期刊
WATER RESEARCH
卷 138, 期 -, 页码 56-66出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.watres.2018.03.045
关键词
Peroxymonosulfate; Steroid estrogens; In situ chemical oxidation; Bromide ion; Chloride ion
资金
- National Key Research and Development Program [2016YFC0401107]
- National Natural Science Foundation of China [51578203]
- State Key Laboratory of Urban Water Resource and Environment (HIT) [2016DX13]
Recently, in situ chemical oxidation (ISCO) using peroxymonosulfate (PMS) for environmental decontamination has received increasing interest. In this study, oxidation kinetics and products of four steroid estrogens (i.e., estrone, 17 beta-estradiol, estriol, and 17 alpha-ethinylestradiol) by PMS under various conditions were investigated. PMS could fairly degrade steroid estrogens over the pH range of 7-10, and the degradation rate increased with the increase of solution pH. This pH-dependence was well described by parallel reactions between individual acid-base species of steroid estrogens (E and E-) and PMS (HSO5- and SO52-), where specific second-order rate constants for E- with HSO5- and SO52- were in the range of 2.11-5.58 M(-1)s(-1) and 0.77-1.25 M(-1)s(-1), respectively. Identification of oxidation products by liquid chromatography/electrospray ionization quadrupole time-of-flight mass spectrometer showed that PMS readily oxidized the phenolic group of steroid estrogens, leading to the generation of hydroxylated and ring-opening products. The presence of bromide and chloride ions (Br- and Cl-) at environmentally relevant levels could greatly accelerate the degradation of steroid estrogens by PMS with the formation of halogenated aromatic products. This effect was quantitatively estimated by a kinetic model, where the formation of free bromine and chorine and their rapid electrophilic substitution with steroid estrogens were taken into consideration. Eco-toxicity of transformation products of 17 alpha-ethinylestradiol by PMS treatment in the absence and presence of bromide and chloride was estimated by quantitative structure -activity relationship analysis using ECOSAR. These findings advance the understanding of ISCO using PMS. (C) 2018 Elsevier Ltd. All rights reserved.
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