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A direct polymeric carbon nitride/tungsten oxide Z-scheme heterostructure for efficient photocatalytic hydrogen generation via reforming of plastics into value-added chemicals

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Abstract

To promote charge transfer and separation for efficient photocatalysis, a direct Z-scheme heterostructure was constructed by coupling polymeric carbon nitride (PCN) and WO3. Interestingly, the obtained PCN/WO3 Z-scheme heterostructure could photocatalytically produce hydrogen and value-added chemicals (e.g., formate and acetate) by reforming of plastic polylactic acid (PLA) in alkaline aqueous condition. By optimizing WO3 contents and reaction conditions, the obtained PCN/WO3 heterostructure exhibits much increased photocatalytic activity for PLA photoreforming under visible light, with hydrogen evolution rate reaching 402.90 μmol·g−1·h−1, which is 3.5 times that of PCN. It is revealed that the Z-scheme charge transfer between PCN and WO3 mainly contributes to the promoted charge separation and thus the improved photocatalytic activity. Moreover, with h+ and ·OH experimentally evidenced as the predominant active species, a possible reaction pathway for the reforming of PLA into value-added chemicals (e.g., formate and acetate) over PCN/WO3 Z-scheme heterostructure is cleared by monitoring the reaction intermediates and radicals. This work paves a carbon neutrality and scalable route toward the synergistical production of hydrogen and value-added chemicals by utilizing and recycling plastic waste.

摘要

为了促进电荷转移和分离以提升光催化效率, 通过耦合聚合氮化碳 (PCN) 和WO3构建了Z型异质结光催化剂 (PCN/WO3) 。在碱性条件下, 这种Z型异质结能够光催化重整聚乳酸 (PLA) 产生氢气和高附加值化学品 (如甲酸盐和乙酸盐) 。通过优化WO3的含量和反应pH条件, PCN/WO3异质结光催化剂光催化重整聚乳酸产氢的反应速率最高可达402.90 μmol·g−1·h−1, 是PCN的3.5倍。研究表明, PCN和WO3之间的Z型电荷转移路径能够显著促进电荷分离从而提升光催化活性。此外, 研究还表明h+ 和 •OH是主要的反应活性物种。通过监测反应中间产物和自由基, 揭示了PCN/WO3 Z型异质结将聚乳酸转化为高附加值化学品 (如甲酸盐和乙酸盐) 可能的反应途径。这项工作为实现塑料废弃物的回收利用和协同生产氢气及增值化学品提供了一条碳中和且可扩展的道路。

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 52225606).

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  1. International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, Xi’an, 710049, China

    Rui-Zhe Wang, Zhi Lin, Yi-Qing Wang, Kai-Ni Zhang & Shao-Hua Shen

  2. School of Civil and Architecture Engineering, Xi’an Technological University, Xi’an, 710021, China

    Ge-Hong Zhang & Jie Zhang

  3. Department of Mechanical Engineering, University of California at Berkeley, Berkeley, CA, 94720, USA

    Samuel S. Mao

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Wang, RZ., Lin, Z., Wang, YQ. et al. A direct polymeric carbon nitride/tungsten oxide Z-scheme heterostructure for efficient photocatalytic hydrogen generation via reforming of plastics into value-added chemicals. Rare Met. (2024). https://doi.org/10.1007/s12598-024-02714-9

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  • DOI: https://doi.org/10.1007/s12598-024-02714-9

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