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Built-in electric field induced S-scheme g-C3N4 homojunction for efficient photocatalytic hydrogen evolution: Interfacial engineering and morphology control

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Abstract

S-scheme possesses superior redox capabilities compared with the II-scheme, providing an effective method to solve the innate defects of g-C3N4 (CN). In this study, S-doped g-C3N4/g-C3N4 (SCN-tm/CN) S-scheme homojunction was constructed by rationally integrating morphology control with interfacial engineering to enhance the photocatalytic hydrogen evolution performance. In-situ Kelvin probe force microscopy (KPFM) confirms the transport of photo-generated electrons from CN to SCN. Density functional theory (DFT) calculations reveal that the generation of a built-in electric field between SCN and CN enables the carrier separation to be more efficient and effective. Femtosecond transient absorption spectrum (fs-TAS) indicates prolonged lifetimes of SCN-tm/CN3 (τ1: 9.7, τ2: 110, and τ3: 1343.5 ps) in comparison to those of CN (τ1: 4.86, τ2: 55.2, and τ3: 927 ps), signifying that the construction of homojunction promotes the separation and transport of electron hole pairs, thus favoring the photocatalytic process. Under visible light irradiation, the optimized SCN-tm/CN3 exhibits excellent photocatalytic activity with the hydrogen evolution rate of 5407.3 µmol·g−1·h−1, which is 20.4 times higher than that of CN (265.7 µmol·g−1·h−1). Moreover, the homojunction also displays an apparent quantum efficiency of 26.8% at 435 nm as well as ultra-long and ultra-stable cycle ability. This work offers a new strategy to construct highly efficient photocatalysts based on the metal-free conjugated polymeric CN for realizing solar energy conversion.

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Acknowledgements

This work is supported by the Natural Science Foundation of Henan (No. 232300421361) and the National Natural Science Foundation of China (Nos. 21671176 and 21001096). We thank Beijing China Education Au-light Co., Ltd. for providing the instrument and assistance with SPV measurements.

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  1. College of Chemistry, Zhengzhou University, Zhengzhou, 450001, China

    Yongpan Gu, Yike Li, Haoqiang Feng, Yanan Han & Zhongjun Li

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Built-in electric field induced S-scheme g-C3N4 homojunction for efficient photocatalytic hydrogen evolution: Interfacial engineering and morphology control

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Gu, Y., Li, Y., Feng, H. et al. Built-in electric field induced S-scheme g-C3N4 homojunction for efficient photocatalytic hydrogen evolution: Interfacial engineering and morphology control. Nano Res. 17, 4961–4970 (2024). https://doi.org/10.1007/s12274-024-6501-0

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