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Orientation controlled photogenerated carriers on self-supporting CdS/Ni3S2 paper toward photocatalytic hydrogen evolution and biomass upgrading

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Abstract

The appropriate regulation of band structure is an effective strategy in constructing efficient photocatalytic systems. Present photocatalytic system mainly employs powder photocatalysts, which makes their recovery reliant on expensive separation processes and severely limits their industrial application. Herein, we constructed a novel CdS/Ni3S2 heterostructure using free-standing and flexible nickel fiber paper as the matrix. The regulated energy band structure achieves effective electron–hole separation. The as-synthesized flexible photocatalyst exhibits considerable photocatalytic activity toward the H2 evolution reaction under visible-light irradiation, with an H2 production rate of 5.63 μmol·cm−2 ·h−1 (14.1 mmol·g−1cat· h−1 according to the catalyst loading content). Additionally, the otherwise-wasted excited holes simultaneously drive organic transformations to yield value-added organic products, thus markedly improving the photocatalytic H2 evolution rate. Such a photocatalytic system is scaled up further, where a self-supported 20 cm × 25 cm sample achieves a champion H2 production rate of 60–80 μmol·h−1 under practical sun irradiation. This newly developed self-supported photocatalyst produces opportunities for practical solar H2 production with biomass upgrading.

Graphical abstract

摘要

合理调控能带结构是构建高效光催化系统的有效策略。目前的光催化系统主要采用回收困难的粉末光催化剂，复杂的分离过程严重限制了其工业应用。本文使用自支撑柔性镍纤维纸作为基质，构建了一种新型的CdS/Ni3S2异质结光催化剂。调控后的能带结构实现了有效的电子-空穴分离。合成的柔性自支撑光催化剂在可见光照射下表现出了非常好的光催化产氢活性显著，氢气产率为5.63 μmol‧cm-2‧h-1（根据催化剂负载量计算为14.1 mmol‧ g-1 cat. h-1）。此外，激发的空穴也可促进有机转化，在生成增值有机产品的同时提高光催化产氢效率。随后，将光催化系统进一步扩大规模。在设计的光催化反应体系中和实际太阳辐照下，20 cm × 25 cm的大尺寸样品最高实现了60–80 μmol‧h-1的氢气产率。这种新开发的自支撑光催化剂为实现可持续太阳能驱动的生物质升级及氢能规划化转化奠定了基础。

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 51972147, 52022037 and 52202366), Taishan Scholars Project Special Funds (No. tsqn201812083), the Innovative Team Project of Jinan (No. 2021GXRC019), the Natural Science Foundation of Shandong Province (Nos. ZR2019YQ20, ZR2021QE011, ZR2021JQ15 and ZR2022YQ42) and the King Abdullah University of Science and Technology (KAUST).

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  1. Xiao-Yan Liu and Qing Cao have contributed equally to this work.

Authors and Affiliations

  1. Institute for Advanced Interdisciplinary Research, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, China

    Xiao-Yan Liu, Hui Liu, Li-Li Zeng, Li-Li Zhao, Bin Chang, Hong Liu & Wei-Jia Zhou

  2. Institute of Chemistry and Biochemistry, Freie Universität Berlin, 14195, Berlin, Germany

    Qing Cao

  3. Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, 1015, Lausanne, Switzerland

    Gui-Xiang Li

  4. KAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia

    Bin Chang

  5. School of Environment and Energy, South China University of Technology, Guangzhou Higher Education Mega Center, Guangzhou, 510006, China

    Xi-Wen Wang

  6. State Key Laboratory of Crystal Materials, Shandong University, Jinan, 250100, China

    Hong Liu

  7. School of Mechanical Engineering, Xi’an Jiaotong University, Xi’an, 710054, China

    Hong Liu

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Liu, XY., Cao, Q., Li, GX. et al. Orientation controlled photogenerated carriers on self-supporting CdS/Ni3S2 paper toward photocatalytic hydrogen evolution and biomass upgrading. Rare Met. 43, 2015–2025 (2024). https://doi.org/10.1007/s12598-023-02555-y

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