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    Activation of peroxymonosulfate by carbonaceous oxygen groups: Experimental and density functional theory calculations

    Access Status
    Fulltext not available
    Authors
    Wang, Y.
    Ao, Z.
    Sun, Hongqi
    Duan, X.
    Wang, Shaobin
    Date
    2016
    Type
    Journal Article
    
    Metadata
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    Citation
    Wang, Y. and Ao, Z. and Sun, H. and Duan, X. and Wang, S. 2016. Activation of peroxymonosulfate by carbonaceous oxygen groups: Experimental and density functional theory calculations. Applied Catalysis B: Environmental. 198: pp. 295-302.
    Source Title
    Applied Catalysis B: Environmental
    DOI
    10.1016/j.apcatb.2016.05.075
    ISSN
    0926-3373
    School
    Department of Chemical Engineering
    Funding and Sponsorship
    http://purl.org/au-research/grants/arc/DP130101319
    URI
    http://hdl.handle.net/20.500.11937/23048
    Collection
    • Curtin Research Publications
    Abstract

    © 2016 Elsevier B.V. The active sites for metal-free carbocatalysis in environmental remediation are intricate compared to those for traditional metal-based catalysis. In this study, we report a facile fabrication of amorphous carbon spheres with varying oxygen functional groups by hydrothermal treatment of glucose solutions. With air/N2 annealing and regeneration in the glucose solution of the as-synthesized carbon spheres, the concentrations of oxygen-containing groups were tailored on the amorphous carbon spheres in an Excess-On-Off-On manner. Accordingly, an Off-On-Off-On catalytic behavior in peroxymonosulfate (PMS) activation using these amorphous carbon spheres was observed. To uncover the mechanism of catalytic activity, electron spin resonance (EPR) spectra were recorded to investigate the variation of the generated OH and SO4-radicals. Moreover, density functional theory (DFT) studies were employed to identify the role of oxygen-containing groups on the amorphous carbon spheres in adsorptive OO bond activation of PMS. Results revealed that ketone groups (CO) are the dominant active sites for PMS activation among oxygen-containing functional groups. In order to simulate real wastewater treatment, influences of chloride anions and humic acid on PMS activation for phenol degradation were further evaluated. This study provides an in-depth insight to discovering the role of oxygen-containing functional groups as the active sites in metal-free carbocatalysis.

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