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Exploring dynamic solvation kinetics at electrocatalyst surfaces

Author

Listed:
  • Francisco Sarabia

    (Fritz-Haber Institute of the Max Planck Society)

  • Carlos Gomez Rodellar

    (Fritz-Haber Institute of the Max Planck Society)

  • Beatriz Roldan Cuenya

    (Fritz-Haber Institute of the Max Planck Society)

  • Sebastian Z. Oener

    (Fritz-Haber Institute of the Max Planck Society)

Abstract

The interface between electrocatalyst and electrolyte is highly dynamic. Even in absence of major structural changes, the intermediate coverage and interfacial solvent are bias and time dependent. This is not accounted for in current kinetic models. Here, we study the kinetics of the hydrogen evolution, ammonia oxidation and oxygen reduction reactions on polycrystalline Pt with distinct intrinsic rates and intermediates (e.g. *H, *OH, *NH2, *N). Despite these differences, we discover shared relationships between the pre-exponential factor and the activation energy that we link to solvation kinetics in the presence of electronic excess charge and charged intermediates. Further, we study dynamic changes of these kinetic parameters with a millisecond time resolution during electrosorption and double layer charging and dynamic *N and *NO poisoning. Finally, we discover a pH-dependent activation entropy that explains non-Nernstian overpotential shifts with pH. In sum, our results demonstrate the importance of accounting for a bias and time-dependent interfacial solvent and catalyst surface.

Suggested Citation

  • Francisco Sarabia & Carlos Gomez Rodellar & Beatriz Roldan Cuenya & Sebastian Z. Oener, 2024. "Exploring dynamic solvation kinetics at electrocatalyst surfaces," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52499-9
    DOI: 10.1038/s41467-024-52499-9
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    References listed on IDEAS

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    1. Isis Ledezma-Yanez & W. David Z. Wallace & Paula Sebastián-Pascual & Victor Climent & Juan M. Feliu & Marc T. M. Koper, 2017. "Interfacial water reorganization as a pH-dependent descriptor of the hydrogen evolution rate on platinum electrodes," Nature Energy, Nature, vol. 2(4), pages 1-7, April.
    2. Aleksandar R. Zeradjanin, 2024. "Understanding entropic barriers," Nature Energy, Nature, vol. 9(5), pages 514-515, May.
    3. Carlos G. Rodellar & José M. Gisbert-Gonzalez & Francisco Sarabia & Beatriz Roldan Cuenya & Sebastian Z. Oener, 2024. "Ion solvation kinetics in bipolar membranes and at electrolyte–metal interfaces," Nature Energy, Nature, vol. 9(5), pages 548-558, May.
    4. 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.
    5. Felix T. Haase & Arno Bergmann & Travis E. Jones & Janis Timoshenko & Antonia Herzog & Hyo Sang Jeon & Clara Rettenmaier & Beatriz Roldan Cuenya, 2022. "Size effects and active state formation of cobalt oxide nanoparticles during the oxygen evolution reaction," Nature Energy, Nature, vol. 7(8), pages 765-773, August.
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