Ultrasensitive Fluorescence Detection of Peroxymonosulfate Based on a Sulfate Radical-Mediated Aromatic Hydroxylation

  • Gui-Xiang Huang
    Gui-Xiang Huang
    CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei 230026, China
  • Jin-Yan Si
    Jin-Yan Si
    CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei 230026, China
    More by Jin-Yan Si
  • Chen Qian
    Chen Qian
    CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei 230026, China
    More by Chen Qian
  • Wei-Kang Wang
    Wei-Kang Wang
    CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei 230026, China
  • Shu-Chuan Mei
    Shu-Chuan Mei
    CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei 230026, China
  • Chu-Ya Wang
    Chu-Ya Wang
    CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei 230026, China
    More by Chu-Ya Wang
  • , and 
  • Han-Qing Yu*
    Han-Qing Yu
    CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei 230026, China
    *Fax: +86 551 63601592. E-mail: [email protected]
    More by Han-Qing Yu
Cite this: Anal. Chem. 2018, 90, 24, 14439–14446
Publication Date (Web):November 19, 2018
https://doi.org/10.1021/acs.analchem.8b04047
Copyright © 2018 American Chemical Society
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Abstract

Recently, peroxymonosulfate (PMS)-based advanced oxidation processes have exhibited broad application prospects in the environment field. Accordingly, a simple, rapid, and ultrasensitive method is highly desired for the specific recognition and accurate quantification of PMS in various aqueous solutions. In this work, SO4•–-induced aromatic hydroxylation was explored, and based on that, for the first time, a novel fluorescence method was developed for the PMS determination using Co2+ as a PMS activator and benzoic acid (BA) as a chemical probe. Through a suite of spectral, chromatographic, and mass spectrometric analyses, SO4•– was proven to be the dominant radical species, and salicylic acid was identified as the fluorescent molecule. As a result, a whole radical chain reaction mechanism for the generation of salicylic acid in the BA/PMS/Co2+ system was proposed. This fluorescence method possessed a rapid reaction equilibrium (<1 min), an ultrahigh sensitivity (detection limit = 10 nM; quantification limit = 33 nM), an excellent specificity, and a wide detection range (0–100 μM). Moreover, it performed well in the presence of possible interfering substances, including two other peroxides (i.e., peroxydisulfate and hydrogen peroxide), some common ions, and organics. The detection results for real water samples further validated the practical utility of the developed fluorescence method. This work provides a new method for the specific recognition and sensitive determination of PMS in complex aqueous solutions.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.analchem.8b04047.

  • Tables showing linear range and detection limit comparison, tested cation and anion concentrations, and conversion factors; figures showing EEMS results, GC-MS chromatogram, MS spectra, EPR spectra, impact of atmosphere conditions on fluorescence intensity, fluorescence emission spectra, relationship between fluorescence intensity and PMS concentration and corresponding calibration curve, effect of solution pH, change of solution pH, calibration curves of PMS, and reaction temperature impacts (PDF)

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