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Oxidative degradation of iodinated X-ray contrast media (iomeprol and iohexol) with sulfate radical: An experimental and theoretical study

文献类型： 外文期刊

作者： Wang, Xiaoxiao 1 ; Wang, Zhaohui 1 ; Tang, Yizhen 4 ; Xiao, Dongxue 5 ; Zhang, Dong 5 ; Huan, Ying 1 ; Guo, Yaoguang 6 ;

作者机构： 1.Donghua Univ, State Environm Protect Engn Ctr Pollut Treatment, Coll Environm Sci & Engn, Shanghai 201620, Peoples R China

2.East China Normal Univ, Sch Ecol & Environm Sci, Shanghai Key Lab Urbanisat & Ecol Restorat, Shanghai 200241, Peoples R China

3.IEC, Shanghai 200062, Peoples R China

4.Qingdao Univ Technol, Sch Environm & Municipal Engn, Fushun Rd 11, Qingdao 266033, Shandong, Peoples R China

5.Chinese Acad Fishery Sci, East China Sea Fisheries Res Inst, Shanghai 200090, Peoples R China

6.Shanghai Polytech Univ, Sch Environm & Mat Engn, Shanghai 201209, Peoples R China

7.Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China

关键词： Sulfate radical; Iodinated X-ray contrast media; Iodinated by-products; Degradation pathways; Theoretical calculations

期刊名称：CHEMICAL ENGINEERING JOURNAL （ 影响因子：13.273； 五年影响因子：11.529 ）

ISSN： 1385-8947

年卷期： 2019 年 368 卷

页码：

收录情况： SCI

摘要： It has already been known that oxidative degradation of organochlorine (e. g. chlorophenols) is accompanied by de novo formation of new polychlorinated compounds, however, whether the similar scenario can happen during decomposition of iodine-containing pollutants is completely unknown. Here degradation of two iodinated X-ray contrast media (ICM), iomeprol and iohexol, by sulfate radical generated through Co(II)-mediated activation of peroxymonosulfate (PMS) was investigated. The influencing parameters, such as the initial concentrations of PMS and Co(II), the initial solution pH and natural water constituents were examined. The pseudofirst-order rate constant of iomeprol in the PMS/Co(II) system is more than twice of iohexol, with values of 7.7x10(-2) and 3.5x10(-2) min(-1), respectively, indicating that iomeprol seems more susceptible to radicals attack than iohexol. The bimolecular rate constants for reaction of sulfate radical (SO4 center dot-) with ICM were determined to be 1.8x10(10) M-1 s(-1) and 7.9 x10(9) M-1 s(-1) for iomeprol and iohexol, respectively. The low degrees of mineralization and identification of iodinated intermediates of iomeprol and iohexol indicate that the degradation of iomeprol and iohexol in the Co/PMS system were incomplete. A de novo formation of new polyiodinated compounds would not happen because most of released inorganic iodine were ultimately oxidized to iodate (IO3-), rather than the reactive iodinated agents. Based on the identified byproducts and quantum chemical calculation, eight main transformation pathways are proposed for the degradation of iomeprol and iohexol as follows: (a) deiodination; (b) hydrogen abstraction; (c) amide hydrolysis; (d) amino oxidation; (e) hydroxyl substituent; (f) transformed alkyl aromatic amides to aromatic carbamoyl; (g) dehydration; (h) oxidized primary alcohol groups to carboxyl groups.

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