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Peroxydisulfate Activation and Singlet Oxygen Generation by Oxygen Vacancy for Degradation of Contaminants

  • Yongguang Bu
    Yongguang Bu
    State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
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  • 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, Nanjing 210094, China
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  • Wenjing Yu
    Wenjing Yu
    School of Environment and Chemical Engineering, Shenyang University of Technology, Shenyang 110870, China
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  • Yifan Pan
    Yifan Pan
    State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
    More by Yifan Pan
  • Lijun Li
    Lijun Li
    State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
    More by Lijun Li
  • Yanfeng Wang
    Yanfeng Wang
    State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
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  • Liangtao Pu
    Liangtao Pu
    State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
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  • Jie Ding
    Jie Ding
    State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
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  • Guandao Gao*
    Guandao Gao
    State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
    Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing 210023, China
    *Email: [email protected]. Tel/Fax: +86-25-89681675.
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  • , and 
  • Bingcai Pan
    Bingcai Pan
    State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
    Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing 210023, China
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Cite this: Environ. Sci. Technol. 2021, 55, 3, 2110–2120
Publication Date (Web):January 11, 2021
https://doi.org/10.1021/acs.est.0c07274
Copyright © 2021 American Chemical Society
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Abstract

Oxygen vacancies (OVs) play a crucial role in the catalytic activity of metal-based catalysts; however, their activation mechanism toward peroxydisulfate (PDS) still lacks reasonable explanation. In this study, by taking bismuth bromide (BiOBr) as an example, we report an OV-mediated PDS activation process for degradation of bisphenol A (BPA) employing singlet oxygen (1O2) as the main reactive species under alkaline conditions. The experimental results show that the removal efficiency of BPA is proportional to the number of OVs and is highly related to the dosage of PDS and the catalyst. The surface OVs of BiOBr provide ideal sites for the inclusion of hydroxyl ions (HO) to form BiIII–OH species, which are regarded as the major active sites for the adsorption and activation of PDS. Unexpectedly, the activation of PDS occurs through a nonradical mechanism mediated by 1O2, which is generated via multistep reactions, involving the formation of an intermediate superoxide radical (O2•–) and the redox cycle of Bi(III)/Bi(IV). This work is dedicated to the in-depth mechanism study into PDS activation over OV-rich BiOBr samples and provides a novel perspective for the activation of peroxides by defective materials in the absence of additional energy supply or aqueous transition metal ions.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c07274.

  • One scheme, two tables, four texts and 24 figures are shown, including, possible oxidative degradation pathway of BPA by 1O2 (Scheme S1); the change of solution pH during the reaction process in the BOB-OV/PDS system (Table S1); mass fragment ions (m/z) of intermediates and BPA obtained from UHPLC-MS spectra (Table S2); HPLC methods (Text S1); UHPLC-MS analysis methods (Text S2); the kinetic models fit the degradation kinetic curves of BPA in different systems (Text S3); experimental procedures of alkali pretreatment of BOB-OV (Text S4); the adsorption capacity of BiOBr samples toward BPA in the dark under stirring for 30 min (Figure S1); specific surface area of BiOBr samples (Figure S2); analysis of XRD patterns (Figures S3, S4, S8b, and S12); OV content of BiOBr samples (Figures S5 and S24a); analysis of XPS spectrum (Figures S6 and S20); HRTEM and SAED images of BOB-OV (Figure S7); the removal ratio of BPA in Bi3+/PDS, Bi(OH)3/PDS and Bi2O3/PDS systems (Figure S8a); the pseudo-first-order kinetic constant fits the degradation kinetic curves of BPA (Figures S9 and S13); the linear relationship between the content of OVs in BiOBr samples and the kobs fit the degradation kinetic curves of BPA in different systems (Figure S10); the zero-point charge of BOB-OV (Figure S11); the removal ratio of BPA in the BOB-OV/PDS systems with 12.5 mM HCl added at different times (Figure S14); analysis of the EPR spectra (Figures S15, S16, S18, and S22); the removal ratio of BPA in the BOB-OV/PDS system with N2 or O2 bubbling (Figure S17); the removal ratio of TOC in the BOB-OV/PDS system at 15 min (Figure S19); decomposition of PDS by BOB-OV and A-BOB-OV in aqueous solution (Figure S21); the removal ratio of BPA in the A-BOB-OV/PDS system (Figure S23); and reusability tests on BOB-OV for the removal of BPA in the BOB-OV/PDS system at 15 min (Figure S24b) (PDF)

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