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Peracetic Acid–Ruthenium(III) Oxidation Process for the Degradation of Micropollutants in Water

  • Ruobai Li
    Ruobai Li
    Program for the Environment and Sustainability, Department of Environmental and Occupational Health, School of Public Health, Texas A&M University, 212 Adriance Lab Road, College Station, Texas 77844, United States
    More by Ruobai Li
  • Kyriakos Manoli
    Kyriakos Manoli
    Program for the Environment and Sustainability, Department of Environmental and Occupational Health, School of Public Health, Texas A&M University, 212 Adriance Lab Road, College Station, Texas 77844, United States
  • Juhee Kim
    Juhee Kim
    School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Juhee Kim
  • Mingbao Feng
    Mingbao Feng
    Program for the Environment and Sustainability, Department of Environmental and Occupational Health, School of Public Health, Texas A&M University, 212 Adriance Lab Road, College Station, Texas 77844, United States
    More by Mingbao Feng
  • Ching-Hua Huang*
    Ching-Hua Huang
    School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    *Email: [email protected]
  • , and 
  • Virender K. Sharma*
    Virender K. Sharma
    Program for the Environment and Sustainability, Department of Environmental and Occupational Health, School of Public Health, Texas A&M University, 212 Adriance Lab Road, College Station, Texas 77844, United States
    *Email: [email protected]
Cite this: Environ. Sci. Technol. 2021, 55, 13, 9150–9160
Publication Date (Web):June 15, 2021
https://doi.org/10.1021/acs.est.0c06676
Copyright © 2021 American Chemical Society
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Abstract

This paper presents an advanced oxidation process (AOP) of peracetic acid (PAA) and ruthenium(III) (Ru(III)) to oxidize micropollutants in water. Studies of PAA–Ru(III) oxidation of sulfamethoxazole (SMX), a sulfonamide antibiotic, in 0.5–20.0 mM phosphate solution at different pH values (5.0–9.0) showed an optimum pH of 7.0 with a complete transformation of SMX in 2.0 min. At pH 7.0, other metal ions (i.e., Fe(II), Fe(III), Mn(II), Mn(III), Co(II), Cu(II), and Ni(II)) in 10 mM phosphate could activate PAA to oxidize SMX only up to 20%. The PAA–Ru(III) oxidation process was also unaffected by the presence of chloride and carbonate ions in solution. Electron paramagnetic resonance (EPR) measurements and quenching experiments showed the dominant involvement of the acetyl(per)oxyl radicals (i.e., CH3C(O)O and CH3C(O)OO) for degrading SMX in the PAA–Ru(III) oxidation process. The transformation pathways of SMX by PAA–Ru(III) were proposed based on the identified intermediates. Tests with other pharmaceuticals demonstrated that the PAA–Ru(III) oxidation system could remove efficiently a wide range of pharmaceuticals (9 compounds) in the presence of phosphate ions in 2.0 min at neutral pH. The knowledge gained herein on the effective role of Ru(III) to activate PAA to oxidize micropollutants may aid in developing Ru(III)-containing catalysts for PAA-based AOPs.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c06676.

  • Texts S1–S4 give the chemicals used in the study, method to collect spectra using a stopped-flow spectrophotometer, analytical approaches to determine concentrations of pharmaceuticals, and EPR experimental procedures. Figure S1 is the oxidation of SMX by metal ions alone, Figures S2 is the PAA decay by Ru(III), Figure S3 shows the effect of N2 purging on the oxidation of SMX, and Figures S4 and S5 are the UV–vis spectra in the PAA–Ru(III) mixed solution. Figure S6 shows the oxidation of SMX under different conditions (i.e., HCO3 alone, Cl alone, PAA–HCO3, PAA–Cl, Ru(III)–HCO3, or Ru(III)–Cl), Figure S7 (A–F) is the LC-HR/MS measured product ion spectra of SMX and its Ops, and Figure S8 shows oxidation of various organic micropollutants by the PAA–Ru(III) process. Tables S1–S4 are the conditions used in analyzing pharmaceuticals by the LC-HR/MS method, accurate mass measurements of SMX and its OPs, the structures of the tested pharmaceuticals, and the extracted spin adduct parameters for radicals detected from EPR analysis (PDF)

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