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Activation of Persulfates Using Siderite as a Source of Ferrous Ions: Sulfate Radical Production, Stoichiometric Efficiency, and Implications

  • Yong Feng
    Yong Feng
    Department of Civil Engineering, The University of Hong Kong, Pok Fu Lam, Hong Kong, China
    More by Yong Feng
  • Deli Wu
    Deli Wu
    State Key Laboratory of Pollution Control and Resources Reuse, School of Environmental Science & Engineering, Tongji University, Shanghai 200092, People’s Republic of China
    More by Deli Wu
  • Hailong Li
    Hailong Li
    Department of Civil Engineering, The University of Hong Kong, Pok Fu Lam, Hong Kong, China
    School of Energy Science and Engineering, Central South University, Changsha 410083, People’s Republic of China
    More by Hailong Li
  • Jianfeng Bai
    Jianfeng Bai
    School of Urban Development and Environmental Engineering, Shanghai Second Polytechnic University, Shanghai 201209, People’s Republic of China
    More by Jianfeng Bai
  • Yibo Hu
    Yibo Hu
    Department of Civil Engineering, The University of Hong Kong, Pok Fu Lam, Hong Kong, China
    More by Yibo Hu
  • Changzhong Liao
    Changzhong Liao
    Department of Civil Engineering, The University of Hong Kong, Pok Fu Lam, Hong Kong, China
    Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management, Guangdong Institute of Eco-Environmental Science & Technology, Guangzhou 510650, People’s Republic of China
  • Xiao-yan Li
    Xiao-yan Li
    Department of Civil Engineering, The University of Hong Kong, Pok Fu Lam, Hong Kong, China
    More by Xiao-yan Li
  • , and 
  • Kaimin Shih*
    Kaimin Shih
    Department of Civil Engineering, The University of Hong Kong, Pok Fu Lam, Hong Kong, China
    *Phone: +852-2859-1973. Fax: +852-2559-5337. E-mail: [email protected] (K.S.).
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Cite this: ACS Sustainable Chem. Eng. 2018, 6, 3, 3624–3631
Publication Date (Web):January 16, 2018
https://doi.org/10.1021/acssuschemeng.7b03948
Copyright © 2018 American Chemical Society
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Abstract

Ferrous ions (Fe2+) rapidly activate persulfates to produce sulfate radicals. However, the high reactivity of Fe2+ toward sulfate radicals means that they are easily scavenged, which reduces the stoichiometric efficiency of persulfates. To improve the stoichiometric efficiency, siderite was used to activate peroxydisulfate (PDS) and peroxymonosulfate (PMS), with phenol as a model contaminant. Near-100% degradation of phenol was achieved by siderite-activated PDS or PMS. In contrast, only 34% and 25% of the phenol was degraded by Fe2+- and nanoscale-magnetite-activated persulfates, respectively. The stoichiometric efficiencies of PMS and PDS activated by siderite were more than 4.4 and 3.6 times higher, respectively, than those activated by Fe2+. Electron paramagnetic resonance recorded both sulfate radicals and hydroxyl radicals. The effects of pH, iron dissolution, and scavenging were characterized, and the results indicated that siderite mainly activated persulfates by acting as a source of Fe2+ and that sulfate radicals were the major active species. The release of Fe2+ and the production of sulfate radicals were controllable via the pH of the solution. No deactivation occurred when the siderite was reused, because the acidic environment partially dissolved the surface. These findings may facilitate the application of iron-bearing materials for sulfate radical production.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acssuschemeng.7b03948.

  • Note S1–S4: Chemicals, synthesis of siderite, chemical analysis, and reutilization test of siderite. Figure S1–S3: Zeta potential, X-ray diffraction pattern, and scanning electron micrograph of siderite. Figure S4: Removal of phenol by persulfates or siderite alone. Figure S5: Images of phenol solutions containing PMS at different pH values. Figure S6: Effects of different quenching agents. Figure S7: Accumulation of 2-chlorophenol. Figure S8: Mass spectra of 2-chlorophenol and 4-chlorophenol (PDF)

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