Trace Cupric Species Triggered Decomposition of Peroxymonosulfate and Degradation of Organic Pollutants: Cu(III) Being the Primary and Selective Intermediate Oxidant

  • Lihong Wang
    Lihong Wang
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    Research Center for Eco-Environmental Sciences (RCEES), Chinese Academy of Sciences, Beijing 100085, China
    More by Lihong Wang
  • Haodan Xu
    Haodan Xu
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    Research Center for Eco-Environmental Sciences (RCEES), Chinese Academy of Sciences, Beijing 100085, China
    More by Haodan Xu
  • Ning Jiang
    Ning Jiang
    Research Center for Eco-Environmental Sciences (RCEES), Chinese Academy of Sciences, Beijing 100085, China
    More by Ning Jiang
  • Zimeng Wang
    Zimeng Wang
    Department of Environment Science and Engineering, Fudan University, Shanghai 200438, China
    More by Zimeng Wang
  • Jin Jiang*
    Jin Jiang
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    Institute of Environmental and Ecological Engineering, Guangdong University of Technology, Guangzhou 510006, China
    *Email: [email protected]
    More by Jin Jiang
  • , and 
  • Tao Zhang*
    Tao Zhang
    Research Center for Eco-Environmental Sciences (RCEES), Chinese Academy of Sciences, Beijing 100085, China
    *Email: [email protected]
    More by Tao Zhang
Cite this: Environ. Sci. Technol. 2020, 54, 7, 4686–4694
Publication Date (Web):March 4, 2020
https://doi.org/10.1021/acs.est.0c00284
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Abstract

Activation of persulfates to degrade refractory organic pollutants is currently a hot topic of advanced oxidation. Developing simple and effective activation approaches is crucial for the practical application of persulfates. We report in this research that trace cupric species (Cu(II) in several μM) can efficiently trigger peroxymonosulfate (PMS) oxidation of various organic pollutants under slightly alkaline conditions. The intermediate oxidant dominating this process was investigated with electron paramagnetic resonance (EPR), chemical probing, and in situ Raman spectroscopy. Unlike conventional PMS activation, which generates sulfate radical, hydroxyl radical, or singlet oxygen as major oxidants, Cu(III) was confirmed to be the primary and selective intermediate oxidant during the Cu(II)/PMS oxidation. Hydroxyl radical is the secondary intermediate oxidant formed from the reaction of Cu(III) with OH. Hybrid oxidation by the two oxidants imparts Cu(II)/PMS with high efficiency in the degradation of a series of pollutants. The results of this work suggest that, with no need of introducing complex catalysts, trace Cu(II) inherent in or artificially introduced to some water or wastewater can effectively trigger PMS oxidation of organic pollutants.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c00284.

  • Reagent sources; detection of 1,4-D with GC–MS; in situ confocal Raman analysis for the characterization of Cu(III) formed from PMS–Cu(II) interaction; calculation on MeOH and t-BuOH scavenging of OH in Cu(II)/PMS system; calculation on the fate of 1O2 in Cu(II)/PMS system; chemical structures of organic compounds and HPLC settings; comparison of degradation efficiency with other PMS activation processes; characteristics of real waters for the test; and formation pathway of DMPO–CH2OH adduct derived from the oxidation of methanol by OH and DMPO–OCH3 adduct derived from the oxidation of methanol by Cu(III) (PDF)

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