Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals

Autores
Powell, Andrew D.; Gerrits, Nick; Tchakoua, Theophile; Somers, Mark F.; Busnengo, Heriberto Fabio; Meyer, Jörg; Kroes, Geert Jan; Doblhoff Dier, Katharina
Año de publicación
2024
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Predictive capability, accuracy, and affordability are essential features of a theory that is capable of describing dissociative chemisorption on a metal surface. This type of reaction is importantfor heterogeneous catalysis. Here we present an approach in which we use diffusion Monte Carlo (DMC) to pin the minimum barrier height and construct a density functional that reproduces this value. This predictive approach allows the construction of a potential energy surface at the cost of density functional theory while retaining near DMC accuracy. Scrutinizing effects of energy dissipation andquantum tunneling, dynamics calculations suggest the approach to be of near chemical accuracy, reproducing molecular beam sticking experiments for the showcase H2 + Al(110) system to ∼1.4 kcal/mol.
Fil: Powell, Andrew D.. Leiden University; Países Bajos
Fil: Gerrits, Nick. Leiden University; Países Bajos
Fil: Tchakoua, Theophile. Leiden University; Países Bajos
Fil: Somers, Mark F.. Leiden University; Países Bajos
Fil: Busnengo, Heriberto Fabio. 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: Meyer, Jörg. Leiden University; Países Bajos
Fil: Kroes, Geert Jan. Leiden University; Países Bajos
Fil: Doblhoff Dier, Katharina. Leiden University; Países Bajos
Materia
Diffusion Montecarlo
Density Functional Theory
Surfaces
Molecular Dynamics
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/265383
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/265383
network_acronym_str CONICETDig
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network_name_str CONICET Digital (CONICET)
spelling Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on MetalsPowell, Andrew D.Gerrits, NickTchakoua, TheophileSomers, Mark F.Busnengo, Heriberto FabioMeyer, JörgKroes, Geert JanDoblhoff Dier, KatharinaDiffusion MontecarloDensity Functional TheorySurfacesMolecular Dynamicshttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1Predictive capability, accuracy, and affordability are essential features of a theory that is capable of describing dissociative chemisorption on a metal surface. This type of reaction is importantfor heterogeneous catalysis. Here we present an approach in which we use diffusion Monte Carlo (DMC) to pin the minimum barrier height and construct a density functional that reproduces this value. This predictive approach allows the construction of a potential energy surface at the cost of density functional theory while retaining near DMC accuracy. Scrutinizing effects of energy dissipation andquantum tunneling, dynamics calculations suggest the approach to be of near chemical accuracy, reproducing molecular beam sticking experiments for the showcase H2 + Al(110) system to ∼1.4 kcal/mol.Fil: Powell, Andrew D.. Leiden University; Países BajosFil: Gerrits, Nick. Leiden University; Países BajosFil: Tchakoua, Theophile. Leiden University; Países BajosFil: Somers, Mark F.. Leiden University; Países BajosFil: Busnengo, Heriberto Fabio. 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: Meyer, Jörg. Leiden University; Países BajosFil: Kroes, Geert Jan. Leiden University; Países BajosFil: Doblhoff Dier, Katharina. Leiden University; Países BajosAmerican Chemical Society2024-01info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/265383Powell, Andrew D.; Gerrits, Nick; Tchakoua, Theophile; Somers, Mark F.; Busnengo, Heriberto Fabio; et al.; Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals; American Chemical Society; The Journal of Physical Chemistry Letters; 15; 1; 1-2024; 307-3151948-7185CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpclett.3c02972info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpclett.3c02972info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:55:55Zoai:ri.conicet.gov.ar:11336/265383instacron: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 09:55:55.554CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals
title Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals
spellingShingle Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals
Powell, Andrew D.
Diffusion Montecarlo
Density Functional Theory
Surfaces
Molecular Dynamics
title_short Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals
title_full Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals
title_fullStr Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals
title_full_unstemmed Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals
title_sort Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals
dc.creator.none.fl_str_mv Powell, Andrew D.
Gerrits, Nick
Tchakoua, Theophile
Somers, Mark F.
Busnengo, Heriberto Fabio
Meyer, Jörg
Kroes, Geert Jan
Doblhoff Dier, Katharina
author Powell, Andrew D.
author_facet Powell, Andrew D.
Gerrits, Nick
Tchakoua, Theophile
Somers, Mark F.
Busnengo, Heriberto Fabio
Meyer, Jörg
Kroes, Geert Jan
Doblhoff Dier, Katharina
author_role author
author2 Gerrits, Nick
Tchakoua, Theophile
Somers, Mark F.
Busnengo, Heriberto Fabio
Meyer, Jörg
Kroes, Geert Jan
Doblhoff Dier, Katharina
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Diffusion Montecarlo
Density Functional Theory
Surfaces
Molecular Dynamics
topic Diffusion Montecarlo
Density Functional Theory
Surfaces
Molecular Dynamics
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Predictive capability, accuracy, and affordability are essential features of a theory that is capable of describing dissociative chemisorption on a metal surface. This type of reaction is importantfor heterogeneous catalysis. Here we present an approach in which we use diffusion Monte Carlo (DMC) to pin the minimum barrier height and construct a density functional that reproduces this value. This predictive approach allows the construction of a potential energy surface at the cost of density functional theory while retaining near DMC accuracy. Scrutinizing effects of energy dissipation andquantum tunneling, dynamics calculations suggest the approach to be of near chemical accuracy, reproducing molecular beam sticking experiments for the showcase H2 + Al(110) system to ∼1.4 kcal/mol.
Fil: Powell, Andrew D.. Leiden University; Países Bajos
Fil: Gerrits, Nick. Leiden University; Países Bajos
Fil: Tchakoua, Theophile. Leiden University; Países Bajos
Fil: Somers, Mark F.. Leiden University; Países Bajos
Fil: Busnengo, Heriberto Fabio. 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: Meyer, Jörg. Leiden University; Países Bajos
Fil: Kroes, Geert Jan. Leiden University; Países Bajos
Fil: Doblhoff Dier, Katharina. Leiden University; Países Bajos
description Predictive capability, accuracy, and affordability are essential features of a theory that is capable of describing dissociative chemisorption on a metal surface. This type of reaction is importantfor heterogeneous catalysis. Here we present an approach in which we use diffusion Monte Carlo (DMC) to pin the minimum barrier height and construct a density functional that reproduces this value. This predictive approach allows the construction of a potential energy surface at the cost of density functional theory while retaining near DMC accuracy. Scrutinizing effects of energy dissipation andquantum tunneling, dynamics calculations suggest the approach to be of near chemical accuracy, reproducing molecular beam sticking experiments for the showcase H2 + Al(110) system to ∼1.4 kcal/mol.
publishDate 2024
dc.date.none.fl_str_mv 2024-01
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/11336/265383
Powell, Andrew D.; Gerrits, Nick; Tchakoua, Theophile; Somers, Mark F.; Busnengo, Heriberto Fabio; et al.; Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals; American Chemical Society; The Journal of Physical Chemistry Letters; 15; 1; 1-2024; 307-315
1948-7185
CONICET Digital
CONICET
url http://hdl.handle.net/11336/265383
identifier_str_mv Powell, Andrew D.; Gerrits, Nick; Tchakoua, Theophile; Somers, Mark F.; Busnengo, Heriberto Fabio; et al.; Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals; American Chemical Society; The Journal of Physical Chemistry Letters; 15; 1; 1-2024; 307-315
1948-7185
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpclett.3c02972
info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpclett.3c02972
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/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_ 1844613682955288576
score 13.070432

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