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Oxygen Reduction Reaction Performance Tuning on Pt Nanoparticle/MWCNT Catalysts by Gd Species

  • Kentaro Ichihashi
    Kentaro Ichihashi
    Department of Chemistry, Graduate School of Science, Nagoya University, Furo, Chikusa, Nagoya, Aichi 464-8602, Japan
  • Satoshi Muratsugu*
    Satoshi Muratsugu
    Department of Chemistry, Graduate School of Science, Nagoya University, Furo, Chikusa, Nagoya, Aichi 464-8602, Japan
    *Email: [email protected] (S.M.).
  • Hirosuke Matsui
    Hirosuke Matsui
    Department of Chemistry, Graduate School of Science, Nagoya University, Furo, Chikusa, Nagoya, Aichi 464-8602, Japan
  • Kotaro Higashi
    Kotaro Higashi
    Innovation Research Center for Fuel Cells, The University of Electro-Communications, 1-5-1, Chofugaoka, Chofu, Tokyo 182-8585, Japan
  • Oki Sekizawa
    Oki Sekizawa
    Japan Synchrotron Radiation Research Institute, SPring-8, 1-1-1 Koto, Sayo, Hyogo 679-5198, Japan
    More by Oki Sekizawa
  • Tomoya Uruga
    Tomoya Uruga
    Japan Synchrotron Radiation Research Institute, SPring-8, 1-1-1 Koto, Sayo, Hyogo 679-5198, Japan
    Innovation Research Center for Fuel Cells, The University of Electro-Communications, 1-5-1, Chofugaoka, Chofu, Tokyo 182-8585, Japan
    More by Tomoya Uruga
  • , and 
  • Mizuki Tada*
    Mizuki Tada
    Department of Chemistry, Graduate School of Science/Research Center for Materials Science/Integrated Research Consortium on Chemical Science/Institute for Advanced Science, Nagoya University, Nagoya, Aichi 464-8602, Japan
    *Email: [email protected] (M.T.).
    More by Mizuki Tada
Cite this: J. Phys. Chem. C 2020, 124, 49, 26925–26936
Publication Date (Web):November 30, 2020
https://doi.org/10.1021/acs.jpcc.0c09308
Copyright © 2020 American Chemical Society

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    Abstract

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    Fine Pt nanoparticles functionalized with Gd3+ hydroxide/oxide species were prepared on multiwalled carbon nanotubes (MWCNTs) containing polypyrrole matrix overlayers and found to exhibit remarkable electrocatalytic performance in the oxygen reduction reaction (ORR). Characterization via transmission electron microscopy, scanning transmission electron microscopy with electron energy loss spectroscopy, X-ray absorption fine structure, and X-ray photoelectron spectroscopy revealed that the Gd3+ hydroxide/oxide species were located in close proximity to the Pt0 nanoparticles on the MWCNTs. The prepared Pt nanoparticle–Gd hydroxide/oxide composites exhibited superior ORR activity to Gd-free Pt nanoparticles prepared in a similar manner, and the decoration with the Gd species suppressed Pt oxidation and accelerated Pt oxide reduction, as demonstrated by cyclic voltammetry and in situ Pt LIII-edge X-ray absorption near-edge structure analysis under potential application. The effect of the Gd loading on the ORR performance was also examined, revealing the existence of an optimal Gd loading beyond which further Gd incorporation resulted in aggregation of the Gd3+ domains and decreased crystallinity of the Pt nanoparticles.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcc.0c09308.

    • Pt and Gd LIII-edge XANES spectra and EXAFS curve-fitting results, additional TEM and STEM-EELS images, TGA, and ORR electrocatalytic data (PDF)

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