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

Zhujun Zhang, Takashi Tsuchimochi, Toshiaki Ina, Yoshitaka Kumabe, Shunsuke Muto, Koji Ohara, Hiroki Yamada, Seiichiro L. Ten-no and Takashi Tachikawa ()
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Zhujun Zhang: Molecular Photoscience Research Center, Kobe University
Takashi Tsuchimochi: Kobe University
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
Takashi Tachikawa: Molecular Photoscience Research Center, Kobe University

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-28944-y

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