Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective

Autores
Gómez, Guillermina; Belelli, Patricia Gabriela; Cabeza, Gabriela Fernanda; Castellani, Norberto Jorge
Año de publicación
2014
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The partial hydrogenation of 1,3-butadiene (13BD) to several C4H8 products, including 1-butene (1B), 2-butene (2B) and butan-1,3-diyl (B13R), on both Pd/Ni(1 1 1) and Pd3/Ni(1 1 1) bimetallic surfaces was theoretically investigated using DFT methods. For that purpose, different intermediates C4H7 and C4H8 radical species were evaluated according to the Horiuti–Polanyi mechanism performed in two sequential steps. The whole process was found to be exothermic on Pd/Ni(1 1 1) and endothermic on Pd3/Ni(1 1 1). Furthermore, the former surface, where the intermediate adsorptions are more favorable, exhibits lower activation barriers than Pd3/Ni(1 1 1). On both surfaces, the B13R formation is associated with high transition state energies through the pathways studied here; for this reason, it is extremely improbable to obtain B13R. Our calculations predict that on the Pd/Ni(1 1 1) catalyst model, the products would be mainly the butene isomers, with a little more selectivity toward 2B, in contrast to the pure Pd surface and in agreement with experimental data.
Fil: Gómez, Guillermina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Belelli, Patricia Gabriela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Cabeza, Gabriela Fernanda. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Castellani, Norberto Jorge. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Materia
1,3-Butadiene
Partial Hydrogenation
Pd-Ni Surfaces
Periodic Dft
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/30951
Acceder
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network_name_str CONICET Digital (CONICET)
spelling Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspectiveGómez, GuillerminaBelelli, Patricia GabrielaCabeza, Gabriela FernandaCastellani, Norberto Jorge1,3-ButadienePartial HydrogenationPd-Ni SurfacesPeriodic Dfthttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2The partial hydrogenation of 1,3-butadiene (13BD) to several C4H8 products, including 1-butene (1B), 2-butene (2B) and butan-1,3-diyl (B13R), on both Pd/Ni(1 1 1) and Pd3/Ni(1 1 1) bimetallic surfaces was theoretically investigated using DFT methods. For that purpose, different intermediates C4H7 and C4H8 radical species were evaluated according to the Horiuti–Polanyi mechanism performed in two sequential steps. The whole process was found to be exothermic on Pd/Ni(1 1 1) and endothermic on Pd3/Ni(1 1 1). Furthermore, the former surface, where the intermediate adsorptions are more favorable, exhibits lower activation barriers than Pd3/Ni(1 1 1). On both surfaces, the B13R formation is associated with high transition state energies through the pathways studied here; for this reason, it is extremely improbable to obtain B13R. Our calculations predict that on the Pd/Ni(1 1 1) catalyst model, the products would be mainly the butene isomers, with a little more selectivity toward 2B, in contrast to the pure Pd surface and in agreement with experimental data.Fil: Gómez, Guillermina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaFil: Belelli, Patricia Gabriela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaFil: Cabeza, Gabriela Fernanda. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaFil: Castellani, Norberto Jorge. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaElsevier Science2014-07info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/30951Gómez, Guillermina; Castellani, Norberto Jorge; Cabeza, Gabriela Fernanda; Belelli, Patricia Gabriela; Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective; Elsevier Science; Journal of Molecular Catalysis A: Chemical; 394; 7-2014; 151-1611381-1169CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.molcata.2014.06.035info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S1381116914002866info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-10T13:12:32Zoai:ri.conicet.gov.ar:11336/30951instacron: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 13:12:32.95CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective
title Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective
spellingShingle Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective
Gómez, Guillermina
1,3-Butadiene
Partial Hydrogenation
Pd-Ni Surfaces
Periodic Dft
title_short Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective
