Sub-50 nm perovskite-type tantalum-based oxynitride single crystals with enhanced photoactivity for water splitting.
basic_science · Level V
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- Record sourced from PubMed, PMID 38049410.
- Also identified by DOI 10.1038/s41467-023-43838-3 and PMC identifier 10696056.
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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 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 mixtures of tantalum disulfide, metal hydroxides (A(OH)<sub>2</sub>), and molten-salt fluxes (e.g., SrCl<sub>2</sub>) as precursors. The SrTaO<sub>2</sub>N nanocrystals modified with a tailored Ir-Pt alloy@Cr<sub>2</sub>O<sub>3</sub> cocatalyst evolved H<sub>2</sub> around two orders of magnitude more efficiently than the previously reported SrTaO<sub>2</sub>N photocatalysts, with a record solar-to-hydrogen energy conversion efficiency of 0.15% for SrTaO<sub>2</sub>N 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.