Identifying the Nonradical Mechanism in the Peroxymonosulfate Activation Process: Singlet Oxygenation Versus Mediated Electron Transfer

  • Eun-Tae Yun
    Eun-Tae Yun
    School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 136-701, Korea
    More by Eun-Tae Yun
  • Jeong Hoon Lee
    Jeong Hoon Lee
    School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 136-701, Korea
  • Jaesung Kim
    Jaesung Kim
    School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 136-701, Korea
    More by Jaesung Kim
  • Hee-Deung Park
    Hee-Deung Park
    School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 136-701, Korea
  • , and 
  • Jaesang Lee*
    Jaesang Lee
    School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 136-701, Korea
    *Phone: +82-2-3290-4864; fax: +82-2-928-7656; e-mail: [email protected] (J.L.).
    More by Jaesang Lee
Cite this: Environ. Sci. Technol. 2018, 52, 12, 7032–7042
Publication Date (Web):May 23, 2018
Copyright © 2018 American Chemical Society
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Select persulfate activation processes were demonstrated to initiate oxidation not reliant on sulfate radicals, although the underlying mechanism has yet to be identified. This study explored singlet oxygenation and mediated electron transfer as plausible nonradical mechanisms for organic degradation by carbon nanotube (CNT)-activated peroxymonosulfate (PMS). The degradation of furfuryl alcohol (FFA) as a singlet oxygen (1O2) indicator and the kinetic retardation of FFA oxidation in the presence of l-histidine and azide as 1O2 quenchers apparently supported a role of 1O2 in the CNT/PMS system. However, the 1O2 scavenging effect was ascribed to a rapid PMS depletion by l-histidine and azide. A comparison of CNT/PMS and photoexcited Rose Bengal (RB) excluded the possibility of singlet oxygenation during heterogeneous persulfate activation. In contrast to the case of excited RB, solvent exchange (H2O to D2O) did not enhance FFA degradation by CNT/PMS and the pH- and substrate-dependent reactivity of CNT/PMS did not reflect the selective nature of 1O2. Alternatively, concomitant PMS reduction and trichlorophenol oxidation were achieved when PMS and trichlorophenol were physically separated in two chambers using a conductive vertically aligned CNT membrane. This result suggested that CNT-mediated electron transfer from organics to persulfate was primarily responsible for the nonradical degradative route.

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This material is available free of charge via the Internet at The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b00959.

  • Description of chemicals used in this study (Text S1), VA-CNT membrane fabrication (Scheme S1), SEM images and Raman spectrum of aligned CNTs (Figures S1 and S2), XPS survey spectrum of VA-CNT membrane (Figure S3), emission spectrum of fluorescent lamp and absorption spectrum of RB (Figure S4), PMS decay by CNTs in H2O and D2O (Figure S5), H2O2 production during ascorbate oxidation by CNT/PMS and photoexcited RB (Figure S6), FFA oxidation by PMS with excess l-histidine (Figure S7), reactivity of azide/PMS toward organics (Figure S8), EPR spectra of azide only, PMS only, and azide/PMS with DMPO as a spin trap (Figure S9), FFA degradation by CNT/PMS and CNT/PDS (Figure S10), effects of l-histidine and D2O on 4-CP oxidation by CNT/PMS and CNT/PDS (Figure S11), direct reduction of PMS and PDS by l-histidine (Figure S12), direct FFA oxidation by PMS and PDS (Figure S13), effect of pH on chlorophenol degradation by CNT/PMS and photoexcited RB (Figure S14), zeta potential of CNTs (Figure S15), EPR spectra of CNT/PMS and photoirradiated RB with DMPO as a spin trap (Figure S16), chloride permeability of VA-CNT membrane (Figure S17), time-dependent changes in PMS concentration with Co2+ and PMS in chambers A and B (Figure S18), concurrent TCP oxidation (chamber A) and PMS reduction (chamber B) without a phosphate buffer (Figure S19), concurrent TCP oxidation (chamber A) and PDS reduction (chamber B) (Figure S20), time-dependent changes in TCP concentration with aqueous TCP and pure water in chambers A and B (Figure S21), and ATR-FTIR and Raman spectra of fresh and used CNTs (Figure S22) (PDF)

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