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Evidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reduction

Author

Listed:
  • Nicolas A. Ishiki

    (LEPMI
    CP 780
    ITODYS)

  • Keyla Teixeira Santos

    (LEPMI
    270)

  • Nicolas Bibent

    (1919 route de Mende)

  • Kavita Kumar

    (LEPMI)

  • Ina Reichmann

    (Cauerstraße 1
    Cauerstraße 1)

  • Yu-Ping Ku

    (Cauerstraße 1
    Cauerstraße 1)

  • Tristan Asset

    (1919 route de Mende
    25 rue Becquerel)

  • Laetitia Dubau

    (LEPMI)

  • Michel Mermoux

    (LEPMI)

  • Hongxin Ge

    (CS 10207 rue Claude Daunesse)

  • Sandrine Berthon-Fabry

    (CS 10207 rue Claude Daunesse)

  • Viktoriia A. Saveleva

    (71 Avenue des Martyrs
    1025 rue de la Piscine)

  • Vinod K. Paidi

    (71 Avenue des Martyrs)

  • Pieter Glatzel

    (71 Avenue des Martyrs)

  • Andrea Zitolo

    (BP 48 Saint Aubin)

  • Tzonka Mineva

    (1919 route de Mende)

  • Hazar Guesmi

    (1919 route de Mende)

  • Serhiy Cherevko

    (Cauerstraße 1)

  • Edson A. Ticianelli

    (CP 780)

  • Frédéric Maillard

    (LEPMI)

  • Frédéric Jaouen

    (1919 route de Mende)

Abstract

While Fe–N–C materials have shown promising initial oxygen reduction reaction (ORR) activity, they lack durability in acidic medium. Key degradation mechanisms include FeN4 site demetallation and deactivation by reactive oxygen species. Here we show for mainstream Fe–N–Cs that adding 1 wt.% Pt nanoparticles via a soft polyol method results in well-defined and stable Pt/Fe–N–C hybrids. The Pt addition strongly reduces the H2O2 production and Fe leaching rate during ORR, while post mortem Mössbauer spectroscopy reveals that the highly active but unstable Fe(III)N4 site is partially stabilized. The similar H2O2 electroreduction activity of Pt/Fe–N–C and Fe–N–C and other analyses point toward a long-distance electronic effect of Pt nanoparticles in stabilizing FeN4 sites. Computational chemistry reveals that spin polarization of distant Pt atoms mitigates the structural changes of FeN4 sites upon adsorption of oxygenated species atop Fe, especially in high-spin state.

Suggested Citation

  • Nicolas A. Ishiki & Keyla Teixeira Santos & Nicolas Bibent & Kavita Kumar & Ina Reichmann & Yu-Ping Ku & Tristan Asset & Laetitia Dubau & Michel Mermoux & Hongxin Ge & Sandrine Berthon-Fabry & Viktori, 2025. "Evidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reduction," Nature Communications, Nature, vol. 16(1), pages 1-15, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-61806-x
    DOI: 10.1038/s41467-025-61806-x
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    References listed on IDEAS

    as
    1. Yanyan Sun & Shlomi Polani & Fang Luo & Sebastian Ott & Peter Strasser & Fabio Dionigi, 2021. "Advancements in cathode catalyst and cathode layer design for proton exchange membrane fuel cells," Nature Communications, Nature, vol. 12(1), pages 1-14, December.
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