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dc.creatorYancey, David F.en_US
dc.creatorZhang, Liangen_US
dc.creatorCrooks, Richard M.en_US
dc.creatorHenkelman, Graemeen_US
dc.date.accessioned2016-09-23T18:05:02Z
dc.date.available2016-09-23T18:05:02Z
dc.date.issued2012-01en_US
dc.identifierdoi:10.15781/T2T43J42D
dc.identifier.citationYancey, David F., Liang Zhang, Richard M. Crooks, and Graeme Henkelman. "Au@ Pt dendrimer encapsulated nanoparticles as model electrocatalysts for comparison of experiment and theory." Chemical Science 3, no. 4 (Jan., 2012): 1033-1040.en_US
dc.identifier.issn2041-6520en_US
dc.identifier.urihttp://hdl.handle.net/2152/41034
dc.description.abstractIn this paper we report the electrochemical synthesis of core@shell dendrimer-encapsulated nanoparticles (DENs) consisting of cores containing 147 Au atoms (Au-147) and Pt shells having similar to 54 or similar to 102 atoms (Au-147@Pt-n (n = 54 or 102)). The significance of this work arises from the correlation of the experimentally determined structural and electrocatalytic properties of these particles with density functional theory (DFT) calculations. Specifically, we describe an experimental and theoretical study of Pb underpotential deposition (UPD) on Au-147 DENs, the structure of both Au-147@Pb-n and Au-147@Pt-n DENs, and the activity of these DENs for the oxygen reduction reaction (ORR). DFT calculations show that Pb binding is stronger on the (100) facets of Au as compared to (111), and the calculated deposition and stripping potentials are consistent with those measured experimentally. Galvanic exchange is used to replace the surface Pb atoms with Pt, and a surface distortion is found for Au-147@Pt-n particles using molecular dynamics simulations in which the Pt-covered (100) facets shear into (111) diamond structures. DFT calculations of oxygen binding show that the distorted surfaces are the most active for the ORR, and that their activity is similar regardless of the Pt coverage. These calculations are consistent with rotating ring-disk voltammetry measurements.en_US
dc.description.sponsorshipChemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U. S. Department of Energy DE-FG02-09ER16090en_US
dc.description.sponsorshipRobert A. Welch Foundation F-0032, F-1601en_US
dc.description.sponsorshipInstitute of Computational and Engineering Sciences at UT-Austinen_US
dc.language.isoEnglishen_US
dc.relation.ispartofen_US
dc.rightsAdministrative deposit of works to Texas ScholarWorks: This works author(s) is or was a University faculty member, student or staff member; this article is already available through open access or the publisher allows a PDF version of the article to be freely posted online. The library makes the deposit as a matter of fair use (for scholarly, educational, and research purposes), and to preserve the work and further secure public access to the works of the University.en_US
dc.subjectoxygen reduction reactionen_US
dc.subjectaugmented-wave methoden_US
dc.subjectgold nanoparticlesen_US
dc.subjectcatalytic-activityen_US
dc.subjecto-2 reductionen_US
dc.subjectplatinumen_US
dc.subjectshapeen_US
dc.subjectelectrochemistryen_US
dc.subjectsubstrateen_US
dc.subjectkineticsen_US
dc.subjectchemistry, multidisciplinaryen_US
dc.titleAu@Pt Dendrimer Encapsulated Nanoparticles As Model Electrocatalysts for Comparison of Experiment and Theoryen_US
dc.typeArticleen_US
dc.description.departmentChemistryen_US
dc.rights.restrictionOpenen_US
dc.identifier.doi10.1039/c2sc00971den_US
dc.contributor.utaustinauthorYancey, David F.en_US
dc.contributor.utaustinauthorZhang, Liangen_US
dc.contributor.utaustinauthorCrooks, Richard M.en_US
dc.contributor.utaustinauthorHenkelman, Graemeen_US
dc.relation.ispartofserialChemical Scienceen_US


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