Is Sulfate Radical Really Generated from Peroxydisulfate Activated by Iron(II) for Environmental Decontamination?

  • Zhen Wang
    Zhen Wang
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    More by Zhen Wang
  • Jin Jiang*
    Jin Jiang
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    *E-mail: [email protected] or [email protected]
    More by Jin Jiang
  • Suyan Pang
    Suyan Pang
    School of Municipal and Environmental Engineering, Jilin Jianzhu University, Changchun 130118, China
    More by Suyan Pang
  • Yang Zhou
    Yang Zhou
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    More by Yang Zhou
  • Chaoting Guan
    Chaoting Guan
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
  • Yuan Gao
    Yuan Gao
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    More by Yuan Gao
  • Juan Li
    Juan Li
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    More by Juan Li
  • Yi Yang
    Yi Yang
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    More by Yi Yang
  • Wei Qiu
    Wei Qiu
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
    More by Wei Qiu
  • , and 
  • Chengchun Jiang
    Chengchun Jiang
    School of Civil and Environmental Engineering, Shenzhen Polytechnic, Shenzhen 518055, China
Cite this: Environ. Sci. Technol. 2018, 52, 19, 11276–11284
Publication Date (Web):September 12, 2018
https://doi.org/10.1021/acs.est.8b02266
Copyright © 2018 American Chemical Society
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Abstract

It is well documented that the traditional Fenton reagent (i.e., the combination of Fe(II) and H2O2) produces hydroxyl radical (OH) under acidic conditions, while at near-neutral pH the reactive intermediate converts to ferryl ion (Fe(IV)) that can oxidize sulfoxides to produce corresponding sulfones, markedly differing from their OH-induced products. However, it remains unclear whether Fe(IV) is generated in the Fe(II) activated peroxydisulfate (PDS) process, where sulfate radical (SO4•–) is long recognized as the dominant intermediate in literature. Here we demonstrated that SO4•– oxidized methyl phenyl sulfoxide (PMSO, a model sulfoxide) to produce biphenyl compounds rather than methyl phenyl sulfone (PMSO2). Interestingly, the formation of PMSO2 was observed when PMSO was treated by the Fe(II)/PDS system over a wide pH range, and the yields of PMSO2 were quantified to be ∼100% at acidic pH 3–5. The identification of Fe(IV) in the Fe(II)/PDS system could also reasonably explain the literature results on alcohol scavenging effect and ESR spectra analysis. Further, a Fe(IV)-based kinetic model was shown to accurately simulate the experimental data. This work urges re-evaluation of the Fe(II)/PDS system for environmental decontamination, given that Fe(IV) would have different reactivity toward environmental contaminants compared with SO4•– and/or OH.

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  • Additional information on the identification of PMSO oxidation products, competition kinetic experiments, TMSO transformation experiments, alcohol scavenging experiments, and ESR spectra, as well as kinetic model simulation (PDF)

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