Activation of Peroxydisulfate on Carbon Nanotubes: Electron-Transfer Mechanism

  • Wei Ren
    Wei Ren
    Department of Environmental Science and Engineering, Hubei Environmental Remediation Material Engineering Technology Research Center, Wuhan University, Wuhan 430079, P. R. China
    School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia
    More by Wei Ren
  • Liangliang Xiong
    Liangliang Xiong
    Department of Environmental Science and Engineering, Hubei Environmental Remediation Material Engineering Technology Research Center, Wuhan University, Wuhan 430079, P. R. China
  • Xuehong Yuan
    Xuehong Yuan
    Department of Environmental Science and Engineering, Hubei Environmental Remediation Material Engineering Technology Research Center, Wuhan University, Wuhan 430079, P. R. China
    More by Xuehong Yuan
  • Ziwei Yu
    Ziwei Yu
    Department of Environmental Science and Engineering, Hubei Environmental Remediation Material Engineering Technology Research Center, Wuhan University, Wuhan 430079, P. R. China
    More by Ziwei Yu
  • Hui Zhang*
    Hui Zhang
    Department of Environmental Science and Engineering, Hubei Environmental Remediation Material Engineering Technology Research Center, Wuhan University, Wuhan 430079, P. R. China
    *E-mail: [email protected] (H.Z.).
    More by Hui Zhang
  • Xiaoguang Duan*
    Xiaoguang Duan
    School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia
    *E-mail: [email protected] (X.D.).
  • , and 
  • Shaobin Wang
    Shaobin Wang
    School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia
    More by Shaobin Wang
Cite this: Environ. Sci. Technol. 2019, 53, 24, 14595–14603
Publication Date (Web):November 13, 2019
https://doi.org/10.1021/acs.est.9b05475
Copyright © 2019 American Chemical Society
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Abstract

This study proposed an electrochemical technique for investigating the mechanism of nonradical oxidation of organics with peroxydisulfate (PDS) activated by carbon nanotubes (CNT). The electrochemical property of twelve phenolic compounds (PCs) was evaluated by their half-wave potentials, which were then correlated to their kinetic rate constants in the PDS/CNT system. Integrated with quantitative structure–activity relationships (QSARs), electron paramagnetic resonance (EPR), and radical scavenging tests, the nature of nonradical pathways of phenolic compound oxidation was unveiled to be an electron-transfer regime other than a singlet oxygenation process. The QSARs were established according to their standard electrode potentials, activation energy, and pre-exponential factor. A facile electrochemical analysis method (chronopotentiometry combined with chronoamperometry) was also employed to probe the mechanism, suggesting that PDS was catalyzed initially by CNT to form a CNT surface-confined and -activated PDS (CNT–PDS*) complex with a high redox potential. Then, the CNT–PDS* complex selectively abstracted electrons from the co-adsorbed PCs to initiate the oxidation. Finally, a comparison of PDS/CNT and graphite anodic oxidation under constant potentials was comprehensively analyzed to unveil the relative activity of the nonradical CNT–PDS* complex toward the oxidation of different PCs, which was found to be dependent on the oxidative potentials of the CNT–PDS* complex and the adsorbed organics.

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  • Electrochemical analysis; approach for anodic oxidation of PCs; evaluation of electrochemical property of PE; theoretical calculation of Nernst formula; physiochemical properties, analytical method, and degradation kinetics of 12 PCs; activation energies of carbon materials; CV, LSV, and chronopotentiometry curves; impacts of solution pH and reaction temperature; zeta potentials of CNT; EPR spectra (PDF)

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