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 compositions Mamatkulov, Mikhail Yudanov, Ilya Bukhtiyarov, Andrey V. Neyman, Konstantin M. Nanopartícules Pal·ladi (Element químic) Compostos metàl·lics Aliatges Nanoparticles Palladium Metallic composites Alloys 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. MDPI https://hdl.handle.net/2445/174819
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
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
topic Nanopartícules
Pal·ladi (Element químic)
Compostos metàl·lics
Aliatges
Nanoparticles
Palladium
Metallic composites
Alloys
topic_facet 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
format article
status_str publishedVersion
url https://hdl.handle.net/2445/174819
eu_rights_str_mv openAccess
publisher MDPI
institution Universidad de Barcelona
collection Dipòsit Digital de la UB
reponame_str Dipòsit Digital de la UB
instname_str Universidad de Barcelona
_version_ 1878736360532082688
publishDateSort 2021
author_browse Bukhtiyarov, Andrey V.
Mamatkulov, Mikhail
Neyman, Konstantin M.
Yudanov, Ilya
publisherStr MDPI
score 6,8972664

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