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Binary dopant segregation enables hematite-based heterostructures for highly efficient solar H2O2 synthesis

Author

Listed:
  • Zhujun Zhang

    (Molecular Photoscience Research Center, Kobe University)

  • Takashi Tsuchimochi

    (Kobe University
    PRESTO, Japan Science and Technology Agency (JST))

  • Toshiaki Ina

    (Japan Synchrotron Radiation Research Institute)

  • Yoshitaka Kumabe

    (Molecular Photoscience Research Center, Kobe University)

  • Shunsuke Muto

    (Nagoya University, Furo-Cho, Chikusa-Ku)

  • Koji Ohara

    (Japan Synchrotron Radiation Research Institute)

  • Hiroki Yamada

    (Japan Synchrotron Radiation Research Institute)

  • Seiichiro L. Ten-no

    (Kobe University
    Kobe University)

  • Takashi Tachikawa

    (Molecular Photoscience Research Center, Kobe University
    Kobe University)

Abstract

Dopant segregation, frequently observed in ionic oxides, is useful for engineering materials and devices. However, due to the poor driving force for ion migration and/or the presence of substantial grain boundaries, dopants are mostly confined within a nanoscale region. Herein, we demonstrate that core–shell heterostructures are formed by oriented self-segregation using one-step thermal annealing of metal-doped hematite mesocrystals at relatively low temperatures in air. The sintering of highly ordered interfaces between the nanocrystal subunits inside the mesocrystal eliminates grain boundaries, leaving numerous oxygen vacancies in the bulk. This results in the efficient segregation of dopants (~90%) on the external surface, which forms their oxide overlayers. The optimized photoanode based on hematite mesocrystals with oxide overlayers containing Sn and Ti dopants realises high activity (~0.8 μmol min−1 cm−2) and selectivity (~90%) for photoelectrochemical H2O2 production, which provides a wide range of application for the proposed concept.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28944-y
    DOI: 10.1038/s41467-022-28944-y
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    References listed on IDEAS

    as
    1. Zhenfeng Bian & Takashi Tachikawa & Peng Zhang & Mamoru Fujitsuka & Tetsuro Majima, 2014. "A nanocomposite superstructure of metal oxides with effective charge transfer interfaces," Nature Communications, Nature, vol. 5(1), pages 1-9, May.
    2. Hye-In Yoon & Dong-Kyu Lee & Hyung Bin Bae & Gi-Young Jo & Hee-Suk Chung & Jin-Gyu Kim & Suk-Joong L. Kang & Sung-Yoon Chung, 2017. "Probing dopant segregation in distinct cation sites at perovskite oxide polycrystal interfaces," Nature Communications, Nature, vol. 8(1), pages 1-8, December.
    3. Xinjian Shi & Samira Siahrostami & Guo-Ling Li & Yirui Zhang & Pongkarn Chakthranont & Felix Studt & Thomas F. Jaramillo & Xiaolin Zheng & Jens K. Nørskov, 2017. "Understanding activity trends in electrochemical water oxidation to form hydrogen peroxide," Nature Communications, Nature, vol. 8(1), pages 1-6, December.
    4. Zhujun Zhang & Izuru Karimata & Hiroki Nagashima & Shunsuke Muto & Koji Ohara & Kunihisa Sugimoto & Takashi Tachikawa, 2019. "Interfacial oxygen vacancies yielding long-lived holes in hematite mesocrystal-based photoanodes," Nature Communications, Nature, vol. 10(1), pages 1-12, December.
    5. 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.
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