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Direct oxygen isotope effect identifies the rate-determining step of electrocatalytic OER at an oxidic surface

Author

Listed:
  • Sandra Haschke

    (Friedrich-Alexander-Universität Erlangen-Nürnberg)

  • Michael Mader

    (Friedrich-Alexander-Universität Erlangen-Nürnberg)

  • Stefanie Schlicht

    (Friedrich-Alexander-Universität Erlangen-Nürnberg)

  • André M. Roberts

    (Friedrich-Alexander-Universität Erlangen-Nürnberg)

  • Alfredo M. Angeles-Boza

    (University of Connecticut)

  • Johannes A. C. Barth

    (Friedrich-Alexander-Universität Erlangen-Nürnberg)

  • Julien Bachmann

    (Friedrich-Alexander-Universität Erlangen-Nürnberg
    Saint Petersburg State University)

Abstract

Understanding the mechanism of water oxidation to dioxygen represents the bottleneck towards the design of efficient energy storage schemes based on water splitting. The investigation of kinetic isotope effects has long been established for mechanistic studies of various such reactions. However, so far natural isotope abundance determination of O2 produced at solid electrode surfaces has not been applied. Here, we demonstrate that such measurements are possible. Moreover, they are experimentally simple and sufficiently accurate to observe significant effects. Our measured kinetic isotope effects depend strongly on the electrode material and on the applied electrode potential. They suggest that in the case of iron oxide as the electrode material, the oxygen evolution reaction occurs via a rate-determining O−O bond formation via nucleophilic water attack on a ferryl unit.

Suggested Citation

  • Sandra Haschke & Michael Mader & Stefanie Schlicht & André M. Roberts & Alfredo M. Angeles-Boza & Johannes A. C. Barth & Julien Bachmann, 2018. "Direct oxygen isotope effect identifies the rate-determining step of electrocatalytic OER at an oxidic surface," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-07031-1
    DOI: 10.1038/s41467-018-07031-1
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    Cited by:

    1. Shikang Yin & Yiying Zhou & Zhonghuan Liu & Huijie Wang & Xiaoxue Zhao & Zhi Zhu & Yan Yan & Pengwei Huo, 2024. "Elucidating protonation pathways in CO2 photoreduction using the kinetic isotope effect," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    2. Che Lah, Nurul Akmal, 2021. "Late transition metal nanocomplexes: Applications for renewable energy conversion and storage," Renewable and Sustainable Energy Reviews, Elsevier, vol. 145(C).
    3. Kun Du & Lifu Zhang & Jieqiong Shan & Jiaxin Guo & Jing Mao & Chueh-Cheng Yang & Chia-Hsin Wang & Zhenpeng Hu & Tao Ling, 2022. "Interface engineering breaks both stability and activity limits of RuO2 for sustainable water oxidation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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