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Synergy between Iron and Selenide on FeSe2(111) Surface Driving Peroxymonosulfate Activation for Efficient Degradation of Pollutants

  • 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
  • Teng Zhang
    Teng Zhang
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, P. R. China
    School of Earth and Environment, Anhui University of Science and Technology, Huainan 232001, P. R. China
    More by Teng Zhang
  • Hongbiao Cui
    Hongbiao Cui
    School of Earth and Environment, Anhui University of Science and Technology, Huainan 232001, P. R. China
    More by Hongbiao Cui
  • 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
  • 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
  • Juan Gao
    Juan Gao
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, P. R. China
    More by Juan Gao
  • 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
    *Email: [email protected]. Tel.: +86 25 86881182. Fax: +86 25 86881000.
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  • , 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
    State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, P. R. China
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Cite this: Environ. Sci. Technol. 2020, 54, 23, 15489–15498
Publication Date (Web):November 18, 2020
https://doi.org/10.1021/acs.est.0c06091
Copyright © 2020 American Chemical Society
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Abstract

In this study, iron selenide nanoparticles (FeSe2) were synthesized and applied in Fenton-like reactions for degradation of pollutants. It was found that FeSe2 exerts excellent catalytic reactivity toward different oxidants including peroxymonosulfate (PMS), peroxydisulfate, and H2O2, which can degrade a wide range of pollutants such as 2,4,4′-trichlorobiphenyl, bisphenol A, sulfamethoxazole, chlortetracycline, and perfluorooctanoic acid, with the degradation efficiency and TOC removal of pollutants reaching 55–95 and 20.3–50.9%, respectively. The mechanism of PMS activation by FeSe2 was elucidated, and the synergistic effect between Fe and Se for PMS activation was discovered to be the dominant catalytic mechanism, as evidenced by free-radical quenching, electron paramagnetic resonance, and density functional theory studies. Briefly, the Fe(II) site on the FeSe2 surface (111) accounted for PMS activation, while the reducing Se species on the surface not only acted as an electron donor contributing to Fe(II) regeneration but also produced Se vacancies further facilitating Fe(II) regeneration to improve the performance of PMS activation. In addition, FeSe2 exhibited high catalytic activity and stability for PMS activation with different pH, and can degrade PCBs efficiently in the presence of anions, natural organic matter water matrices or in complex soil eluents. This study presents the development and evaluation of FeSe2 as a novel and highly efficient activator that exhibits promise for practical applications for the degradation of pollutants in wastewater and soil wash eluent with Fenton-like reactions.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c06091.

  • Chemicals; analytic methods; DFT calculations; comparison of FeSe2 with other metal-based catalysts; calculated surface energy (Table S1); calculated Bader charge (Table S2); calculated decomposition energies (Table S3); types and concentrations of PCBs (Table S4); comparison of performance of FeSe2 with other catalysts (Table S5); characterizations of FeSe2 (Figure S1); TEM images (Figure S2); kinetics of PCB28 decay (Figure S3); total ion current chromatogram (Figure S4); catalytic activation of oxidants (Figure S5); EPR spectra (Figure S6 and S8); kinetics of PCB28 adsorption (Figure S7); effects of 2,2-bipyridine on PCB28 degradation (Figure S9); effects of Fe3+ ion addition on PCB28 degradation (Figure S10); DFT optimized geometries (Figure S11); pseudo-first-order fitting (Figure S12); effects of different anions and humic acid on PCB28 degradation (Figure S13); and degradation of PCBs by FeSe2/PMS (Figure S14) (PDF)

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