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Sub-50 nm perovskite-type tantalum-based oxynitride single crystals with enhanced photoactivity for water splitting

Jiadong Xiao, Mamiko Nakabayashi, Takashi Hisatomi, Junie Jhon M. Vequizo, Wenpeng Li, Kaihong Chen, Xiaoping Tao, Akira Yamakata, Naoya Shibata, Tsuyoshi Takata, Yasunobu Inoue and Kazunari Domen ()
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Jiadong Xiao: Shinshu University
Mamiko Nakabayashi: The University of Tokyo
Takashi Hisatomi: Shinshu University
Junie Jhon M. Vequizo: Shinshu University
Wenpeng Li: Shinshu University
Kaihong Chen: Shinshu University
Xiaoping Tao: Shinshu University
Akira Yamakata: Okayama University
Naoya Shibata: The University of Tokyo
Tsuyoshi Takata: Shinshu University
Yasunobu Inoue: Japan Technological Research Association of Artificial Photosynthetic Chemical Process (ARPChem)
Kazunari Domen: Shinshu University

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract A long-standing trade-off exists between improving crystallinity and minimizing particle size in the synthesis of perovskite-type transition-metal oxynitride photocatalysts via the thermal nitridation of commonly used metal oxide and carbonate precursors. Here, we overcome this limitation to fabricate ATaO2N (A = Sr, Ca, Ba) single nanocrystals with particle sizes of several tens of nanometers, excellent crystallinity and tunable long-wavelength response via thermal nitridation of mixtures of tantalum disulfide, metal hydroxides (A(OH)2), and molten-salt fluxes (e.g., SrCl2) as precursors. The SrTaO2N nanocrystals modified with a tailored Ir–Pt alloy@Cr2O3 cocatalyst evolved H2 around two orders of magnitude more efficiently than the previously reported SrTaO2N photocatalysts, with a record solar-to-hydrogen energy conversion efficiency of 0.15% for SrTaO2N in Z-scheme water splitting. Our findings enable the synthesis of perovskite-type transition-metal oxynitride nanocrystals by thermal nitridation and pave the way for manufacturing advanced long-wavelength-responsive particulate photocatalysts for efficient solar energy conversion.

Date: 2023
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DOI: 10.1038/s41467-023-43838-3

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