Coexposure Degradation of Purine Derivatives in the Sulfate Radical-Mediated Oxidation Process

  • Shuangshuang Cheng
    Shuangshuang Cheng
    School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou 510275, China
  • Yu Lei
    Yu Lei
    School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou 510275, China
    More by Yu Lei
  • Xin Lei
    Xin Lei
    School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou 510275, China
    More by Xin Lei
  • Yanheng Pan
    Yanheng Pan
    School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou 510275, China
    More by Yanheng Pan
  • Yunho Lee
    Yunho Lee
    School of Earth Sciences and Environmental Engineering, Gwangju Institute of Science and Technology (GIST), Gwangju 61005, Republic of Korea
    More by Yunho Lee
  • , and 
  • Xin Yang*
    Xin Yang
    School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou 510275, China
    *E-mail: [email protected]. Phone: +86-2039332690.
    More by Xin Yang
Cite this: Environ. Sci. Technol. 2020, 54, 2, 1186–1195
Publication Date (Web):December 22, 2019
https://doi.org/10.1021/acs.est.9b04974
Copyright © 2019 American Chemical Society
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Abstract

Purines are the most widely occurring heterocyclic-N compounds. The degradation behaviors of purine derivatives, theophylline (TPL) and adenine (ADN) as representatives, in both single-component and mixture systems during UV/peroxydisulfate (PDS) treatment were explored. In the mixture system when the concentrations of SO4•– and HO were reduced by more than half in comparison to a single-component system, the observed first-order rate constant of TPL was reduced by 11%, whereas ADN degradation was almost completely inhibited. An ADN “revert” pathway, that is, back transformation of ADN(−H) to ADN by TPL via single electron-transfer reactions, was found. The second-order rate constant of ADN(−H) with TPL was determined to be (1.94 ± 0.21) × 108 M–1 s–1. A kinetic model was developed, which successfully quantifies the contribution of each reaction pathway at various target compound concentrations. In the copresence of 0.1 μM TPL, 58% ADN (3.0 μM) was reduced back to ADN at the PDS dose of 290 μM. The ADN revert pathway’s effectiveness is governed by the relative reduction potentials of the reactants. Purines and phenols with lower reduction potentials are able to react via the ADN revert pathway. These findings improve the understanding of the removal of mixture pollutants from real water media in advanced oxidation processes.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.9b04974.

  • Additional descriptions of determination of reaction rate constants of SO4•–, second-order rate constants of TPL and ADN(−H), total antioxidant capacity (TAC) methods, structures and properties of selected target compounds, modeled steady-state concentrations, model parameters, properties of the surface water, degradation kinetics of target compounds, kinetic traces of SO4•– and ADN(−H), and predicted degradation rate constant (PDF)

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This article is cited by 8 publications.

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