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Activation of Peroxymonosulfate by Benzoquinone: A Novel Nonradical Oxidation Process.
Environ Sci Technol. 2015 Nov 03; 49(21):12941-50.ES

Abstract

The reactions between peroxymonosulfate (PMS) and quinones were investigated for the first time in this work, where benzoquinone (BQ) was selected as a model quinone. It was demonstrated that BQ could efficiently activate PMS for the degradation of sulfamethoxazole (SMX; a frequently detected antibiotic in the environments), and the degradation rate increased with solution pH from 7 to 10. Interestingly, quenching studies suggested that neither hydroxyl radical (•OH) nor sulfate radical (SO4•-) was produced therein. Instead, the generation of singlet oxygen (1O2) was proved by using two chemical probes (i.e., 2,2,6,6-tetramethyl-4-piperidinol and 9,10-diphenylanthracene) with the appearance of 1O2 indicative products detected by electron paramagnetic resonance spectrometry and liquid chromatography mass spectrometry, respectively. A catalytic mechanism was proposed involving the formation of a dioxirane intermediate between PMS and BQ and the subsequent decomposition of this intermediate into 1O2. Accordingly, a kinetic model was developed, and it well described the experimental observation that the pH-dependent decomposition rate of PMS was first-order with respect to BQ. These findings have important implications for the development of novel nonradical oxidation processes based on PMS, because 1O2 as a moderately reactive electrophile may suffer less interference from background organic matters compared with nonselective •OH and SO4•-.

Authors+Show Affiliations

State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology , Harbin, Heilongjiang 150090, China.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology , Harbin, Heilongjiang 150090, China.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology , Harbin, Heilongjiang 150090, China.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology , Harbin, Heilongjiang 150090, China.Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province, College of Chemical and Environmental Engineering, Harbin University of Science and Technology , Harbin, Heilongjiang 150040, China.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology , Harbin, Heilongjiang 150090, China.Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province, College of Chemical and Environmental Engineering, Harbin University of Science and Technology , Harbin, Heilongjiang 150040, China.Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province, College of Chemical and Environmental Engineering, Harbin University of Science and Technology , Harbin, Heilongjiang 150040, China.

Pub Type(s)

Journal Article
Research Support, Non-U.S. Gov't

Language

eng

PubMed ID

26452059

Citation

Zhou, Yang, et al. "Activation of Peroxymonosulfate By Benzoquinone: a Novel Nonradical Oxidation Process." Environmental Science & Technology, vol. 49, no. 21, 2015, pp. 12941-50.
Zhou Y, Jiang J, Gao Y, et al. Activation of Peroxymonosulfate by Benzoquinone: A Novel Nonradical Oxidation Process. Environ Sci Technol. 2015;49(21):12941-50.
Zhou, Y., Jiang, J., Gao, Y., Ma, J., Pang, S. Y., Li, J., Lu, X. T., & Yuan, L. P. (2015). Activation of Peroxymonosulfate by Benzoquinone: A Novel Nonradical Oxidation Process. Environmental Science & Technology, 49(21), 12941-50. https://doi.org/10.1021/acs.est.5b03595
Zhou Y, et al. Activation of Peroxymonosulfate By Benzoquinone: a Novel Nonradical Oxidation Process. Environ Sci Technol. 2015 Nov 3;49(21):12941-50. PubMed PMID: 26452059.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Activation of Peroxymonosulfate by Benzoquinone: A Novel Nonradical Oxidation Process. AU - Zhou,Yang, AU - Jiang,Jin, AU - Gao,Yuan, AU - Ma,Jun, AU - Pang,Su-Yan, AU - Li,Juan, AU - Lu,Xue-Ting, AU - Yuan,Li-Peng, Y1 - 2015/10/23/ PY - 2015/10/10/entrez PY - 2015/10/10/pubmed PY - 2016/6/11/medline SP - 12941 EP - 50 JF - Environmental science & technology JO - Environ. Sci. Technol. VL - 49 IS - 21 N2 - The reactions between peroxymonosulfate (PMS) and quinones were investigated for the first time in this work, where benzoquinone (BQ) was selected as a model quinone. It was demonstrated that BQ could efficiently activate PMS for the degradation of sulfamethoxazole (SMX; a frequently detected antibiotic in the environments), and the degradation rate increased with solution pH from 7 to 10. Interestingly, quenching studies suggested that neither hydroxyl radical (•OH) nor sulfate radical (SO4•-) was produced therein. Instead, the generation of singlet oxygen (1O2) was proved by using two chemical probes (i.e., 2,2,6,6-tetramethyl-4-piperidinol and 9,10-diphenylanthracene) with the appearance of 1O2 indicative products detected by electron paramagnetic resonance spectrometry and liquid chromatography mass spectrometry, respectively. A catalytic mechanism was proposed involving the formation of a dioxirane intermediate between PMS and BQ and the subsequent decomposition of this intermediate into 1O2. Accordingly, a kinetic model was developed, and it well described the experimental observation that the pH-dependent decomposition rate of PMS was first-order with respect to BQ. These findings have important implications for the development of novel nonradical oxidation processes based on PMS, because 1O2 as a moderately reactive electrophile may suffer less interference from background organic matters compared with nonselective •OH and SO4•-. SN - 1520-5851 UR - https://www.unboundmedicine.com/medline/citation/26452059/Activation_of_Peroxymonosulfate_by_Benzoquinone:_A_Novel_Nonradical_Oxidation_Process_ L2 - https://dx.doi.org/10.1021/acs.est.5b03595 DB - PRIME DP - Unbound Medicine ER -