Sulfate Radical Scavenging by Mineral Surfaces in Persulfate-Driven Oxidation Systems: Reaction Rate Constants and Implications

  • Klara Rusevova Crincoli
    Klara Rusevova Crincoli
    National Research Council, Robert S. Kerr Environmental Research Center, 919 Kerr Lab Dr., Ada, Oklahoma 74820, United States
  • Constance Green
    Constance Green
    Department of Biology, East Central University, 1100 E. 14th, Ada, Oklahoma 74820, United States
  • , and 
  • Scott G. Huling*
    Scott G. Huling
    U.S. Environmental Protection Agency, Office of Research and Development, National Risk Management Research Laboratory, Robert S. Kerr Environmental Research Center, 919 Kerr Lab Dr., Ada, Oklahoma 74820, United States
    *E-mail: [email protected]. Phone: (580) 436-8610.
Cite this: Environ. Sci. Technol. 2020, 54, 3, 1955–1962
Publication Date (Web):January 22, 2020
https://doi.org/10.1021/acs.est.9b06442
Copyright © 2020 American Chemical Society
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Abstract

Activated persulfate (PS) is a common method used to generate sulfate radicals (SO4•–), a powerful oxidant capable of degrading a broad array of environmental contaminants. The reaction of SO4•– with nontarget species (i.e., scavenging) contributes significantly to treatment inefficiency. Radical scavenging in this manner has been quantified for nontarget chemical species in the aqueous phase but has never been quantified for solid phase media. Kinetic analysis and laboratory methods were developed to quantify the SO4•– scavenging rate constant (k≡S) for alumina, a naturally occurring mineral in soil and aquifer materials. SO4•– were generated in UV and thermally activated persulfate (UV-APS, T-APS) batch systems, and the loss of rhodamine B (RhB) served as an indicator of SO4•– activity. k≡S for alumina was 2.42 × 104 and 2.03 × 104 m–2 s–1 for UV-APS and T-APS oxidative treatment systems, respectively. At [alumina] >5 g L–1, the reaction of SO4•– with solid phase media increased over the aqueous phase reactions with RhB and aqueous scavengers. SO4•– scavenging by solid surfaces was orders of magnitude greater than the reaction with the target compound and scavengers in the aqueous phase, underscoring the significant role of solid surfaces in scavenging SO4•–.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.9b06442.

  • Molecular forms of rhodamine B (RhB); X-ray diffraction patterns of commercial alumina; summary of control experiments; kinetics of RhB oxidation in alumina-amended UV-APS and T-APS oxidation systems; estimation of second-order rate constant for RhB and SO4•– (k5 in this study); role of the hydroxyl radical in UV- and T-APS reaction systems; results of semicontinuous mode experiments; UV and thermal activation of PS and RhB treatment efficiency analysis; reactions of SO4•– consumption and OH formation and consumption in UV- and T-APS reaction systems; and summary of PSO4•– and kPS for UV- and T-APS treatment systems (PDF)

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This article is cited by 12 publications.

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  8. Daniel T. Oyekunle, Xinquan Zhou, Ajmal Shahzad, Zhuqi Chen. Review on carbonaceous materials as persulfate activators: structure–performance relationship, mechanism and future perspectives on water treatment. Journal of Materials Chemistry A 2021, 9 (13) , 8012-8050. https://doi.org/10.1039/D1TA00033K
  9. Klara Rusevova Crincoli, Scott G. Huling. Contrasting hydrogen peroxide- and persulfate-driven oxidation systems: Impact of radical scavenging on treatment efficiency and cost. Chemical Engineering Journal 2021, 404 , 126404. https://doi.org/10.1016/j.cej.2020.126404
  10. Qingwen Tang, Xiaoqiang An, Jing Zhou, Huachun Lan, Huijuan Liu, Jiuhui Qu. One-step exfoliation of polymeric C3N4 by atmospheric oxygen doping for photocatalytic persulfate activation. Journal of Colloid and Interface Science 2020, 579 , 455-462. https://doi.org/10.1016/j.jcis.2020.06.064
  11. Frank-Dieter Kopinke. Comment to the article “Hydroxyl radical scavenging by solid mineral surfaces in oxidative treatment systems: Rate constants and implications” published by K. Rusevova Crincoli and S. G. Huling in Water Research 169, 2020, 115240. Water Research 2020, 186 , 116308. https://doi.org/10.1016/j.watres.2020.116308
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