Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositions

Structure of model bimetallic PdAu nanoparticles is analyzed aiming to find Pd:Au ratios optimal for existence of Pd1 single-atom surface sites inside outer Au atomic shell. The analysis is performed using density-functional theory (DFT) calculations and topological approach based on DFT-parameteriz...

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Autores: Mamatkulov, Mikhail, Yudanov, Ilya, Bukhtiyarov, Andrey V., Neyman, Konstantin M.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2021
País:España
Institución:Universidad de Barcelona
Repositorio:Dipòsit Digital de la UB
OAI Identifier:oai:diposit.ub.edu:2445/174819
Acceso en línea:https://hdl.handle.net/2445/174819
Access Level:acceso abierto
Palabra clave:Nanopartícules
Pal·ladi (Element químic)
Compostos metàl·lics
Aliatges
Nanoparticles
Palladium
Metallic composites
Alloys
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spelling Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositionsMamatkulov, MikhailYudanov, IlyaBukhtiyarov, Andrey V.Neyman, Konstantin M.NanopartículesPal·ladi (Element químic)Compostos metàl·licsAliatgesNanoparticlesPalladiumMetallic compositesAlloysStructure of model bimetallic PdAu nanoparticles is analyzed aiming to find Pd:Au ratios optimal for existence of Pd1 single-atom surface sites inside outer Au atomic shell. The analysis is performed using density-functional theory (DFT) calculations and topological approach based on DFT-parameterized topological energy expression. The number of the surface Pd1 sites in the absence of adsorbates is calculated as a function of Pd concentration inside the particles. At low Pd contents none of the Pd atoms emerge on the surface in the lowest-energy chemical orderings. However, surface Pd1 sites become stable, when Pd content inside a Pd-Au particle reaches ca. 60%. Further Pd content increase up to almost pure Pd core is accompanied by increased concentration of surface Pd atoms, mostly as Pd1 sites, although larger Pd ensembles as dimers and linear trimers are formed as well. Analysis of the chemical orderings inside PdAu nanoparticles at different Pd contents revealed that enrichment of the subsurface shell by Pd with predominant occupation of its edge positions precedes emergence of Pd surface species.MDPI2021info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttps://hdl.handle.net/2445/174819Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaInglésReproducció del document publicat a: https://doi.org/10.3390/nano11010122Nanomaterials, 2021, vol. 11(1), num. 122https://doi.org/10.3390/nano11010122cc-by (c) Mamatkulov, Mikhail et al., 2021http://creativecommons.org/licenses/by/3.0/esinfo:eu-repo/semantics/openAccessoai:diposit.ub.edu:2445/1748192026-05-27T06:46:51Z
dc.title.none.fl_str_mv Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositions
title Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositions
spellingShingle Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositions
Mamatkulov, Mikhail
Nanopartícules
Pal·ladi (Element químic)
Compostos metàl·lics
Aliatges
Nanoparticles
Palladium
Metallic composites
Alloys
title_short Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositions
title_full Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositions
title_fullStr Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositions
title_full_unstemmed Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositions
title_sort Pd single-atom sites on the surface of PdAu nanoparticles: A DFT-based Topological search for suitable compositions
dc.creator.none.fl_str_mv Mamatkulov, Mikhail
Yudanov, Ilya
Bukhtiyarov, Andrey V.
Neyman, Konstantin M.
author Mamatkulov, Mikhail
author_facet Mamatkulov, Mikhail
Yudanov, Ilya
Bukhtiyarov, Andrey V.
Neyman, Konstantin M.
author_role author
author2 Yudanov, Ilya
Bukhtiyarov, Andrey V.
Neyman, Konstantin M.
author2_role author
author
author
dc.subject.none.fl_str_mv Nanopartícules
Pal·ladi (Element químic)
Compostos metàl·lics
Aliatges
Nanoparticles
Palladium
Metallic composites
Alloys
topic Nanopartícules
Pal·ladi (Element químic)
Compostos metàl·lics
Aliatges
Nanoparticles
Palladium
Metallic composites
Alloys
description Structure of model bimetallic PdAu nanoparticles is analyzed aiming to find Pd:Au ratios optimal for existence of Pd1 single-atom surface sites inside outer Au atomic shell. The analysis is performed using density-functional theory (DFT) calculations and topological approach based on DFT-parameterized topological energy expression. The number of the surface Pd1 sites in the absence of adsorbates is calculated as a function of Pd concentration inside the particles. At low Pd contents none of the Pd atoms emerge on the surface in the lowest-energy chemical orderings. However, surface Pd1 sites become stable, when Pd content inside a Pd-Au particle reaches ca. 60%. Further Pd content increase up to almost pure Pd core is accompanied by increased concentration of surface Pd atoms, mostly as Pd1 sites, although larger Pd ensembles as dimers and linear trimers are formed as well. Analysis of the chemical orderings inside PdAu nanoparticles at different Pd contents revealed that enrichment of the subsurface shell by Pd with predominant occupation of its edge positions precedes emergence of Pd surface species.
publishDate 2021
dc.date.none.fl_str_mv 2021
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/174819
url https://hdl.handle.net/2445/174819
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció del document publicat a: https://doi.org/10.3390/nano11010122
Nanomaterials, 2021, vol. 11(1), num. 122
https://doi.org/10.3390/nano11010122
dc.rights.none.fl_str_mv cc-by (c) Mamatkulov, Mikhail et al., 2021
http://creativecommons.org/licenses/by/3.0/es
info:eu-repo/semantics/openAccess
rights_invalid_str_mv cc-by (c) Mamatkulov, Mikhail et al., 2021
http://creativecommons.org/licenses/by/3.0/es
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv MDPI
publisher.none.fl_str_mv MDPI
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Dipòsit Digital de la UB
instname:Universidad de Barcelona
instname_str Universidad de Barcelona
reponame_str Dipòsit Digital de la UB
collection Dipòsit Digital de la UB
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.301603

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