Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (7): 1927-1936.DOI: 10.1016/S1872-2067(21)64050-0

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Ultradurable fluorinated V2AlC for peroxymonosulfate activation in organic pollutant degradation processes

Chao Lia,, Chenjie Songa,b,, Hui Lic, Liqun Yea,b,*(), Yixue Xua,b, Yingping Huangd, Gongzhe Niea, Rumeng Zhanga, Wei Liua,b, Niu Huanga,b, Po Keung Wonge, Tianyi Mac,#()   

  1. aKey Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, College of Materials and Chemical Engineering, China Three Gorges University, Yichang 443002, Hubei, China
    bHubei Three Gorges Laboratory,Yichang 443007, Hubei, China
    cSchool of Science, RMIT University, Melbourne, VIC 3000, Australia
    dEngineering Research Center of Eco-environment in Three Gorges Reservoir Region, Ministry of Education, China Three Gorges University, Yichang 443002, Hubei, China
    eSchool of Life Sciences, The Chinese University of Hong Kong, Shatin, Hong Kong SAR, China
  • Received:2022-03-20 Accepted:2022-03-29 Online:2022-07-18 Published:2022-05-20
  • Contact: Liqun Ye, Tianyi Ma
  • About author:First author contact:

    Contributed equally to this work.

  • Supported by:
    National Natural Science Foundation of China(51872147);National Natural Science Foundation of China(22136003);111 Project(D20015)

Abstract:

Vanadium-based catalysts are considered the most promising materials to replace cobalt-based catalysts for the activation of peroxymonosulfate (PMS) to degrade organic pollutants. However, these traditional vanadium species easily leak out metal ions that can affect the environment, even though the of vanadium is much less than that of cobalt. Compared to other vanadium-based catalysts, e.g., V2O3, fluorinated V2AlC shows a high and constant activity and reusability regarding PMS activation. Furthermore, it features extremely low ion leakage. Active oxygen species scavenging and electron spin resonance measurements reveal that the main reactive oxygen species was 1O2, which was induced by a two-dimensional confinement effect. More importantly, for the real-life application of tetracycline (TC) degradation, the introduction of fluorine changed the adsorption mode of TC over the catalyst, thereby changing the degradation path. The intermediate products were detected by liquid-chromatography mass spectroscopy (LC-MS), and a possible degradation path was proposed. The environmental impact test of the decomposition products showed that the toxicity of the degradation intermediates was greatly reduced. Therefore, the investigated ultradurable catalyst material provides a basis for the practical application of advanced PMS oxidation technology.

Key words: Fluorination, Advance oxidation technology, V2AlC, Reactive oxygen species