Versatile Optimization of Chemical Ordering in Bimetallic Nanoparticles

Handle URI:
http://hdl.handle.net/10754/623253
Title:
Versatile Optimization of Chemical Ordering in Bimetallic Nanoparticles
Authors:
Kovács, Gábor; Kozlov, Sergey M.; Neyman, Konstantin M. ( 0000-0002-5242-5567 )
Abstract:
Chemical ordering in bimetallic nanocrystallites can now be efficiently determined by density-functional calculations with the help of topological energy expressions. Herein, we deal with extending the usage of that computational scheme. We show that it enables one to structurally characterize bimetallic nanoparticles of less regular shapes than previously studied magic-type particles. In fcc Pd–Au particles of different shapes (cuboctahedral Pd58Au58, C3v Pd61Au61, cubic Pd68Au67, and truncated octahedral Pd70Au70), we identify the surface segregation of gold as the driving force to the lowest-energy chemical ordering. We applied the calculated descriptor values quantifying the segregation propensity of Au and energies of Pd–Au bonds in these ∼1.5 nm large particles to optimize and analyze the chemical ordering in 3.7–6 nm large Pd–Au particles. We also discuss how to predict the chemical ordering in nanoalloys at elevated temperatures. The present study paves the way to advanced structural investigations of nanoalloys to substantially accelerate their knowledge-driven engineering and manufacturing.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division
Citation:
Kovács G, Kozlov SM, Neyman KM (2017) Versatile Optimization of Chemical Ordering in Bimetallic Nanoparticles. The Journal of Physical Chemistry C. Available: http://dx.doi.org/10.1021/acs.jpcc.6b11923.
Publisher:
American Chemical Society (ACS)
Journal:
The Journal of Physical Chemistry C
Issue Date:
5-Jan-2017
DOI:
10.1021/acs.jpcc.6b11923
Type:
Article
ISSN:
1932-7447; 1932-7455
Sponsors:
This study was supported by the European Commission (FP7-NMP.2012.1.1-1 project ChipCAT, ref. 310191), the Spanish MINECO (grants CTQ2012-34969, CTQ2015-64618-R with FEDER), and the Generalitat de Catalunya (projects 2014SGR97 and XRQTC). The authors thank the Red Española de Supercomputación for the computer resources at memento and the technical support provided by caesaraugusta (QCM-2015-1-0025, QCM-2015-2-0016).
Additional Links:
http://pubs.acs.org/doi/full/10.1021/acs.jpcc.6b11923
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorKovács, Gáboren
dc.contributor.authorKozlov, Sergey M.en
dc.contributor.authorNeyman, Konstantin M.en
dc.date.accessioned2017-04-17T11:33:47Z-
dc.date.available2017-04-17T11:33:47Z-
dc.date.issued2017-01-05en
dc.identifier.citationKovács G, Kozlov SM, Neyman KM (2017) Versatile Optimization of Chemical Ordering in Bimetallic Nanoparticles. The Journal of Physical Chemistry C. Available: http://dx.doi.org/10.1021/acs.jpcc.6b11923.en
dc.identifier.issn1932-7447en
dc.identifier.issn1932-7455en
dc.identifier.doi10.1021/acs.jpcc.6b11923en
dc.identifier.urihttp://hdl.handle.net/10754/623253-
dc.description.abstractChemical ordering in bimetallic nanocrystallites can now be efficiently determined by density-functional calculations with the help of topological energy expressions. Herein, we deal with extending the usage of that computational scheme. We show that it enables one to structurally characterize bimetallic nanoparticles of less regular shapes than previously studied magic-type particles. In fcc Pd–Au particles of different shapes (cuboctahedral Pd58Au58, C3v Pd61Au61, cubic Pd68Au67, and truncated octahedral Pd70Au70), we identify the surface segregation of gold as the driving force to the lowest-energy chemical ordering. We applied the calculated descriptor values quantifying the segregation propensity of Au and energies of Pd–Au bonds in these ∼1.5 nm large particles to optimize and analyze the chemical ordering in 3.7–6 nm large Pd–Au particles. We also discuss how to predict the chemical ordering in nanoalloys at elevated temperatures. The present study paves the way to advanced structural investigations of nanoalloys to substantially accelerate their knowledge-driven engineering and manufacturing.en
dc.description.sponsorshipThis study was supported by the European Commission (FP7-NMP.2012.1.1-1 project ChipCAT, ref. 310191), the Spanish MINECO (grants CTQ2012-34969, CTQ2015-64618-R with FEDER), and the Generalitat de Catalunya (projects 2014SGR97 and XRQTC). The authors thank the Red Española de Supercomputación for the computer resources at memento and the technical support provided by caesaraugusta (QCM-2015-1-0025, QCM-2015-2-0016).en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/full/10.1021/acs.jpcc.6b11923en
dc.rightsThis is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.en
dc.rights.urihttp://pubs.acs.org/page/policy/authorchoice_termsofuse.htmlen
dc.titleVersatile Optimization of Chemical Ordering in Bimetallic Nanoparticlesen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalThe Journal of Physical Chemistry Cen
dc.eprint.versionPublisher's Version/PDFen
dc.contributor.institutionDepartament de Ciència de Materials i Química Física and Institut de Quimica Teòrica i Computacional, Universitat de Barcelona, c/Martí i Franquès 1, 08028 Barcelona, Spainen
dc.contributor.institutionICREA (Institució Catalana de Recerca i Estudis Avançats), Pg. Lluís Companys 23, 08010 Barcelona, Spainen
kaust.authorKozlov, Sergey M.en
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