New Insights into the Activation of Peracetic Acid by Co(II): Role of Co(II)-Peracetic Acid Complex as the Dominant Intermediate Oxidant

  • Zihao Zhao
    Zihao Zhao
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
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  • Xinhong Li
    Xinhong Li
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
    More by Xinhong Li
  • Hongchao Li*
    Hongchao Li
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
    *(H.L.) Phone: +86-18680581522; Email: [email protected]
    More by Hongchao Li
  • Jieshu Qian
    Jieshu Qian
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
    Research Center for Environmental Nanotechnology (ReCENT), State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
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  • , and 
  • Bingcai Pan
    Bingcai Pan
    Research Center for Environmental Nanotechnology (ReCENT), State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
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Cite this: ACS EST Engg. 2021, 1, 10, 1432–1440
Publication Date (Web):August 23, 2021
https://doi.org/10.1021/acsestengg.1c00166
Copyright © 2021 American Chemical Society
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Abstract

The combination of Co(II) and peracetic acid (PAA) is an important alternative advanced oxidation process (AOPs), in which R-O radicals including acetyloxyl radicals (CH3C(O)O) and acetylperoxyl radicals (CH3C(O)OO) have been considered to be the primary reactive species for the oxidative degradation of contaminants. However, it is still unclear how the active Co species participates in this process. In this study, we conduct a series of experiments including chemical probing, radical quenching, electron paramagnetic resonance (EPR), and Co(III) oxidation to investigate the degradation mechanism of contaminants in the Co(II)/PAA process, using bisphenol A (BPA) as target pollutant. On the basis of these results, we propose a Co(II)-PAA complex (Co(II)-OO(O)CCH3) to be the primary reactive species, while R-O radicals and Co(III) (available as dimeric Co-peroxide species) derived from the decomposition of Co(II)-PAA complex are the minor contributors for the oxidation of BPA. Factors, including PAA concentration, Co(II) concentration, solution pH, inorganic anions, and natural organic matters (NOM), that might affect the oxidation performance of the Co(II)/PAA process were also investigated systematically. This study sheds new light on the mechanistic understanding of the Co(II)/PAA process for the oxidation of contaminants in water.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsestengg.1c00166.

  • Analytical methods (Text S1), operating conditions for HPLC and HPLC-MS (Text S2 and Table S1), values of solution pH before and after reaction (Table S2), oxidation of MPSO and its degradation products in different systems (Figure S1–S4), degradation of CBZ (Figure S5), generation of HCHO (Figure S6), EPR signals in Co(III) solution (Figure S7), degradation of MPSO and BPA in Co(III) solution (Figure S8 and S9), Raman spectra (Figure S10), degradation of BPA in PAA alone (Figure S11), distribution of Co and PAA species (Figure S12), decomposition of PAA (Figure S13), pseudo-first-order rate constant of BPA removal (Figure S14), and effect of H2O2 concentration on the removal of BPA (Figure S15) (PDF)

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