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    Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized Using a Direct Electrochemical Method
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    • Aliya S. Lapp
      Aliya S. Lapp
      Department of Chemistry  and  Texas Materials Institute, The University of Texas at Austin, 2506 Speedway, Stop A5300, Austin, Texas 78712-1224, United States
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    • Zhiyao Duan
      Zhiyao Duan
      Department of Chemistry  and  Institute for Computational and Engineering Sciences, The University of Texas at Austin, 2506 Speedway, Stop A5300, Austin, Texas 78712-1224, United States
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    • Nicholas Marcella
      Nicholas Marcella
      Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11794, United States
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      Orcidhttp://orcid.org/0000-0002-2224-532X
    • Long Luo
      Long Luo
      Department of Chemistry  and  Texas Materials Institute, The University of Texas at Austin, 2506 Speedway, Stop A5300, Austin, Texas 78712-1224, United States
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      Orcidhttp://orcid.org/0000-0001-5771-6892
    • Arda Genc
      Arda Genc
      Thermo Fisher Scientific, 5350 NE Dawson Creek Drive, Hillsboro, Oregon 97124, United States
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    • Jan Ringnalda
      Jan Ringnalda
      Thermo Fisher Scientific, 5350 NE Dawson Creek Drive, Hillsboro, Oregon 97124, United States
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    • Anatoly I. Frenkel*
      Anatoly I. Frenkel
      Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11794, United States
      *[email protected]
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      Orcidhttp://orcid.org/0000-0002-5451-1207
    • Graeme Henkelman*
      Graeme Henkelman
      Department of Chemistry  and  Institute for Computational and Engineering Sciences, The University of Texas at Austin, 2506 Speedway, Stop A5300, Austin, Texas 78712-1224, United States
      *[email protected]
      More by Graeme Henkelman
      Orcidhttp://orcid.org/0000-0002-0336-7153
    • Richard M. Crooks*
      Richard M. Crooks
      Department of Chemistry  and  Texas Materials Institute, The University of Texas at Austin, 2506 Speedway, Stop A5300, Austin, Texas 78712-1224, United States
      *[email protected]
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      Orcidhttp://orcid.org/0000-0001-5186-4878
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2018, 140, 20, 6249–6259
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    https://doi.org/10.1021/jacs.7b12306
    Published May 11, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    In this report, we examine the structure of bimetallic nanomaterials prepared by an electrochemical approach known as hydride-terminated (HT) electrodeposition. It has been shown previously that this method can lead to deposition of a single Pt monolayer on bulk-phase Au surfaces. Specifically, under appropriate electrochemical conditions and using a solution containing PtCl42–, a monolayer of Pt atoms electrodeposits onto bulk-phase Au immediately followed by a monolayer of H atoms. The H atom capping layer prevents deposition of Pt multilayers. We applied this method to ∼1.6 nm Au nanoparticles (AuNPs) immobilized on an inert electrode surface. In contrast to the well-defined, segregated Au/Pt structure of the bulk-phase surface, we observe that HT electrodeposition leads to the formation of AuPt quasi-random alloy NPs rather than the core@shell structure anticipated from earlier reports relating to deposition onto bulk phases. The results provide a good example of how the phase behavior of macro materials does not always translate to the nano world. A key component of this study was the structure determination of the AuPt NPs, which required a combination of electrochemical methods, electron microscopy, X-ray absorption spectroscopy, and theory (DFT and MD).

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.7b12306.

    • UV–vis and TEM for Au147 DENs; evidence of self-terminating Pt deposition; CVs for the EXAFS sample; EDS for the EXAFS sample; best fits to the experimental EXAFS data; XANES spectra; simulated Au and Pt foil k-space spectra; simulated k-space spectra for the NP453 Pt cluster, NP453 shell-2, and Pt38 models; plots showing the effects of vibrational disorder; R-factors for assessing the fits to the simulated EXAFS spectra; calculated Au surface energies for bulk and NP surfaces with and without H; molecular dynamics (MD) simulations for Pt deposition on icosahedral Au147; the driving force for Au surface segregation after alloying; EXAFS sample preparation; TEM of the EXAFS sample; controls for the selectivity of Pt deposition (TEM, CV); Cu UPD for the EXAFS sample; and additional EXAFS fitting considerations (PDF)

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2018, 140, 20, 6249–6259
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.7b12306
    Published May 11, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

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