Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface

Autores
Chen, Jian Cheng; Ramos Acevedo, Maximiliano; Arasa, Carina; Juanes Marcos, Juan Carlos; Somers, Mark F.; Martinez, Alejandra Elisa; Díaz, Cristina; Olsen, Roar A.; Kroes, Geert Jan
Año de publicación
2012
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The dissociation of H2 on Ti-covered Al surfaces is relevant to the rehydrogenation and dehydrogenation of the NaAlH_4 hydrogen storage material. The energetically most stable structure for a 1/2 monolayer of Ti deposited on the Al (100) surface has the Ti atoms in the second layer with a c(2×2) structure, as has been confirmed by both low-energy electron diffraction and low-energy ion scattering experiments and density functional theory studies. we investigate the dynamics of H2 dissociation on a slab model of this Ti/Al(100) surface. Two six-dimensional potential energy surfaces (PESs) have been built for this H_2 + Ti/Al(100) system, based on the density functional theory PW91 and RPBE exchange?correlation functionals. In the PW91 (RPBE) PES, the lowest H_2 dissociation barrier is found to be 0.65 (0.84) eV, with the minimum energy path occurring for H2 dissociating above the bridge to top sites. Using both PESs, H2 dissociation probabilities are calculated using the classical trajectory (CT), the quasi-classical trajectory (QCT), and the time-dependent wave-packet methods. We find that the QCT H_2 dissociation probabilities are in good agreement with the quantum dynamics results in the collision energy range studied up to 1.0 eV. We have also performed molecular beam simulations and present predictions for molecular beam experiments. Our molecular beam simulations show that H2 dissociation on the 1/2 ML Ti/Al(100) surface is an activated process, and the reaction probability is found to be 6.9% for the PW91 functional and 1.8% for the RPBE at a nozzle temperature of 1700 K. Finally, we have also calculated H_2 dissociation rate constants by applying transition state theory and the QCT method, which could be relevant to modeling Ti-catalyzed rehydrogenation and dehydrogenation of NaAlH4.
Fil: Chen, Jian Cheng. Leiden University; Países Bajos
Fil: Ramos Acevedo, Maximiliano. 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: Arasa, Carina. Leiden University; Países Bajos
Fil: Juanes Marcos, Juan Carlos. Leiden University; Países Bajos
Fil: Somers, Mark F.. Leiden University; Países Bajos
Fil: Martinez, Alejandra Elisa. 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: Díaz, Cristina. Universidad Autónoma de Madrid; España
Fil: Olsen, Roar A.. Leiden University; Países Bajos
Fil: Kroes, Geert Jan. Leiden University; Países Bajos
Materia
SURFACES
BIMETALLIC
ADSORPTION
MOLECULES
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:11336/269542
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/269542
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surfaceChen, Jian ChengRamos Acevedo, MaximilianoArasa, CarinaJuanes Marcos, Juan CarlosSomers, Mark F.Martinez, Alejandra ElisaDíaz, CristinaOlsen, Roar A.Kroes, Geert JanSURFACESBIMETALLICADSORPTIONMOLECULEShttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1The dissociation of H2 on Ti-covered Al surfaces is relevant to the rehydrogenation and dehydrogenation of the NaAlH_4 hydrogen storage material. The energetically most stable structure for a 1/2 monolayer of Ti deposited on the Al (100) surface has the Ti atoms in the second layer with a c(2×2) structure, as has been confirmed by both low-energy electron diffraction and low-energy ion scattering experiments and density functional theory studies. we investigate the dynamics of H2 dissociation on a slab model of this Ti/Al(100) surface. Two six-dimensional potential energy surfaces (PESs) have been built for this H_2 + Ti/Al(100) system, based on the density functional theory PW91 and RPBE exchange?correlation functionals. In the PW91 (RPBE) PES, the lowest H_2 dissociation barrier is found to be 0.65 (0.84) eV, with the minimum energy path occurring for H2 dissociating above the bridge to top sites. Using both PESs, H2 dissociation probabilities are calculated using the classical trajectory (CT), the quasi-classical trajectory (QCT), and the time-dependent wave-packet methods. We find that the QCT H_2 dissociation probabilities are in good agreement with the quantum dynamics results in the collision energy range studied up to 1.0 eV. We have also performed molecular beam simulations and present predictions for molecular beam experiments. Our molecular beam simulations show that H2 dissociation on the 1/2 ML Ti/Al(100) surface is an activated process, and the reaction probability is found to be 6.9% for the PW91 functional and 1.8% for the RPBE at a nozzle temperature of 1700 K. Finally, we have also calculated H_2 dissociation rate constants by applying transition state theory and the QCT method, which could be relevant to modeling Ti-catalyzed rehydrogenation and dehydrogenation of NaAlH4.Fil: Chen, Jian Cheng. Leiden University; Países BajosFil: Ramos Acevedo, Maximiliano. 