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Unifying the ORR and OER with surface oxygen and extracting their intrinsic activities on platinum

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  • Benedikt Axel Brandes

    (Department of Energy Conversion and Storage)

  • Yogeshwaran Krishnan

    (Department of Energy Conversion and Storage)

  • Fabian Luca Buchauer

    (Department of Energy Conversion and Storage)

  • Heine Anton Hansen

    (Department of Energy Conversion and Storage)

  • Johan Hjelm

    (Department of Energy Conversion and Storage)

Abstract

Common half-cell measurements deliver oxygen reduction activities linked to the chosen scan rate, limiting their value for fundamental and comparative studies on platinum. Here we show a deconvolution of the intrinsic kinetics from the effect of surface oxygen on platinum. We find an electronic effect of the surface oxygen, substantiate a Tafel slope of ~120 mV/decade, obtain an exchange current density of 13 ± 4 µA/cm2, and an activity of 7 mA/cm2 at 900 mV. Eventually, we broaden the scope of this analysis to the effects of surface rearrangement, alloying, and supported Pt nanoparticles, the latter providing insight into discrepancies between half-cell and fuel cell measurements. We find through computational methods that binding energies of intermediates would be weakened by the presence of highly coordinated oxygen atoms. Finally, we obtain a phenomenological rate equation for the oxygen reduction and evolution reaction, suggesting that both reactions follow a shared mechanism.

Suggested Citation

  • Benedikt Axel Brandes & Yogeshwaran Krishnan & Fabian Luca Buchauer & Heine Anton Hansen & Johan Hjelm, 2024. "Unifying the ORR and OER with surface oxygen and extracting their intrinsic activities on platinum," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-51605-1
    DOI: 10.1038/s41467-024-51605-1
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    References listed on IDEAS

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    2. Rubén Rizo & Julia Fernández-Vidal & Laurence J. Hardwick & Gary A. Attard & Francisco J. Vidal-Iglesias & Victor Climent & Enrique Herrero & Juan M. Feliu, 2022. "Investigating the presence of adsorbed species on Pt steps at low potentials," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    3. Hong Nhan Nong & Lorenz J. Falling & Arno Bergmann & Malte Klingenhof & Hoang Phi Tran & Camillo Spöri & Rik Mom & Janis Timoshenko & Guido Zichittella & Axel Knop-Gericke & Simone Piccinin & Javier P, 2020. "Key role of chemistry versus bias in electrocatalytic oxygen evolution," Nature, Nature, vol. 587(7834), pages 408-413, November.
    4. Hernan Sanchez Casalongue & Sarp Kaya & Venkatasubramanian Viswanathan & Daniel J. Miller & Daniel Friebel & Heine A. Hansen & Jens K. Nørskov & Anders Nilsson & Hirohito Ogasawara, 2013. "Direct observation of the oxygenated species during oxygen reduction on a platinum fuel cell cathode," Nature Communications, Nature, vol. 4(1), pages 1-6, December.
    5. Rubén Rizo & Julia Fernández-Vidal & Laurence J. Hardwick & Gary A. Attard & Francisco J. Vidal-Iglesias & Victor Climent & Enrique Herrero & Juan M. Feliu, 2022. "Author Correction: Investigating the presence of adsorbed species on Pt steps at low potentials," Nature Communications, Nature, vol. 13(1), pages 1-1, December.
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