Tuning of Persulfate Activation from a Free Radical to a Nonradical Pathway through the Incorporation of Non-Redox Magnesium Oxide

  • Ali Jawad
    Ali Jawad
    Hubei Provincial Engineering Laboratory of Solid Waste Treatment, Disposal and Recycling, School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
    Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, and Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
    More by Ali Jawad
  • Kun Zhan
    Kun Zhan
    Hubei Provincial Engineering Laboratory of Solid Waste Treatment, Disposal and Recycling, School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
    More by Kun Zhan
  • Haibin Wang
    Haibin Wang
    Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, and Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
    More by Haibin Wang
  • Ajmal Shahzad
    Ajmal Shahzad
    Hubei Provincial Engineering Laboratory of Solid Waste Treatment, Disposal and Recycling, School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
  • Zehua Zeng
    Zehua Zeng
    Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, and Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
    More by Zehua Zeng
  • Jia Wang
    Jia Wang
    Hubei Provincial Engineering Laboratory of Solid Waste Treatment, Disposal and Recycling, School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
    More by Jia Wang
  • Xinquan Zhou
    Xinquan Zhou
    Hubei Provincial Engineering Laboratory of Solid Waste Treatment, Disposal and Recycling, School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
    More by Xinquan Zhou
  • Habib Ullah
    Habib Ullah
    Environment and Sustainably Institute (ESI), University of Exeter, Penryn Campus, Penryn, Cornwall TR109FE, United Kingdom
    More by Habib Ullah
  • Zhulei Chen
    Zhulei Chen
    Hubei Provincial Engineering Laboratory of Solid Waste Treatment, Disposal and Recycling, School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
    More by Zhulei Chen
  • , and 
  • Zhuqi Chen*
    Zhuqi Chen
    Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, and Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China
    *(Z.C.) Email: [email protected]
    More by Zhuqi Chen
Cite this: Environ. Sci. Technol. 2020, 54, 4, 2476–2488
Publication Date (Web):January 23, 2020
https://doi.org/10.1021/acs.est.9b04696
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Abstract

Nonradical-based advanced oxidation processes for pollutant removal have attracted much attention due to their inherent advantages. Herein we report that magnesium oxides (MgO) in CuOMgO/Fe3O4 not only enhanced the catalytic properties but also switched the free radical peroxymonosulfate (PMS)-activated process into the 1O2 based nonradical process. CuOMgO/Fe3O4 catalyst exhibited consistent performance in a wide pH range from 5.0 to 10.0, and the degradation kinetics were not inhibited by the common free radical scavengers, anions, or natural organic matter. Quantitative structure–activity relationships (QSARs) revealed the relationship between the degradation rate constant of 14 substituted phenols and their conventional descriptor variables (i.e., Hammett constants σ, σ, σ+), half-wave oxidation potential (E1/2), and pKa values. QSARs together with the kinetic isotopic effect (KIE) recognized the electron transfer as the dominant oxidation process. Characterizations and DFT calculation indicated that the incorporated MgO alters the copper sites to highly oxidized metal centers, offering a more suitable platform for PMS to generate metastable copper intermediates. These highly oxidized metals centers of copper played the key role in producing O2•– after accepting an electron from another PMS molecule, and finally 1O2 as sole reactive species was generated from the direct oxidation of O2•– through thermodynamically feasible reactions.

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