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: Arasa, Carina. Leiden University; Países BajosFil: Juanes Marcos, Juan Carlos. Leiden University; Países BajosFil: Somers, Mark F.. Leiden University; Países BajosFil: Martinez, Alejandra Elisa. 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: Díaz, Cristina. Universidad Autónoma de Madrid; EspañaFil: Olsen, Roar A.. Leiden University; Países BajosFil: Kroes, Geert Jan. Leiden University; Países BajosRoyal Society of Chemistry2012-02info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/269542Chen, Jian Cheng ; Ramos Acevedo, Maximiliano; Arasa, Carina; Juanes Marcos, Juan Carlos; Somers, Mark F.; et al.; Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 14; 9; 2-2012; 3234-32471463-9076CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.rsc.org/en/content/articlelanding/2012/cp/c2cp23693ainfo:eu-repo/semantics/altIdentifier/doi/10.1039/C2CP23693Ainfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2026-01-14T11:53:58Zoai:ri.conicet.gov.ar:11336/269542instacron: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:34982026-01-14 11:53:58.88CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface
title Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface
spellingShingle Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface
Chen, Jian Cheng
SURFACES
BIMETALLIC
ADSORPTION
MOLECULES
title_short Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface
title_full Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface
title_fullStr Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface
title_full_unstemmed Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface
title_sort Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface
dc.creator.none.fl_str_mv Chen, Jian Cheng
Ramos Acevedo, Maximiliano
Arasa, Carina
Juanes Marcos, Juan Carlos
Somers, Mark F.
Martinez, Alejandra Elisa
Díaz, Cristina
Olsen, Roar A.
Kroes, Geert Jan
author Chen, Jian Cheng
author_facet Chen, Jian Cheng
Ramos Acevedo, Maximiliano
Arasa, Carina
Juanes Marcos, Juan Carlos
Somers, Mark F.
Martinez, Alejandra Elisa
Díaz, Cristina
Olsen, Roar A.
Kroes, Geert Jan
author_role author
author2 Ramos Acevedo, Maximiliano
Arasa, Carina
Juanes Marcos, Juan Carlos
Somers, Mark F.
Martinez, Alejandra Elisa
Díaz, Cristina
Olsen, Roar A.
Kroes, Geert Jan
author2_role author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv SURFACES
BIMETALLIC
ADSORPTION
MOLECULES
topic SURFACES
BIMETALLIC
ADSORPTION
MOLECULES
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The dissociation of H2 on Ti-covered Al surfaces is relevant to the rehydrogenation and dehydrogenation of the NaAlH_4 hydrogen storage material. The energetically most stable structure for a 1/2 monolayer of Ti deposited on the Al (100) surface has the Ti atoms in the second layer with a c(2×2) structure, as has been confirmed by both low-energy electron diffraction and low-energy ion scattering experiments and density functional theory studies. we investigate the dynamics of H2 dissociation on a slab model of this Ti/Al(100) surface. Two six-dimensional potential energy surfaces (PESs) have been built for this H_2 + Ti/Al(100) system, based on the density functional theory PW91 and RPBE exchange?correlation functionals. In the PW91 (RPBE) PES, the lowest H_2 dissociation barrier is found to be 0.65 (0.84) eV, with the minimum energy path occurring for H2 dissociating above the bridge to top sites. Using both PESs, H2 dissociation probabilities are calculated using the classical trajectory (CT), the quasi-classical trajectory (QCT), and the time-dependent wave-packet methods. We find that the QCT H_2 dissociation probabilities are in good agreement with the quantum dynamics results in the collision energy range studied up to 1.0 eV. We have also performed molecular beam simulations and present predictions for molecular beam experiments. Our molecular beam simulations show that H2 dissociation on the 1/2 ML Ti/Al(100) surface is an activated process, and the reaction probability is found to be 6.9% for the PW91 functional and 1.8% for the RPBE at a nozzle temperature of 1700 K. Finally, we have also calculated H_2 dissociation rate constants by applying transition state theory and the QCT method, which could be relevant to modeling Ti-catalyzed rehydrogenation and dehydrogenation of NaAlH4.
