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Two-site H2O2 photo-oxidation on haematite photoanodes

Author

Listed:
  • Yotam Y. Avital

    (Ben-Gurion University of the Negev)

  • Hen Dotan

    (Technion – Israel Institute of Technology)

  • Dino Klotz

    (Technion – Israel Institute of Technology)

  • Daniel A. Grave

    (Technion – Israel Institute of Technology)

  • Anton Tsyganok

    (Technion – Israel Institute of Technology)

  • Bhavana Gupta

    (Ben-Gurion University of the Negev)

  • Sofia Kolusheva

    (Ben-Gurion University of the Negev)

  • Iris Visoly-Fisher

    (Ben-Gurion University of the Negev)

  • Avner Rothschild

    (Technion – Israel Institute of Technology)

  • Arik Yochelis

    (Ben-Gurion University of the Negev
    Ben-Gurion University of the Negev)

Abstract

H2O2 is a sacrificial reductant that is often used as a hole scavenger to gain insight into photoanode properties. Here we show a distinct mechanism of H2O2 photo-oxidation on haematite (α-Fe2O3) photoanodes. We found that the photocurrent voltammograms display non-monotonous behaviour upon varying the H2O2 concentration, which is not in accord with a linear surface reaction mechanism that involves a single reaction site as in Eley–Rideal reactions. We postulate a nonlinear kinetic mechanism that involves concerted interaction between adions induced by H2O2 deprotonation in the alkaline solution with adjacent intermediate species of the water photo-oxidation reaction, thereby involving two reaction sites as in Langmuir–Hinshelwood reactions. The devised kinetic model reproduces our main observations and predicts coexistence of two surface reaction paths (bi-stability) in a certain range of potentials and H2O2 concentrations. This prediction is confirmed experimentally by observing a hysteresis loop in the photocurrent voltammogram measured in the predicted coexistence range.

Suggested Citation

  • Yotam Y. Avital & Hen Dotan & Dino Klotz & Daniel A. Grave & Anton Tsyganok & Bhavana Gupta & Sofia Kolusheva & Iris Visoly-Fisher & Avner Rothschild & Arik Yochelis, 2018. "Two-site H2O2 photo-oxidation on haematite photoanodes," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-06141-0
    DOI: 10.1038/s41467-018-06141-0
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    Cited by:

    1. Zhujun Zhang & Takashi Tsuchimochi & Toshiaki Ina & Yoshitaka Kumabe & Shunsuke Muto & Koji Ohara & Hiroki Yamada & Seiichiro L. Ten-no & Takashi Tachikawa, 2022. "Binary dopant segregation enables hematite-based heterostructures for highly efficient solar H2O2 synthesis," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

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