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Abnormal Metal Bond Distances in PtAu Alloy Nanoparticles: In Situ Back-Illumination XAFS Investigations of the Structure of PtAu Nanoparticles on a Flat HOPG Substrate Prepared by Arc Plasma Deposition

  • Bing Hu
    Bing Hu
    Institute for Catalysis, Hokkaido University, Sapporo, Hokkaido 001-0021, Japan
    More by Bing Hu
  • Bapurao Bharate
    Bapurao Bharate
    Institute for Catalysis, Hokkaido University, Sapporo, Hokkaido 001-0021, Japan
  • Juan D. Jimenez
    Juan D. Jimenez
    Department of Chemical Engineering, University of South Carolina, 541 Main Street, Columbia, South Carolina 29208, United States
  • Jochen Lauterbach
    Jochen Lauterbach
    Department of Chemical Engineering, University of South Carolina, 541 Main Street, Columbia, South Carolina 29208, United States
  • Naoto Todoroki
    Naoto Todoroki
    Graduate School of Environmental Studies, Tohoku University, Sendai, Miyagi 980-8579, Japan
  • Toshimasa Wadayama
    Toshimasa Wadayama
    Graduate School of Environmental Studies, Tohoku University, Sendai, Miyagi 980-8579, Japan
  • Kotaro Higashi
    Kotaro Higashi
    Innovation Research Center for Fuel Cells, University of Electro-Communications, Chofu, Tokyo 182-8585, Japan
  • Tomoya Uruga
    Tomoya Uruga
    Innovation Research Center for Fuel Cells, University of Electro-Communications, Chofu, Tokyo 182-8585, Japan
    Japan Synchrotron Radiation Research Institute (JASRI), Sayo, Hyogo 679-5148, Japan
    More by Tomoya Uruga
  • Yasuhiro Iwasawa
    Yasuhiro Iwasawa
    Innovation Research Center for Fuel Cells, University of Electro-Communications, Chofu, Tokyo 182-8585, Japan
  • Hiroko Ariga-Miwa
    Hiroko Ariga-Miwa
    Innovation Research Center for Fuel Cells, University of Electro-Communications, Chofu, Tokyo 182-8585, Japan
  • Satoru Takakusagi
    Satoru Takakusagi
    Institute for Catalysis, Hokkaido University, Sapporo, Hokkaido 001-0021, Japan
  • , and 
  • Kiyotaka Asakura*
    Kiyotaka Asakura
    Institute for Catalysis, Hokkaido University, Sapporo, Hokkaido 001-0021, Japan
    *Email: [email protected]
Cite this: J. Phys. Chem. C 2022, 126, 2, 1006–1016
Publication Date (Web):January 10, 2022
https://doi.org/10.1021/acs.jpcc.1c08393
Copyright © 2022 American Chemical Society
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Abstract

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To reveal the origin of the difference between the Pt–Pt bond distance in Au(core)–Pt(shell)-type (PtAu) nanoparticles and that in a Pt overlayer on Au(111), alloy-type PtAu nanoparticles were prepared on a highly oriented pyrolytic graphite (HOPG) surface by arc plasma deposition and their structure was investigated under various electrochemical conditions by bent-crystal Laue analyzer (BCLA)-empowered back-illuminated X-ray absorption fine structure (BCLA + BI-XAFS) and high-energy-resolution fluorescence detection (HERFD)-empowered back-illuminated X-ray absorption near-edge structure (HERFD + BI-XANES) methods. On the basis of the XAFS analysis at both edges, we proposed the formation of a PtAu alloy core covered with a Pt-rich shell at 0.4 VRHE, where the Pt–Pt, Pt–Au, and Au–Au bond lengths were all found to be ∼2.76 Å. The Au–Au bond length was abnormally shorter than that for bulk Au. The Pt shell was dissolved under applied potentials greater than 0.8 VRHE with the aid of the high-intensity X-rays, and the Au–Au distance increased. We concluded that the abnormal bond lengths were due to the strong surface tension from the Pt-rich shell and the relaxation of the lattice distortion. The Pt–Pt bond length in the PtAu nanoparticles decreases as a result of the surface tension of the nanoparticles; this surface tension does not exist on flat Au surfaces, where the lattice distortion between the Pt overlayer and the substrate is the main driving force for the expansion of the Pt–Pt bond length.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcc.1c08393.

  • Experimental details, XPS results, CV and its analysis details, EXAFS and its analysis details, change of the edge height, XANES of Pt L3 and Au L3 measured by BCLA + BI-XAFS, edge height of Pt10Au90 foil, error estimation using the χ2 test, HERFD-XANES by FEFF8, edge height dependence on potential, BCLA + BI-XAFS experiment setup and XAFS analysis, quantification of Pt in PtAu/HOPG using XPS, deriving the error bar for the parameters in EXAFS fitting, and discerning the O adsorption site from HERFD-XANES (PDF)

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