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Peroxymonosulfate Activation by Fe–Co–O-Codoped Graphite Carbon Nitride for Degradation of Sulfamethoxazole

  • Shizong Wang
    Shizong Wang
    Collaborative Innovation Center for Advanced Nuclear Energy Technology, INET, Tsinghua University, Beijing 100084, P. R. China
    More by Shizong Wang
  • Yong Liu
    Yong Liu
    College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, Sichuan 610068, P. R. China
    More by Yong Liu
  • , and 
  • Jianlong Wang*
    Jianlong Wang
    Collaborative Innovation Center for Advanced Nuclear Energy Technology, INET, Tsinghua University, Beijing 100084, P. R. China
    Beijing Key Laboratory of Radioactive Wastes Treatment, Tsinghua University, Beijing 100084, P. R. China
    *Email: [email protected]. Tel: +86-10-62784843. Fax: +861062771150.
Cite this: Environ. Sci. Technol. 2020, 54, 16, 10361–10369
Publication Date (Web):July 16, 2020
https://doi.org/10.1021/acs.est.0c03256
Copyright © 2020 American Chemical Society
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Abstract

Graphite carbon nitride (g-C3N4) has a stable structure but poor catalytic capability for activating peroxymonosulfate (PMS). In this study, the codoping of g-C3N4 with bimetallic oxides (iron and cobalt) and oxygen was investigated to enhance its catalytic capability. The results showed that iron, cobalt, and oxygen codoped g-C3N4 (Fe–Co–O–g-C3N4) was successfully prepared, which was capable of completely degrading sulfamethoxazole (SMX) (0.04 mM) within 30 min, with a reaction rate of 0.085 min–1, indicating the superior catalytic activity of Fe–Co–O–g-C3N4. The mineralization efficiency of SMX was 22.1%. Sulfate radicals and singlet oxygen were detected during the process of PMS activation. However, the role that singlet oxygen played in degrading SMX was not obvious. Surface-bound reactive species and sulfate radicals were responsible for SMX degradation, in which sulfate radicals contributed to 46.6% of SMX degradation. The superior catalytic activity was due to the synergistic effect of metal oxides and O–g-C3N4, in which O–g-C3N4 could act as a carrier and an activator as well as an electron mediator to promote the conversion of Fe(III) to Fe(II) and Co(III) to Co(II). Four main steps of SMX degradation were proposed, including direct oxidation of SMX, bond fission of N–C, bond fission of N–S, and bond fission of S–C. The effect of the pH, temperature, PMS concentration, chloridion, bicarbonate, and humic acids on SMX degradation was investigated. Cycling experiments demonstrated the good stability of Fe–Co–O–g-C3N4. This study first reported the preparation of bimetallic oxide and oxygen codoped g-C3N4, which was an effective PMS activator for degradation of toxic organic pollutants.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c03256.

  • Text S1, information of chemicals used in this study; Text S2, characterization of Fe–Co–O–g-C3N4; Text S3, analytical methods for HPLC and electrochemical analysis; Text S4, determination of the concentration and contributions of radicals and singlet oxygen; Figure S1, PMS decomposition during the process of SMX degradation; Figure S2, proposed degradation pathway of SMX; Figure S3, degradation mechanism study; Figure S4, first-order kinetics of atrazine and furfuryl alcohol by Fe–Co–O–g-C3N4-activated PMS; Figure S6, stability test of Fe–Co–O–g-C3N4; Figure S7, XPS image of Fe–Co–O–g-C3N4 after experiments; Figure S8, XRD image of Fe–Co–O–g-C3N4 after experiments; Figure S9, electric current density in the presence of O–g-C3N4; Figure S10, charge distribution of g-C3N4 before and after oxygen doping; and Table S1, binding energy of each element before and after the reaction (PDF)

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