Identifying the Nonradical Mechanism in the Peroxymonosulfate Activation Process: Singlet Oxygenation Versus Mediated Electron Transfer
Abstract
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 ( 1 O 2 ) indicator and the kinetic retardation of FFA oxidation in the presence of l -histidine and azide as 1 O 2 quenchers apparently supported a role of 1 O 2 in the CNT/PMS system. However, the 1 O 2 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 (H 2 O to D 2 O) 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 1 O 2 . 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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Reactive species generated in CO2 activation are mild and sustainable, such as singlet oxygen, with greater selectivity to electron-rich organics and less surface oxidation on carbon matrices compared to conventional radical species.
“Intriguingly, the reactive species generated in this process were mild and sustainable species such as singlet oxygen ( 1 O2) with greater selectivity to electron-rich organics and less surface oxidation on carbon matrices as compared to the conventional radical species (i.e., • OH, SO4 •-, and • O2 -). 25”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [25]
Well-ordered carbon matrices possess distinct electronic properties that allow them to serve as efficient electron shuttles, deliver charges among aromatic units, and prompt inherent catalytic redox reactions on carbonaceous material surfaces.
“Lately, well-ordered carbon matrices are found to pose distinct electronic properties to serve as efficient electron shuttles, deliver charges among aromatic units, and prompt inherent catalytic redox reactions on the surface of carbonaceous materials.25,167”
From Sustainable remediation with an electroactive biochar system: mechanisms and perspectives (2020) · cites this paper as [25]
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- Authors
- Yun, E.-T., Lee, J. H., Kim, J., Park, H.-D., & Lee, J.
- Affiliations
- Korea University (KR)
- School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 136-701, Korea
- Corresponding author
- Lee, Jaesang
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-05-23
- Volume
- 52
- Issue
- 12
- Pages
- 7032-7042
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W2804308463
- Cited by
- 1,175
- References
- 56
- Citations by year
- 2026: 97 · 2025: 185 · 2024: 163 · 2023: 197 · 2022: 216 · 2021: 142 · 2020: 96 · 2019: 68 · 2018: 11
- FWCI
- 34.67
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Environmental Science & Technology (publishedVersion)
- PubMed (publishedVersion)
- Funders
- National Research Foundation of Korea (2016M3A7B4909318, 2017R1A2B4002235)
- Topics
- Physical Sciences › Environmental Science › Water Science and Technology › Advanced oxidation water treatment
- Physical Sciences › Engineering › Biomedical Engineering › Environmental remediation with nanomaterials
- Physical Sciences › Environmental Science › Environmental Chemistry › Per- and polyfluoroalkyl substances research
- Keywords
- peroxymonosulfate activation, non-radical oxidation, singlet oxygen, mediated electron transfer, carbon nanotubes, histidine, azide, rose bengal, heterogeneous catalysis
- MeSH terms
- Electron Transport, Electrons, Oxidation-Reduction, Peroxides
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