supports of varying natures, such as stoichiometric and reduced, result in a drastic change in their chemical properties toward methane adsorption and dissociation as well as the dry reforming of methane reaction. The coverage of Ni has a drastic effect on the ability of the system to dissociate methane and catalyze the dry re-forming process.Fil: Lustemberg, Pablo German. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; ArgentinaFil: Ramírez, Pedro J.. Universidad Central de Venezuela. Facultad de Ciencias; VenezuelaFil: Liu, Zongyuan. State University of New York; Estados UnidosFil: Gutiérrez, Ramón A.. Universidad Central de Venezuela. Facultad de Ciencias; VenezuelaFil: Grinter, David G.. State University of New York; Estados UnidosFil: Carrasco, Javier. CIC EnergiGUNE; EspañaFil: Senanayake, Sanjaya D.. Brookhaven National Laboratory; Estados UnidosFil: Rodriguez, José A.. Brookhaven National Laboratory; Estados UnidosFil: Ganduglia Pirovano, Maria Veronica. Consejo Superior de Investigaciones Científicas. Instituto de Catálisis y Petroleoquímica; EspañaAmerican Chemical Society2016-12info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/61045Lustemberg, Pablo German; Ramírez, Pedro J.; Liu, Zongyuan; Gutiérrez, Ramón A.; Grinter, David G.; et al.; Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage; American Chemical Society; ACS Catalysis; 6; 12; 12-2016; 8184-81912155-5435CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/acscatal.6b02360info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acscatal.6b02360info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-10T13:00:32Zoai:ri.conicet.gov.ar:11336/61045instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-10 13:00:32.742CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage
title Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage
spellingShingle Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage
Lustemberg, Pablo German
Ceria
Dft
Dry Re-Forming
Methane Activation
Nickel
Support Effect
Supported Catalysts
Xps
title_short Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage
title_full Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage
title_fullStr Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage
title_full_unstemmed Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage
title_sort Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage
dc.creator.none.fl_str_mv Lustemberg, Pablo German
Ramírez, Pedro J.
Liu, Zongyuan
Gutiérrez, Ramón A.
Grinter, David G.
Carrasco, Javier
Senanayake, Sanjaya D.
Rodriguez, José A.
Ganduglia Pirovano, Maria Veronica
author Lustemberg, Pablo German
author_facet Lustemberg, Pablo German
Ramírez, Pedro J.
Liu, Zongyuan
Gutiérrez, Ramón A.
Grinter, David G.
Carrasco, Javier
Senanayake, Sanjaya D.
Rodriguez, José A.
Ganduglia Pirovano, Maria Veronica
author_role author
author2 Ramírez, Pedro J.
Liu, Zongyuan
Gutiérrez, Ramón A.
Grinter, David G.
Carrasco, Javier
Senanayake, Sanjaya D.
Rodriguez, José A.
Ganduglia Pirovano, Maria Veronica
author2_role author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Ceria
Dft
Dry Re-Forming
Methane Activation
Nickel
Support Effect
Supported Catalysts
Xps
topic Ceria
Dft
Dry Re-Forming
Methane Activation
Nickel
Support Effect
Supported Catalysts
Xps
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The results of core-level photoemission indicate that Ni-CeO2(111) surfaces with small or medium coverages of nickel are able to activate methane at 300 K, producing adsorbed CHx and COx (x = 2, 3) groups. Calculations based on density functional theory predict a relatively low activation energy of 0.6-0.7 eV for the cleavage of the first C-H bond in the adsorbed methane molecule. Ni and O centers of ceria work in a cooperative way in the dissociation of the C-H bond at room temperature, where a low Ni loading is crucial for the catalyst activity and stability. The strong electronic perturbations in the Ni nanoparticles produced by the ceria supports of varying natures, such as stoichiometric and reduced, result in a drastic change in their chemical properties toward methane adsorption and dissociation as well as the dry reforming of methane reaction. The coverage of Ni has a drastic effect on the ability of the system to dissociate methane and catalyze the dry re-forming process.
Fil: Lustemberg, Pablo German. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Ramírez, Pedro J.. Universidad Central de Venezuela. Facultad de Ciencias; Venezuela
Fil: Liu, Zongyuan. State University of New York; Estados Unidos
Fil: Gutiérrez, Ramón A.. Universidad Central de Venezuela. Facultad de Ciencias; Venezuela
Fil: Grinter, David G.. State University of New York; Estados Unidos
Fil: Carrasco, Javier. CIC EnergiGUNE; España
Fil: Senanayake, Sanjaya D.. Brookhaven National Laboratory; Estados Unidos
Fil: Rodriguez, José A.. Brookhaven National Laboratory; Estados Unidos
Fil: Ganduglia Pirovano, Maria Veronica. Consejo Superior de Investigaciones Científicas. Instituto de Catálisis y Petroleoquímica; España
description The results of core-level photoemission indicate that Ni-CeO2(111) surfaces with small or medium coverages of nickel are able to activate methane at 300 K, producing adsorbed CHx and COx (x = 2, 3) groups. Calculations based on density functional theory predict a relatively low activation energy of 0.6-0.7 eV for the cleavage of the first C-H bond in the adsorbed methane molecule. Ni and O centers of ceria work in a cooperative way in the dissociation of the C-H bond at room temperature, where a low Ni loading is crucial for the catalyst activity and stability. The strong electronic perturbations in the Ni nanoparticles produced by the ceria supports of varying natures, such as stoichiometric and reduced, result in a drastic change in their chemical properties toward methane adsorption and dissociation as well as the dry reforming of methane reaction. The coverage of Ni has a drastic effect on the ability of the system to dissociate methane and catalyze the dry re-forming process.
publishDate 2016
dc.date.none.fl_str_mv 2016-12
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/61045
Lustemberg, Pablo German; Ramírez, Pedro J.; Liu, Zongyuan; Gutiérrez, Ramón A.; Grinter, David G.; et al.; Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage; American Chemical Society; ACS Catalysis; 6; 12; 12-2016; 8184-8191
2155-5435
CONICET Digital
CONICET
url http://hdl.handle.net/11336/61045
identifier_str_mv Lustemberg, Pablo German; Ramírez, Pedro J.; Liu, Zongyuan; Gutiérrez, Ramón A.; Grinter, David G.; et al.; Room-Temperature Activation of Methane and Dry Re-forming with CO2 on Ni-CeO2(111) Surfaces: Effect of Ce3+ Sites and Metal-Support Interactions on C-H Bond Cleavage; American Chemical Society; ACS Catalysis; 6; 12; 12-2016; 8184-8191
2155-5435
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1021/acscatal.6b02360
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acscatal.6b02360
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
_version_ 1842979887878504448
score 12.993085

Publicaciones similares