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The development of visible-light-responsive photocatalysts for promoting solar-driven oxygen (O2) production from water splitting is a potentially attractive but still a challenging scheme. In the present work, a (111)-type layered perovskite oxynitride, Sr5Nb4O15−xNx, was synthesized via the nitridation treatment of the disk-like oxide precursor under the ammonia flow, which was fabricated using a flux method. The homogeneous dispersion of nitrogen (N) dopant in N-doped Sr5Nb4O15 was ascertained by energy-dispersive X-ray spectroscopy characterization, and the Sr5Nb4O15−xNx was found to be a direct semiconductor with a light absorption edge of approximately 640 nm. Density functional theory investigation implies that the hybridization between the outmost N 2p orbitals and O 2p orbitals upshifts the original valence band maximum of Sr5Nb4O15 and endows its visible-light-responsive characteristics. Loading with cobalt oxide (CoOx) as cocatalyst, the as-prepared Sr5Nb4O15−xNx exhibited an enhanced photocatalytic O2 evolution activity from water splitting under visible-light illumination (λ > 420 nm). Moreover, another homogeneous N-doped layered perovskite-type niobium (Nb)-based oxynitride, Ba5Nb4O15−xNx, was also developed and investigated for the visible-light-actuated O2 production, highlighting the versatility of the present approach for exploring novel visible-light-responsive photocatalysts.

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Publication history

Received: 08 April 2022
Revised: 11 May 2022
Accepted: 11 May 2022
Published: 14 June 2022
Issue date: November 2022

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

The authors are thankful for the financial support from the National Key R&D Program of China (No. 2020YFA0406102), the National Natural Science Foundation of China (Nos. 21633009 and 21925206), the International Partnership Program of Chinese Academy of Sciences (No. 121421KYSB20190025), the Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund, CAS (No. DNL 201913), and the DICP Foundation of Innovative Research (No. DICP I201927).

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Email: nanores@tup.tsinghua.edu.cn

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