Oxidation of Organic Compounds in Water by Unactivated Peroxymonosulfate

  • Yi Yang
    Yi Yang
    Department of Environmental Sciences, The Connecticut Agricultural Experiment Station, 123 Huntington Street, P.O. Box 1106, New Haven, Connecticut 06504, United States
    More by Yi Yang
  • Gourab Banerjee
    Gourab Banerjee
    Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States
  • Gary W. Brudvig
    Gary W. Brudvig
    Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States
  • Jae-Hong Kim
    Jae-Hong Kim
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520, United States
    More by Jae-Hong Kim
  • , and 
  • Joseph J. Pignatello*
    Joseph J. Pignatello
    Department of Environmental Sciences, The Connecticut Agricultural Experiment Station, 123 Huntington Street, P.O. Box 1106, New Haven, Connecticut 06504, United States
    *E-mail: [email protected]. Phone: (1)-203-974-8518.
Cite this: Environ. Sci. Technol. 2018, 52, 10, 5911–5919
Publication Date (Web):April 17, 2018
https://doi.org/10.1021/acs.est.8b00735
Copyright © 2018 American Chemical Society
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Abstract

Peroxymonosulfate (HSO5 and PMS) is an optional bulk oxidant in advanced oxidation processes (AOPs) for treating wastewaters. Normally, PMS is activated by the input of energy or reducing agent to generate sulfate or hydroxyl radicals or both. This study shows that PMS without explicit activation undergoes direct reaction with a variety of compounds, including antibiotics, pharmaceuticals, phenolics, and commonly used singlet-oxygen (1O2) traps and quenchers, specifically furfuryl alcohol (FFA), azide, and histidine. Reaction time frames varied from minutes to a few hours at pH 9. With the use of a test compound with intermediate reactivity (FFA), electron paramagnetic resonance (EPR) and scavenging experiments ruled out sulfate and hydroxyl radicals. Although 1O2 was detected by EPR and is produced stoichiometrically through PMS self-decomposition, 1O2 plays only a minor role due to its efficient quenching by water, as confirmed by experiments manipulating the 1O2 formation rate (addition of H2O2) or lifetime (deuterium solvent isotope effect). Direct reactions with PMS are highly pH- and ionic-strength-sensitive and can be accelerated by (bi)carbonate, borate, and pyrophosphate (although not phosphate) via non-radical pathways. The findings indicate that direct reaction with PMS may steer degradation pathways and must be considered in AOPs and other applications. They also signal caution to researchers when choosing buffers as well as 1O2 traps and quenchers.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b00735.

  • Additional details on materials and methods, trace metals, determination of 1O2 formation, organic compounds analysis, EPR measurements, determination of pKa,2, and influence on PMS self-decomposition. Tables showing HPLC parameters and published rate constants. Figures showing the effect of Fe(III) concentration, the degradation of FFA, linear relationships, PMS decomposition, loss of FFA and PMS, the effect of pH, kinetics of PMS self-decomposition, absorbances, reactions with added hydrogen peroxide, the effect of scavengers, and the EPR spectra. (PDF)

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