SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2024, Vol. 71 ›› Issue (7): 235-248.DOI: 10.1016/j.cjche.2024.03.027

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Mesoporous amorphous FeOOH-encapsulated BiO2–x photocatalyst with harnessing broad spectrum toward activation of persulfate for tetracycline degradation

Pengfei Wu1,2, Zhaolong Liu2,3, Li Wu4, Yingkun Zhang2,3, Bing Wang2, Zhanghao Cheng2,3, Wenquan Cui3, Xiangyang Lv2, Qingling Liu1   

  1. 1. Tianjin Key Laboratory of Indoor Air Environmental Quality Control, School of Environmental Science and Engineering, Tianjin University, Tianjin 300350, China;
    2. Hebei Pollution Control Technology Innovation Center of Steel and Coking Industry, Department of Environmental and Chemical Engineering, Hebei College of Industry and Technology, Shijiazhuang 050091, China;
    3. Hebei Key Laboratory of Environmental Photocatalytic and Electrocatalytic Materials, College of Chemical Engineering, North China University of Science and Technology, Tangshan 063210, China;
    4. Hebei Academy of Product Quality Supervision & Inspection, Shijiazhuang 050227, China
  • Received:2023-08-22 Revised:2024-03-21 Online:2024-08-30 Published:2024-07-28
  • Contact: Xiangyang Lv,E-mail:wuherui@126.com;Qingling Liu,E-mail:liuql@tju.edu.cn
  • Supported by:
    This work was supported by the National Key Research and Development Program of China (2019YFC1904100), the National Natural Science Foundation of China (21503144), the Science and Technology Innovation Project for Students of Hebei Province (22E50174D), the Science and Technology Project of Hebei Education Department (QN2021047), the Program of Hebei Vocational University of Industry and Technology (dxs202207, ZY202401), and the Key Program of Natural Science of Hebei Province (B2020209017).

Mesoporous amorphous FeOOH-encapsulated BiO2–x photocatalyst with harnessing broad spectrum toward activation of persulfate for tetracycline degradation

Pengfei Wu1,2, Zhaolong Liu2,3, Li Wu4, Yingkun Zhang2,3, Bing Wang2, Zhanghao Cheng2,3, Wenquan Cui3, Xiangyang Lv2, Qingling Liu1   

  1. 1. Tianjin Key Laboratory of Indoor Air Environmental Quality Control, School of Environmental Science and Engineering, Tianjin University, Tianjin 300350, China;
    2. Hebei Pollution Control Technology Innovation Center of Steel and Coking Industry, Department of Environmental and Chemical Engineering, Hebei College of Industry and Technology, Shijiazhuang 050091, China;
    3. Hebei Key Laboratory of Environmental Photocatalytic and Electrocatalytic Materials, College of Chemical Engineering, North China University of Science and Technology, Tangshan 063210, China;
    4. Hebei Academy of Product Quality Supervision & Inspection, Shijiazhuang 050227, China
  • 通讯作者: Xiangyang Lv,E-mail:wuherui@126.com;Qingling Liu,E-mail:liuql@tju.edu.cn
  • 基金资助:
    This work was supported by the National Key Research and Development Program of China (2019YFC1904100), the National Natural Science Foundation of China (21503144), the Science and Technology Innovation Project for Students of Hebei Province (22E50174D), the Science and Technology Project of Hebei Education Department (QN2021047), the Program of Hebei Vocational University of Industry and Technology (dxs202207, ZY202401), and the Key Program of Natural Science of Hebei Province (B2020209017).

Abstract: With the growing concern about the water environment, the advanced oxidation process of persulfate activation assisted by photocatalysis has attracted considerable attention to decompose dissolved organic micropollutants. In this work, to overcome the drawbacks of the photocatalytic activity reduction caused by the photo-corrosion of non-stoichiometric BiO2–x, a novel material with amorphous FeOOH in situ grown on layered BiO2–x to form a core-shell structure similar to popcorn chicken-like morphology was produced in two simple and environmentally beneficial steps. Through a series of degradation activity tests of hybrid materials under different conditions, the as-prepared materials exhibited remarkable degradation activity and stability toward tetracycline in the FeOOH@BiO2–x/Vis/PS system due to the synergism of photocatalysis and persulfate activation. The results of XRD, SEM, TEM, XPS, FTIR, and BET show that the loading of FeOOH increases the specific surface area and active sites appreciably; the heterogeneous structure formed by FeOOH and BiO2–x is more favorable to the effective separation of photogenerated carriers. The optimal degradation conditions were at a catalyst addition of 0.7 g·L–1, a persulfate concentration of 1.0 g·L–1, and an initial pH of 4.5, at which the degradation rate could reach 94.7% after 90 min. The influence of typical inorganic anions on degradation was also examined. ESR studies and radical quenching experiments revealed that ·OH, SO4-·, and ·O2- were the principal active species generated during the degradation of tetracycline. The results of the 1,10-phenanthroline approach proved that the effect of dissolved iron ions on the tetracycline degradation was limited, and the interfacial reaction that occurs on the active sites on the material's surface was a critical factor. This work provides a novel method for producing efficient broad-spectrum Bismuth-based composite photocatalysts and photocatalytic-activated persulfate synergistic degradation of tetracycline.

Key words: Amorphous FeOOH, BiO2–x, Activated persulfate, Photocatalytic, Tetracycline degradation

摘要: With the growing concern about the water environment, the advanced oxidation process of persulfate activation assisted by photocatalysis has attracted considerable attention to decompose dissolved organic micropollutants. In this work, to overcome the drawbacks of the photocatalytic activity reduction caused by the photo-corrosion of non-stoichiometric BiO2–x, a novel material with amorphous FeOOH in situ grown on layered BiO2–x to form a core-shell structure similar to popcorn chicken-like morphology was produced in two simple and environmentally beneficial steps. Through a series of degradation activity tests of hybrid materials under different conditions, the as-prepared materials exhibited remarkable degradation activity and stability toward tetracycline in the FeOOH@BiO2–x/Vis/PS system due to the synergism of photocatalysis and persulfate activation. The results of XRD, SEM, TEM, XPS, FTIR, and BET show that the loading of FeOOH increases the specific surface area and active sites appreciably; the heterogeneous structure formed by FeOOH and BiO2–x is more favorable to the effective separation of photogenerated carriers. The optimal degradation conditions were at a catalyst addition of 0.7 g·L–1, a persulfate concentration of 1.0 g·L–1, and an initial pH of 4.5, at which the degradation rate could reach 94.7% after 90 min. The influence of typical inorganic anions on degradation was also examined. ESR studies and radical quenching experiments revealed that ·OH, SO4-·, and ·O2- were the principal active species generated during the degradation of tetracycline. The results of the 1,10-phenanthroline approach proved that the effect of dissolved iron ions on the tetracycline degradation was limited, and the interfacial reaction that occurs on the active sites on the material's surface was a critical factor. This work provides a novel method for producing efficient broad-spectrum Bismuth-based composite photocatalysts and photocatalytic-activated persulfate synergistic degradation of tetracycline.

关键词: Amorphous FeOOH, BiO2–x, Activated persulfate, Photocatalytic, Tetracycline degradation