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Thermal Activation of Peracetic Acid in Aquatic Solution: The Mechanism and Application to Degrade Sulfamethoxazole

  • Jingwen Wang
    Jingwen Wang
    School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
    More by Jingwen Wang
  • Ying Wan
    Ying Wan
    School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
    More by Ying Wan
  • Jiaqi Ding
    Jiaqi Ding
    School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
    More by Jiaqi Ding
  • Zongping Wang
    Zongping Wang
    School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
  • Jun Ma
    Jun Ma
    State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, China
    More by Jun Ma
  • Pengchao Xie*
    Pengchao Xie
    School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
    Center for the Environmental Implications of Nanotechnology (CEINT), Durham, North Carolina 27708-0287, United States
    *Email: [email protected]
    More by Pengchao Xie
  • , and 
  • Mark R. Wiesner
    Mark R. Wiesner
    Center for the Environmental Implications of Nanotechnology (CEINT), Durham, North Carolina 27708-0287, United States
Cite this: Environ. Sci. Technol. 2020, 54, 22, 14635–14645
Publication Date (Web):October 27, 2020
https://doi.org/10.1021/acs.est.0c02061
Copyright © 2020 American Chemical Society
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Abstract

Chemical oxidation using peracetic acid (PAA) can be enhanced by activation with the formation of reactive species such as organic radicals (R–O) and HO. Thermal activation is an alternative way for PAA activation, which was first applied to degrade micropollutants in this study. PAA is easily decomposed by heat via both radical and nonradical pathways. Our experimental results suggest that a series of reactive species including R–O, HO, and 1O2 can be produced through the thermal decomposition of PAA. Sulfamethoxazole (SMX), a typical sulfa drug, can be effectively removed by the thermoactivated PAA process under conditions of neutral pH. R–O including CH3C(O)O and CH3C(O)OO has been shown to play a primary role in the degradation of SMX followed by direct PAA oxidation in the thermoactivated PAA process. Both higher temperature (60 °C) and higher PAA dose benefit SMX degradation, while coexisting H2O2 inhibits SMX degradation in the thermoactivated PAA process. With a variation of solution pH, conditions near a neutral value show the best performance of this process in SMX degradation. Based on the identified intermediates, transformation of SMX was proposed to undergo oxidation of the amine group and oxidative coupling reactions. This study definitively illustrates the PAA decomposition pathways at high temperature in aquatic solution and addresses the possibility of the thermoactivated PAA process for contaminant destruction, demonstrating this process to be a feasible advanced oxidation process.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c02061.

  • Chemicals; oxidation product analysis; detection of gaseous CO2 released from PAA solution; determination of the role of HO by TBA; reaction rate between 1O2 and SMX at pH 7; fraction of HO reacting with SMX; contribution of direct oxidation of SMX by PAA; calculated energy use for the thermoactivated PAA process; details of the eluents and detection wavelengths of HPLC; reactions between CH3C(O)OO and organic compounds; bond electron density based on bond critical point analysis; predicted acute and chronic toxicity of SMX and TPs; kinetics of PAA decomposition at different pHs; EPR spectra; detection of gaseous CO2 released from PAA solution; concentration of the released O2 in solution; HCHO formation; degradation of FFA and SMX; effect of HA on SMX degradation; pseudo-first-order of SMX degradation; effect of extra addition of H2O2; consumed PAA and RSE values; optimized O–O bond lengths; product ion spectra; possible reaction pathways; and variation of P. phosphoreum T3 luminescence (PDF)

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