Chinese Journal of Catalysis ›› 2023, Vol. 55: 171-181.DOI: 10.1016/S1872-2067(23)64559-0

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A synchronous defluorination-oxidation process for efficient mineralization of fluoroarenes with photoelectrocatalysis

Haibo Chia,b, Wangyin Wangb, Jiangping Mab,c, Ruizhi Duanb,c, Chunmei Dingb, Rui Songb,c, Can Lia,b,c,*()   

  1. aSchool of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, Anhui, China
    bState Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
    cKey Laboratory of advanced catalysis, Gansu Province; State Key Laboratory of Applied Organic Chemistry College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, Gansu, China
  • Received:2023-09-25 Accepted:2023-11-06 Online:2023-12-18 Published:2023-12-07
  • Contact: *E-mail: canli@dicp.ac.cn (C. Li).
  • Supported by:
    National Natural Science Foundation of China(22088102);National Natural Science Foundation of China(22372162);LiaoNing Revitalization Talents Program(XLYC2007002);Youth Innovation Promotion Association CAS(2022178)

Abstract:

Fluoroarene (FA) derivatives are persistent, toxic, and bioaccumulative pollutants, which pose severe risks to ecosystems and human health. Efficient cleavage of C-F bonds and complete mineralization of defluorinated intermediates are the keys for the deep treatment of FAs due to the high dissociation energy of C-F bonds and the high stability of aromatic rings. Herein, we report a synchronous defluorination-oxidation process using a photoelectrocatalytic device with a TiO2 photoanode, in which FAs are selectively cleavage of C-F bonds by photolysis and subsequently efficient oxidized by on-site generated •OH radical. Complete defluorination and mineralization (both over 99.9%) of 4-fluorophenol are achieved under irradiation at 1.0 VRHE in 120 min, the apparent reaction rate constant is 14.4 g h-1 m-2. This synchronous defluorination-oxidation process provides an efficient and practical technique for the mineralization of FAs in wastewater under mild conditions.

Key words: Wastewater treatment, Fluoroarene, Photoelectrocatalytic degradation, Defluorination, Total organic carbon removal