Towards bond selective chemistry from first principles: Methane on metal surfaces

Autores
Shen, X. J.; Lozano, Ariel; Dong, W.; Busnengo, Heriberto Fabio; Yan, X. H.
Año de publicación
2014
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Controlling bond-selective chemical reactivity is of great importance and has a broad range of applications. Here, we present a molecular dynamics study of bond selective reactivity of methane and its deuterated isotopologues (i.e., CH4−xDx, x=0,1,2,3,4) on Ni(111) and Pt(111) from first principles calculations. Our simulations allow for reproducing the full C-H bond selectivity recently achieved experimentally via mode-specific vibrational excitation and explain its origin. Moreover, we also predict the hitherto unexplored influence of the molecular translational energy on such a selectivity as well as the conditions under which the full selectivity can be realized for the a priori less active C-D bond.
Fil: Shen, X. J.. Ecole Normale Supérieure de Lyon. Laboratoire de Chimie; Francia. Nanjing University of Aeronautics and Astronautics. College of Science; China
Fil: Lozano, Ariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); Argentina
Fil: Dong, W.. Ecole Normale Supérieure de Lyon. Laboratoire de Chimie; Francia
Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); Argentina
Fil: Yan, X. H.. Nanjing University of Aeronautics and Astronautics. College of Science; China
Materia
Methane
Adsorption
Dft
Forcefields
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:11336/6195
Acceder
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repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Towards bond selective chemistry from first principles: Methane on metal surfacesShen, X. J.Lozano, ArielDong, W.Busnengo, Heriberto FabioYan, X. H.MethaneAdsorptionDftForcefieldshttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1Controlling bond-selective chemical reactivity is of great importance and has a broad range of applications. Here, we present a molecular dynamics study of bond selective reactivity of methane and its deuterated isotopologues (i.e., CH4−xDx, x=0,1,2,3,4) on Ni(111) and Pt(111) from first principles calculations. Our simulations allow for reproducing the full C-H bond selectivity recently achieved experimentally via mode-specific vibrational excitation and explain its origin. Moreover, we also predict the hitherto unexplored influence of the molecular translational energy on such a selectivity as well as the conditions under which the full selectivity can be realized for the a priori less active C-D bond.Fil: Shen, X. J.. Ecole Normale Supérieure de Lyon. Laboratoire de Chimie; Francia. Nanjing University of Aeronautics and Astronautics. College of Science; ChinaFil: Lozano, Ariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); ArgentinaFil: Dong, W.. Ecole Normale Supérieure de Lyon. Laboratoire de Chimie; FranciaFil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); ArgentinaFil: Yan, X. H.. Nanjing University of Aeronautics and Astronautics. College of Science; ChinaAmerican Physical Society2014-01info: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/11336/6195Shen, X. J.; Lozano, Ariel; Dong, W.; Busnengo, Heriberto Fabio; Yan, X. H.; Towards bond selective chemistry from first principles: Methane on metal surfaces; American Physical Society; Physical Review Letters; 112; 1-2014; 46101-461010031-9007enginfo:eu-repo/semantics/altIdentifier/url/http://journals.aps.org/prl/abstract/10.1103/PhysRevLett.112.046101info:eu-repo/semantics/altIdentifier/doi/10.1103/PhysRevLett.112.046101info:eu-repo/semantics/altIdentifier/doi/info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:03:53Zoai:ri.conicet.gov.ar:11336/6195instacron: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:34982025-09-29 10:03:54.041CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Towards bond selective chemistry from first principles: Methane on metal surfaces
title Towards bond selective chemistry from first principles: Methane on metal surfaces
spellingShingle Towards bond selective chemistry from first principles: Methane on metal surfaces
Shen, X. J.
Methane
Adsorption
Dft
Forcefields
title_short Towards bond selective chemistry from first principles: Methane on metal surfaces
title_full Towards bond selective chemistry from first principles: Methane on metal surfaces
title_fullStr Towards bond selective chemistry from first principles: Methane on metal surfaces
title_full_unstemmed Towards bond selective chemistry from first principles: Methane on metal surfaces
title_sort Towards bond selective chemistry from first principles: Methane on metal surfaces
dc.creator.none.fl_str_mv Shen, X. J.
Lozano, Ariel
Dong, W.
Busnengo, Heriberto Fabio
Yan, X. H.
author Shen, X. J.
author_facet Shen, X. J.
Lozano, Ariel
Dong, W.
Busnengo, Heriberto Fabio
Yan, X. H.
author_role author
author2 Lozano, Ariel
Dong, W.
Busnengo, Heriberto Fabio
Yan, X. H.
author2_role author
author
author
author
dc.subject.none.fl_str_mv Methane
Adsorption
Dft
Forcefields
topic Methane
Adsorption
Dft
Forcefields
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Controlling bond-selective chemical reactivity is of great importance and has a broad range of applications. Here, we present a molecular dynamics study of bond selective reactivity of methane and its deuterated isotopologues (i.e., CH4−xDx, x=0,1,2,3,4) on Ni(111) and Pt(111) from first principles calculations. Our simulations allow for reproducing the full C-H bond selectivity recently achieved experimentally via mode-specific vibrational excitation and explain its origin. Moreover, we also predict the hitherto unexplored influence of the molecular translational energy on such a selectivity as well as the conditions under which the full selectivity can be realized for the a priori less active C-D bond.
Fil: Shen, X. J.. Ecole Normale Supérieure de Lyon. Laboratoire de Chimie; Francia. Nanjing University of Aeronautics and Astronautics. College of Science; China
Fil: Lozano, Ariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); Argentina
Fil: Dong, W.. Ecole Normale Supérieure de Lyon. Laboratoire de Chimie; Francia
Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); Argentina
Fil: Yan, X. H.. Nanjing University of Aeronautics and Astronautics. College of Science; China
description Controlling bond-selective chemical reactivity is of great importance and has a broad range of applications. Here, we present a molecular dynamics study of bond selective reactivity of methane and its deuterated isotopologues (i.e., CH4−xDx, x=0,1,2,3,4) on Ni(111) and Pt(111) from first principles calculations. Our simulations allow for reproducing the full C-H bond selectivity recently achieved experimentally via mode-specific vibrational excitation and explain its origin. Moreover, we also predict the hitherto unexplored influence of the molecular translational energy on such a selectivity as well as the conditions under which the full selectivity can be realized for the a priori less active C-D bond.
publishDate 2014
dc.date.none.fl_str_mv 2014-01
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/11336/6195
Shen, X. J.; Lozano, Ariel; Dong, W.; Busnengo, Heriberto Fabio; Yan, X. H.; Towards bond selective chemistry from first principles: Methane on metal surfaces; American Physical Society; Physical Review Letters; 112; 1-2014; 46101-46101
0031-9007
url http://hdl.handle.net/11336/6195
identifier_str_mv Shen, X. J.; Lozano, Ariel; Dong, W.; Busnengo, Heriberto Fabio; Yan, X. H.; Towards bond selective chemistry from first principles: Methane on metal surfaces; American Physical Society; Physical Review Letters; 112; 1-2014; 46101-46101
0031-9007
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://journals.aps.org/prl/abstract/10.1103/PhysRevLett.112.046101
info:eu-repo/semantics/altIdentifier/doi/10.1103/PhysRevLett.112.046101
info:eu-repo/semantics/altIdentifier/doi/
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 American Physical Society
publisher.none.fl_str_mv American Physical 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_ 1844613860251664384
score 13.070432

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