title_full Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective
title_fullStr Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective
title_full_unstemmed Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective
title_sort Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective
dc.creator.none.fl_str_mv Gómez, Guillermina
Belelli, Patricia Gabriela
Cabeza, Gabriela Fernanda
Castellani, Norberto Jorge
author Gómez, Guillermina
author_facet Gómez, Guillermina
Belelli, Patricia Gabriela
Cabeza, Gabriela Fernanda
Castellani, Norberto Jorge
author_role author
author2 Belelli, Patricia Gabriela
Cabeza, Gabriela Fernanda
Castellani, Norberto Jorge
author2_role author
author
author
dc.subject.none.fl_str_mv 1,3-Butadiene
Partial Hydrogenation
Pd-Ni Surfaces
Periodic Dft
topic 1,3-Butadiene
Partial Hydrogenation
Pd-Ni Surfaces
Periodic Dft
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv The partial hydrogenation of 1,3-butadiene (13BD) to several C4H8 products, including 1-butene (1B), 2-butene (2B) and butan-1,3-diyl (B13R), on both Pd/Ni(1 1 1) and Pd3/Ni(1 1 1) bimetallic surfaces was theoretically investigated using DFT methods. For that purpose, different intermediates C4H7 and C4H8 radical species were evaluated according to the Horiuti–Polanyi mechanism performed in two sequential steps. The whole process was found to be exothermic on Pd/Ni(1 1 1) and endothermic on Pd3/Ni(1 1 1). Furthermore, the former surface, where the intermediate adsorptions are more favorable, exhibits lower activation barriers than Pd3/Ni(1 1 1). On both surfaces, the B13R formation is associated with high transition state energies through the pathways studied here; for this reason, it is extremely improbable to obtain B13R. Our calculations predict that on the Pd/Ni(1 1 1) catalyst model, the products would be mainly the butene isomers, with a little more selectivity toward 2B, in contrast to the pure Pd surface and in agreement with experimental data.
Fil: Gómez, Guillermina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Belelli, Patricia Gabriela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Cabeza, Gabriela Fernanda. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Castellani, Norberto Jorge. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
description The partial hydrogenation of 1,3-butadiene (13BD) to several C4H8 products, including 1-butene (1B), 2-butene (2B) and butan-1,3-diyl (B13R), on both Pd/Ni(1 1 1) and Pd3/Ni(1 1 1) bimetallic surfaces was theoretically investigated using DFT methods. For that purpose, different intermediates C4H7 and C4H8 radical species were evaluated according to the Horiuti–Polanyi mechanism performed in two sequential steps. The whole process was found to be exothermic on Pd/Ni(1 1 1) and endothermic on Pd3/Ni(1 1 1). Furthermore, the former surface, where the intermediate adsorptions are more favorable, exhibits lower activation barriers than Pd3/Ni(1 1 1). On both surfaces, the B13R formation is associated with high transition state energies through the pathways studied here; for this reason, it is extremely improbable to obtain B13R. Our calculations predict that on the Pd/Ni(1 1 1) catalyst model, the products would be mainly the butene isomers, with a little more selectivity toward 2B, in contrast to the pure Pd surface and in agreement with experimental data.
publishDate 2014
dc.date.none.fl_str_mv 2014-07
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/11336/30951
Gómez, Guillermina; Castellani, Norberto Jorge; Cabeza, Gabriela Fernanda; Belelli, Patricia Gabriela; Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective; Elsevier Science; Journal of Molecular Catalysis A: Chemical; 394; 7-2014; 151-161
1381-1169
CONICET Digital
CONICET
url http://hdl.handle.net/11336/30951
identifier_str_mv Gómez, Guillermina; Castellani, Norberto Jorge; Cabeza, Gabriela Fernanda; Belelli, Patricia Gabriela; Evaluating Pd–Ni layered catalysts for selective hydrogenation of 1,3-butadiene: a theoretical perspective; Elsevier Science; Journal of Molecular Catalysis A: Chemical; 394; 7-2014; 151-161
1381-1169
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.molcata.2014.06.035
info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S1381116914002866
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science
publisher.none.fl_str_mv Elsevier Science
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 12.993085

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