Oxidation of Microcystin-LR via Activation of Peroxymonosulfate Using Ascorbic Acid: Kinetic Modeling and Toxicity Assessment

  • Shiqing Zhou
    Shiqing Zhou
    Department of Water Engineering and Science, College of Civil Engineering, Hunan University, Changsha, Hunan 410082, China
    Brook Byer Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Shiqing Zhou
  • Yanghai Yu
    Yanghai Yu
    Department of Water Engineering and Science, College of Civil Engineering, Hunan University, Changsha, Hunan 410082, China
    More by Yanghai Yu
  • Weiqiu Zhang
    Weiqiu Zhang
    Brook Byer Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Weiqiu Zhang
  • Xiaoyang Meng
    Xiaoyang Meng
    Brook Byer Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
  • Jinming Luo
    Jinming Luo
    Brook Byer Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Jinming Luo
  • Lin Deng
    Lin Deng
    Department of Water Engineering and Science, College of Civil Engineering, Hunan University, Changsha, Hunan 410082, China
    Brook Byer Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Lin Deng
  • Zhou Shi
    Zhou Shi
    Department of Water Engineering and Science, College of Civil Engineering, Hunan University, Changsha, Hunan 410082, China
    More by Zhou Shi
  • , and 
  • John Crittenden*
    John Crittenden
    Brook Byer Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    *Phone: 404-894-5676; fax: 404-894-7896; e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2018, 52, 7, 4305–4312
Publication Date (Web):March 7, 2018
https://doi.org/10.1021/acs.est.7b06560
Copyright © 2018 American Chemical Society
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Abstract

Advanced oxidation processes (AOPs) have been widely used for the destruction of organic contaminants in the aqueous phase. In this study, we introduce an AOP on activated peroxymonosulfate (PMS) by using ascorbic acid (H2A) to generate sulfate radicals (SO4•–). Sulfate radicals, hydroxyl radicals (HO), and ascorbyl radicals (A•–) were found using electron spin resonance (ESR). But we found A•– is negligible in the degradation of microcystin-LR (MCLR) due to its low reactivity. We developed a first-principles kinetic model to simulate the MCLR degradation and predict the radical concentrations. The MCLR degradation rate decreased with increasing pH. The scavenging effect of natural organic matter (NOM) on SO4•– was relatively small compared to that for HO. Considering both energy consumption and MCLR removal, the optimal H2A and PMS doses for H2A/PMS process were determined at 1.0 × 10–6 M and 1.6 × 10–5 M, respectively. In addition, we determined the toxicity using the protein phosphatase 2A (PP2A) test and the results showed that MCLR was readily detoxified and its oxidation byproducts were not hepatotoxic. Overall, our work provides a new type of AOP and a promising, efficient, and environmental-friendly method for removing microcystins in algae-laden water.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.7b06560.

  • Supplemental text describing chemicals, ESR procedures for detection of sulfate, hydroxyl and ascorbyl radicals, toxicity assessment of MCLR, modeling approach and rate constants determination, kinetic equations, and energy costs. Tables showing objective function values for kinetic model, and oxidation products of MCLR. Figures showing calibration curve for toxicity assessments, and proposed activated mechanism of PMS by ascorbic acid; model-predicted peroxymonosulfate radical concentrations; intensity profiles of hydroxyl radical, sulfate radical and ascorbyl radical; fractions of H2A, HA and A2– species under different pH values; model-predicted sulfate radical and hydroxyl radical distributions under different NOM concentrations; EE/Ototal (in kWh L–1) of H2A/PMS process vary with H2A and PMS doses; proposed pathways of MC-LR degradation in the H2/PMS process (PDF)

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