Insights into the Electron-Transfer Regime of Peroxydisulfate Activation on Carbon Nanotubes: The Role of Oxygen Functional Groups

  • Wei Ren
    Wei Ren
    Department of Environmental Science and Engineering, Wuhan University, Wuhan 430079, China
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide SA5005, Australia
    More by Wei Ren
  • Liangliang Xiong
    Liangliang Xiong
    Department of Environmental Science and Engineering, Wuhan University, Wuhan 430079, China
  • Gang Nie
    Gang Nie
    Department of Environmental Science and Engineering, Wuhan University, Wuhan 430079, China
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide SA5005, Australia
    More by Gang Nie
  • Hui Zhang*
    Hui Zhang
    Department of Environmental Science and Engineering, Wuhan University, Wuhan 430079, China
    *E-mail: [email protected] (H.Z.).
    More by Hui Zhang
  • Xiaoguang Duan*
    Xiaoguang Duan
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide SA5005, Australia
    *E-mail: [email protected] (X.D.).
  • , and 
  • Shaobin Wang
    Shaobin Wang
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide SA5005, Australia
    More by Shaobin Wang
Cite this: Environ. Sci. Technol. 2020, 54, 2, 1267–1275
Publication Date (Web):December 17, 2019
Copyright © 2019 American Chemical Society
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Carbon-driven advanced oxidation processes are appealing in wastewater purification because of the metal-free feature of the carbocatalysts. However, the regime of the emerging nonradical pathway is ambiguous because of the intricate carbon structure. To this end, this study was dedicated to unveil the intrinsic structure-performance relationship of peroxydisulfate (PDS) activation by carbon nanotubes (CNTs) toward nonradical oxidation of organics such as phenol (PE) via electron transfer. Eighteen analogical CNTs were synthesized and functionalized with different categories and contents of oxygen species. The quenching tests and chronopotentiometry suggest that an improved reactivity of surface-regulated CNTs was attributed to the reinforced electron-transfer regime without generation of free radicals and singlet oxygen. The quantitative structure–activity relationships were established and correlated to the Tafel equation, which unveils the nature of the nonradical oxidation by CNT-activated PDS complexes (CNT-PDS*). First, a decline in the concentration of oxygen groups in CNTs will make the zeta potential of the CNT become less negative in neutral solutions, which facilitated the adsorption of PDS because of weaker electrostatic repulsion. Then, the metastable CNT-PDS* was formed, which elevated the oxidation capacity of the CNT. Finally, PE would be oxidized over CNT-PDS* via electron transfer to fulfill the redox cycle. Moreover, the nonradical oxidation rate was uncovered to be exponentially related with the potential of the complexes, suggesting that the nonradical oxidation by the CNT-PDS* undergoes a mechanism analogous to anodic oxidation.

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  • The details of electrochemical analysis, Approach for optimization of scavengers, Theoretical derivation of electrochemical equations, Physicochemical properties and zeta potential of eighteen CNTs, PDS adsorption, potential of complexes and kinetic constants of degradation of eighteen CNTs in the PDS/CNT system, Degradation kinetics curves of graphite in the anodic oxidation system, TGA, Raman spectra, XPS spectra, EPR spectra, and LSV curves (PDF)

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