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Research Article

Homogeneous nitrogen-doped (111)-type layered Sr5Nb4O15−xNx as a visible-light-responsive photocatalyst for water oxidation

Shiwen Du1, Hai Zou1,2, Yunfeng Bao1, Yu Qi1, Xueshang Xin1,2, Shuowen Wang1, Zhaochi Feng1, Fuxiang Zhang1( )
State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
University of Chinese Academy of Sciences, Beijing 100049, China
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Graphical Abstract

Novel homogeneous nitrogen-doped (111)-type layered perovskite oxynitride (Sr5Nb4O15−xNx) is directly synthesized using a thermal ammonolysis method, which exhibits an enhanced photocatalytic oxygen (O2) evolution activity from water splitting under visible-light illumination (λ > 420 nm) after loading with cobalt oxide (CoOx) as cocatalyst.

Abstract

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.

Keywords

nitrogen-dopedvisible-light-responsivelayered perovskiteoxygen (O2) evolutionwater splitting

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Nano Research
Volume 15 Issue 12,
December 2022
Pages 9976-9984
DOI: 10.1007/s12274-022-4529-6
Cite this article:
Du S, Zou H, Bao Y, et al. Homogeneous nitrogen-doped (111)-type layered Sr5Nb4O15−xNx as a visible-light-responsive photocatalyst for water oxidation. Nano Research, 2022, 15(12): 9976-9984. https://doi.org/10.1007/s12274-022-4529-6
Topics:
Photocatalysts
Part of a topical collection:
NR45 Awards in Nanocatalysis, 2022

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Received: 08 April 2022
Revised: 11 May 2022
Accepted: 11 May 2022
Published: 14 June 2022
© Tsinghua University Press 2022
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