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Chloride-Mediated Enhancement in Heat-Induced Activation of Peroxymonosulfate: New Reaction Pathways for Oxidizing Radical Production

Authors
Ahn, Yong-YoonChoi, JaeminKim, MinjeongKim, Min SikLee, DonghyunBang, Woo HyuckYun, Eun-TaeLee, HongshinLee, Jung-HyunLee, ChanghaMaeng, Sung KyuHong, SeungkwanLee, Jaesang
Issue Date
20-4월-2021
Publisher
AMER CHEMICAL SOC
Citation
ENVIRONMENTAL SCIENCE & TECHNOLOGY, v.55, no.8, pp.5382 - 5392
Indexed
SCIE
SCOPUS
Journal Title
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume
55
Number
8
Start Page
5382
End Page
5392
URI
https://scholar.korea.ac.kr/handle/2021.sw.korea/128218
DOI
10.1021/acs.est.0c07964
ISSN
0013-936X
Abstract
This study is the first to demonstrate the capability of Cl- to markedly accelerate organic oxidation using thermally activated peroxymonosulfate (PMS) under acidic conditions. The treatment efficiency gain allowed heat-activated PMS to surpass heat-activated peroxydisulfate (PDS). During thermal PMS activation at excess Cl-, accelerated oxidation of 4-chlorophenol (susceptible to oxidation by hypochlorous acid (HOCl)) was observed along with significant degradation of benzoic acid and ClO3- occurrence, which involved oxidants with low substrate specificity. This indicated that heat facilitated HOCl formation via nucleophilic Cl- addition to PMS and enabled free chlorine conversion into less selective oxidizing radicals. HOCl acted as a key intermediate in the major oxidant transition based on temperature-dependent variation in HOCl concentration profiles, kinetically retarded organic oxidation upon NH4+ addition, and enabled rapid organic oxidation in heated PMS/HOCl mixtures. Chlorine atom that formed via the one-electron oxidation of Cl- by the sulfate radical served as the primary oxidant and was involved in hydroxyl radical production. This was corroborated by the quenching effects of alcohols and bicarbonates, reactivity toward multiple organics, and electron paramagnetic resonance spectral features. PMS outperformed PDS in degrading benzoic acid during thermal activation operated in reverse osmosis concentrate, which was in conflict with the well-established superiority of heat-activated PDS.
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Lee, Jae sang
공과대학 (건축사회환경공학부)
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