Persulfate Activation on Crystallographic Manganese Oxides: Mechanism of Singlet Oxygen Evolution for Nonradical Selective Degradation of Aqueous Contaminants

  • Shishu Zhu
    Shishu Zhu
    Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, Western Australia 6845, Australia
    State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, 73 Huanghe Road, Harbin 150090, P. R. China
    More by Shishu Zhu
  • Xiaojie Li
    Xiaojie Li
    Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, Western Australia 6845, Australia
    More by Xiaojie Li
  • Jian Kang
    Jian Kang
    Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, Western Australia 6845, Australia
    More by Jian Kang
  • Xiaoguang Duan*
    Xiaoguang Duan
    School of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, Australia
    *(X.D.) E-mail: [email protected]
  • , and 
  • Shaobin Wang*
    Shaobin Wang
    Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, Western Australia 6845, Australia
    School of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, Australia
    *(S.W.) E-mail: [email protected]
    More by Shaobin Wang
Cite this: Environ. Sci. Technol. 2019, 53, 1, 307–315
Publication Date (Web):November 27, 2018
https://doi.org/10.1021/acs.est.8b04669
Copyright © 2018 American Chemical Society
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Abstract

Minerals and transitional metal oxides of earth-abundant elements are desirable catalysts for in situ chemical oxidation in environmental remediation. However, catalytic activation of peroxydisulfate (PDS) by manganese oxides was barely investigated. In this study, one-dimension manganese dioxides (α- and β-MnO2) were discovered as effective PDS activators among the diverse manganese oxides for selective degradation of organic contaminants. Compared with other chemical states and crystallographic structures of manganese oxide, β-MnO2 nanorods exhibited the highest phenol degradation rate (0.044 min–1, 180 min) by activating PDS. A comprehensive study was conducted utilizing electron paramagnetic resonance, chemical probes, radical scavengers, and different solvents to identity the reactive oxygen species (ROS). Singlet oxygen (1O2) was unveiled to be the primary ROS, which was generated by direct oxidation or recombination of superoxide ions and radicals from a metastable manganese intermediate at neutral pH. The study dedicates to the first mechanistic study into PDS activation over manganese oxides and provides a novel catalytic system for selective removal of organic contaminants in wastewater.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b04669.

  • The details of preparation and characterization of manganese oxides. The methods of HPLC, EPR detection, and determination of PDS concentration. Analysis of XRD patterns. The methods of LC–MS. Results of phenol removal by manganese oxides alone and Mn leaching. The phenol degradation rates by different manganese oxides. Crystal structures of Mn2O3 and Mn3O4. TEM and N2 adsorption/desorption results. The degradation rates of different organics. Results of quenching effect. The first order kinetic of FFA decay. PDS decomposition by β-MnO2, phenol, and β-MnO2/phenol. EPR results by DMPO. The phenol removal by PDS alone upon different pH values. XPS spectrum results. FTIR and Raman results. The kinetic model of overall reactions (PDF)

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