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


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.

SUBMITTER: Xiao J 

PROVIDER: S-EPMC10696056 | biostudies-literature | 2023 Dec

REPOSITORIES: biostudies-literature

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

Xiao Jiadong J   Nakabayashi Mamiko M   Hisatomi Takashi T   Vequizo Junie Jhon M JJM   Li Wenpeng W   Chen Kaihong K   Tao Xiaoping X   Yamakata Akira A   Shibata Naoya N   Takata Tsuyoshi T   Inoue Yasunobu Y   Domen Kazunari K  

Nature communications 20231205 1


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 ATaO<sub>2</sub>N (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 mix  ...[more]

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