Fil: Chen, Jian Cheng. Leiden University; Países Bajos
Fil: Ramos Acevedo, Maximiliano. 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: Arasa, Carina. Leiden University; Países Bajos
Fil: Juanes Marcos, Juan Carlos. Leiden University; Países Bajos
Fil: Somers, Mark F.. Leiden University; Países Bajos
Fil: Martinez, Alejandra Elisa. 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: Díaz, Cristina. Universidad Autónoma de Madrid; España
Fil: Olsen, Roar A.. Leiden University; Países Bajos
Fil: Kroes, Geert Jan. Leiden University; Países Bajos
description The dissociation of H2 on Ti-covered Al surfaces is relevant to the rehydrogenation and dehydrogenation of the NaAlH_4 hydrogen storage material. The energetically most stable structure for a 1/2 monolayer of Ti deposited on the Al (100) surface has the Ti atoms in the second layer with a c(2×2) structure, as has been confirmed by both low-energy electron diffraction and low-energy ion scattering experiments and density functional theory studies. we investigate the dynamics of H2 dissociation on a slab model of this Ti/Al(100) surface. Two six-dimensional potential energy surfaces (PESs) have been built for this H_2 + Ti/Al(100) system, based on the density functional theory PW91 and RPBE exchange?correlation functionals. In the PW91 (RPBE) PES, the lowest H_2 dissociation barrier is found to be 0.65 (0.84) eV, with the minimum energy path occurring for H2 dissociating above the bridge to top sites. Using both PESs, H2 dissociation probabilities are calculated using the classical trajectory (CT), the quasi-classical trajectory (QCT), and the time-dependent wave-packet methods. We find that the QCT H_2 dissociation probabilities are in good agreement with the quantum dynamics results in the collision energy range studied up to 1.0 eV. We have also performed molecular beam simulations and present predictions for molecular beam experiments. Our molecular beam simulations show that H2 dissociation on the 1/2 ML Ti/Al(100) surface is an activated process, and the reaction probability is found to be 6.9% for the PW91 functional and 1.8% for the RPBE at a nozzle temperature of 1700 K. Finally, we have also calculated H_2 dissociation rate constants by applying transition state theory and the QCT method, which could be relevant to modeling Ti-catalyzed rehydrogenation and dehydrogenation of NaAlH4.
publishDate 2012
dc.date.none.fl_str_mv 2012-02
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/11336/269542
Chen, Jian Cheng ; Ramos Acevedo, Maximiliano; Arasa, Carina; Juanes Marcos, Juan Carlos; Somers, Mark F.; et al.; Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 14; 9; 2-2012; 3234-3247
1463-9076
CONICET Digital
CONICET
url http://hdl.handle.net/11336/269542
identifier_str_mv Chen, Jian Cheng ; Ramos Acevedo, Maximiliano; Arasa, Carina; Juanes Marcos, Juan Carlos; Somers, Mark F.; et al.; Dynamics of H2 dissociation on the 1/2 ML c(2 × 2)-Ti/Al(100) surface; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 14; 9; 2-2012; 3234-3247
1463-9076
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://pubs.rsc.org/en/content/articlelanding/2012/cp/c2cp23693a
info:eu-repo/semantics/altIdentifier/doi/10.1039/C2CP23693A
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
application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
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
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score 13.113929

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