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Are Free Radicals the Primary Reactive Species in Co(II)-Mediated Activation of Peroxymonosulfate? New Evidence for the Role of the Co(II)–Peroxymonosulfate Complex

  • 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, 200 Xiao Ling Wei, Nanjing 210094, China
    More by Hongchao Li
  • 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, 200 Xiao Ling Wei, Nanjing 210094, China
    More by Zihao Zhao
  • 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, 200 Xiao Ling Wei, 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
    *Email: [email protected]
    More by Jieshu Qian
  • , 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
    More by Bingcai Pan
Cite this: Environ. Sci. Technol. 2021, 55, 9, 6397–6406
Publication Date (Web):April 22, 2021
https://doi.org/10.1021/acs.est.1c02015
Copyright © 2021 American Chemical Society

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    Abstract

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    The catalytic activation of peroxymonosulfate (PMS) is under intensive investigation with potentials as an alternative advanced oxidation process (AOP) in wastewater treatment. Among all catalysts examined, Co(II) exhibits the highest reactivity for the activation of PMS, following the conventional Fenton-like mechanism, in which free radicals (i.e., sulfate radicals and hydroxyl radicals) are reckoned as the reactive species. Herein, we report that the primary reactive species (PRS) is proposed to be a Co(II)–PMS complex (Co(II)–OOSO3), while free radicals and Co(III) species act as the secondary reactive species (SRS) that play a minor role in the Co(II)/PMS process. This Co(II)–OOSO3 exhibits several intriguing properties including ability to conduct both one-electron-transfer and oxygen-atom-transfer reactions with selected molecules, both nucleophilic and electrophilic in nature, and strongly pH-dependent reactivity. This study provides novel insights into the chemical nature of the Co(II)-catalyzed PMS activation process.

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    • Preparation of Co(III) solution, operating conditions for HPLC–MS analysis, calculation details, effects of Co(II) and PMS concentrations, water chemistry composition, parameters of HPLC analysis, list of various rate constants, the calculated scavenging percentages of radicals, and mechanism schemes (PDF)

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