Mechanisms of Interaction between Persulfate and Soil Constituents: Activation, Free Radical Formation, Conversion, and Identification

  • Guodong Fang
    Guodong Fang
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, P.R. China
    More by Guodong Fang
  • Xiru Chen
    Xiru Chen
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, P.R. China
    University of Chinese Academy of Sciences, Beijing 100049, P.R. China
    More by Xiru Chen
  • Wenhui Wu
    Wenhui Wu
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, P.R. China
    More by Wenhui Wu
  • Cun Liu
    Cun Liu
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, P.R. China
    More by Cun Liu
  • Dionysios D. Dionysiou
    Dionysios D. Dionysiou
    Environmental Engineering and Science Program, Department of Chemical and Environmental Engineering (ChEE), University of Cincinnati, Cincinnati, Ohio 45221-0071, United States
  • Tingting Fan
    Tingting Fan
    Nanjing Institute of Environmental Science, Ministry of Environmental Protection of the People’s Republic of China, Nanjing 210042, P.R. China
    More by Tingting Fan
  • Yujun Wang*
    Yujun Wang
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, P.R. China
    *Phone: 86-25-86881180; fax: 86-25-86881180; e-mail: [email protected] (Y.J.W.).
    More by Yujun Wang
  • Changyin Zhu
    Changyin Zhu
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, P.R. China
    More by Changyin Zhu
  • , and 
  • Dongmei Zhou*
    Dongmei Zhou
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, P.R. China
    *Phone: 86-25-86881180; fax: 86-25-86881180; e-mail: [email protected] (D.M.Z.).
    More by Dongmei Zhou
Cite this: Environ. Sci. Technol. 2018, 52, 24, 14352–14361
Publication Date (Web):November 14, 2018
https://doi.org/10.1021/acs.est.8b04766
Copyright © 2018 American Chemical Society
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Abstract

Persulfate-based in situ chemical oxidation (ISCO) for soil remediation has received great attention in recent years. However, the mechanisms of interaction between persulfate (PS) and soil constituents are not fully understood. In this study, PS decomposition, activation, free radical formation and conversion processes in 10 different soils were examined. The results showed that soil organic matter (SOM) was the dominant factor affecting PS decomposition in soil, but Fe/Mn-oxides were mainly responsible for PS decomposition when SOM was removed. Electron paramagnetic resonance (EPR) spectroscopy analysis showed that sulfate radicals (SO4•–) and hydroxyl radicals (•OH) generated from PS decomposition subsequently react with SOM to produce alkyl-like radicals (R), and this process is dependent on SOM content. R and SO4•–/•OH radicals predominated in soil with high and low SOM, respectively, and all three radicals coexist in soil with medium SOM. Chemical probe analysis further identified the types of radicals, and R can reductively degrade hexachloroethane in high SOM soil, while SO4•– and •OH oxidatively degrade phenol in low SOM soil. These findings provide valuable information for PS-ISCO, and new insight into the role of SOM in the remediation of contaminated soil.

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  • The properties of soils used in this study and the rates of PS decomposition in different soils, Tables S1, S2, and S3; and the kinetics of PS decomposition, correlation analysis, EPR simulation, and HCA and phenol degradation, Figures S1–S13 (PDF)

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