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Nonradical Oxidation of Pollutants with Single-Atom-Fe(III)-Activated Persulfate: Fe(V) Being the Possible Intermediate Oxidant

  • Ning Jiang
    Ning Jiang
    Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
    University of Chinese Academy of Sciences, Beijing 100049, China
    More by Ning Jiang
  • Haodan Xu
    Haodan Xu
    Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
    More by Haodan Xu
  • Lihong Wang
    Lihong Wang
    Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
    More by Lihong Wang
  • Jin Jiang
    Jin Jiang
    Institute of Environmental and Ecological Engineering, Guangdong University of Technology, Guangzhou 510006, China
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  • , and 
  • Tao Zhang*
    Tao Zhang
    Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
    *Email: [email protected]
    More by Tao Zhang
Cite this: Environ. Sci. Technol. 2020, 54, 21, 14057–14065
Publication Date (Web):October 23, 2020
https://doi.org/10.1021/acs.est.0c04867
Copyright © 2020 American Chemical Society
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Abstract

When applied for the remediation of polluted water/soil, peroxydisulfate (PDS) usually needs to be effectively activated to generate sulfate radical as the working oxidant. However, a significant part of the oxidation capacity of PDS is lost in this way because sulfate radical unselectively reacts with most of the substances in water/soil. PDS activation without generating radicals is preferred to maximize its oxidation capacity for targeted pollutants. Here, we report that single-atom Fe(III)- and nitrogen-doped carbon (Fe–N–C) can efficiently activate PDS to selectively remove some organic pollutants following an unreported nonradical pathway. The single-atom Fe(III) coordinated with pyridinic N atoms was confirmed to be the active site for the catalytic decomposition of PDS. However, the PDS decomposition did not produce radicals or reactive oxygen species. It is very likely that the coordinated Fe(III) is readily converted to Fe(V) through two-electron abstraction by PDS, and Fe(V) is responsible for the selective degradation of organic pollutants. The PDS/Fe–N–C-coupled process utilizes more oxidation capacity of PDS than both radical oxidation and other reported nonradical oxidation like PDS/CuO under the same experimental conditions. This process provides a new approach to selectively degrade some organic pollutants through PDS activation.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c04867.

  • Chemicals and materials used in this study; DMPO- and TMP-trapping ESR experiment; electrochemical characterization; molecular structures of the organics used in this study; HPLC conditions for the analysis of the pollutants; Eo values obtained from the XANES spectra; TEM images, SAED, and elemental maps of the as-prepared sample; XPS N 1s, O 1s, and C 1s spectra of Fe-N-C; influence of sulfate on 2,4-DCP degradation during PDS/Fe-N-C-coupled oxidation; oxalate degradation during PDS/Fe-N-C-coupled oxidation; KSCN decomposition (100 μM) and its influence on 2,4-DCP degradation in the PDS/Fe-N-C-coupled oxidation; TEM images of FeNP-N-C; degradation of PMSO by the PDS/FeNP-N-C-coupled oxidation; EPR spectra of PDS, Fe-N-C, and PDS/Fe-N-C; EIS Nyquist plots of N-C and Fe-N-C, current response at the N-C and Fe-N-C-coated working electrode, and LSV curves of Fe-N-C under different conditions, if added, [PDS]o = 2 mM and [2,4-DCP]o = 40 μM; GC/MS chromatograms of 2,4-DCP solution after PDS/Fe-N-C oxidation; influence of pH on 2,4-DCP degradation and Fe ion leaching by PDS/Fe-N-C oxidation; 2,4-DCP degradation by the PDS/Fe3+-coupled system; zeta-potential of Fe-N-C under different pHs; comparison of PDS/Fe-N-C with PDS/CuO for 2,4-DCP degradation; 2,4-DCP concentration in the effluent from a continuous-flow column; and removal of selected pollutants by the PDS/Fe-N-C-coupled oxidation (PDF)

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