Chinese Journal of Catalysis

Chinese Journal of Catalysis ›› 2023, Vol. 51: 101-112.DOI: 10.1016/S1872-2067(23)64479-1

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MIL-101(Fe)/BiOBr S-scheme photocatalyst for promoting photocatalytic abatement of Cr(VI) and enrofloxacin antibiotic: Performance and mechanism

Shijie Lia,*(), Chunchun Wanga, Kexin Donga, Peng Zhangb, Xiaobo Chenc,*(), Xin Lid,*()   

  1. aKey Laboratory of Health Risk Factors for Seafood of Zhejiang Province, National Engineering Research Center for Marine Aquaculture, College of Marine Science and Technology, Zhejiang Ocean University, Zhoushan 316022, Zhejiang, China
    bState Centre for International Cooperation on Designer Low-carbon and Environmental Materials (CDLCEM), School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, Henan, China
    cDepartment of Chemistry, University of Missouri-Kansas City, MO 64110, USA
    dInstitute of Biomass Engineering, Key Laboratory of Energy Plants Resource and Utilization, Ministry of Agriculture and Rural Affairs, South China Agricultural University, Guangzhou 510642, Guangdong, China
  • Received:2023-03-02 Accepted:2023-05-08 Online:2023-08-18 Published:2023-09-11
  • Contact: *E-mail: lishijie@zjou.edu.cn (S. Li), chenxiaobo@umkc.edu (X. Chen), xinli@scau.edu.cn (X. Li).
  • Supported by:
    National Natural Science Foundation of China(U1809214);National Natural Science Foundation of China(51708504);Natural Science Foundation of Zhejiang Province(LY20E080014);Natural Science Foundation of Zhejiang Province(TGN23E080003);Science and Technology Project of Zhoushan(2022C41011)

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Abstract:

The development of highly active, economical, and robust bifunctional photocatalysts is a priority for sustainable photocatalytic water remediation. Inadequately available reactive sites and sluggish interface photocarrier transfer and separation remain significant challenges in the photoreaction progress. In this study, the Fe-containing metal-organic framework (MOF) MIL-101(Fe) was integrated with BiOBr microspheres to form a competent S-scheme heterostructure for the photocatalytic mitigation of Cr(VI) and enrofloxacin (ENR) antibiotics. The optimal MIL-101(Fe)/BiOBr exhibited the highest photoactivity, with 99.4% of Cr(VI) and 84.4% of ENR eliminated upon visible-light illumination in a single-pollutant system. The photoactivity of MIL-101(Fe)/BiOBr in the decontamination of the Cr(VI)-ENR co-existence system exhibited a substantial enhancement when compared to that in a single system, owing to the improved utilization of electrons and holes resulting from the synergism between Cr(VI), ENR, and the photocatalyst. The enhanced photoactivity is attributed to two aspects: (1) the incorporation of MIL-101(Fe) results in an increased number of available reactive sites and improved solar harvesting properties; and (2) the S-scheme mechanism enables the effective spatial disassociation of photoexcited carriers and optimization of the photo-redox capability of the system. Through scavenging experiments, electron spin resonance characterization, liquid chromatography-tandem mass spectrometry analysis, and T.E.S.T. theoretical estimation, the catalytic mechanism, antibiotic degradation process, and biotoxicities of the degraded products were analyzed and confirmed. This study provides a viable strategy for building competent MOF-inorganic semiconductor S-scheme photocatalysts with superior photocatalytic decontamination performance.

Key words: MIL-101(Fe)/BiOBr, S-scheme heterostructure, Cr(VI) reduction, Antibiotic degradation, Metal-organic framework