Rapid oxidation of histamine H2-receptor antagonists by peroxymonosulfate during water treatment: Kinetics, products, and toxicity evaluation
Rapid oxidation of histamine H2-receptor antagonists by peroxymonosulfate during water treatment: Kinetics, products, and toxicity evaluation
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水处理过程中过一硫酸盐对组胺 H2 受体拮抗剂的快速氧化：动力学、产物和毒性评估
DOI：
10.1016/j.watres.2020.116278
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发表时间：
2020-10-15
期刊：
影响因子：
12.8
通讯作者：
Chen, Jiabin
中科院分区：
文献类型：
--
作者：
Qian, Yajie;Huang, Jinjing;Chen, Jiabin
过一硫酸盐（PMS）是一种很有吸引力的氧化剂，用于有机污染物的破坏，依赖于活化后产生自由基。本文首次报道了PMS通过非自由基途径促进组胺H-2受体拮抗剂（HRAs）的快速降解。五种常用的HRA，即，雷尼替丁（RNTD）、西咪替丁（CMTD）、法莫替丁（FMTD）、尼扎替丁（NZTD）和罗沙替丁（RXTD）对PMS的反应性。结果表明，HRA（RXTD除外）对PMS表现出高反应性，在pH 7.0时，表观二级速率常数为403至872 M（-1）s（-1）。自由基清除实验排除了自由基的贡献PMS促进降解的HRA，这种非自由基的过程是不受真实的水基质。构效评价和理论计算表明，HRAs（RXTD除外）中的硫醚硫是PMS氧化的主要活性中心。转化产物分析进一步阐明了硫醚硫通过氧原子转移过程氧化为亚砜产物。此外，直链上的硫醚硫比噻唑环上的硫更容易与PMS进行氧转移。毒性评价结果表明，PMS氧化处理后，HRAs的生态毒性明显降低。因此，这项工作提供了一个很有前途的战略，以快速去除HRA和显着降低其毒性在水处理。(C)2020爱思唯尔有限公司保留所有权利。
Peroxymonosulfate (PMS) is an appealing oxidant for organic contaminant destruction relying on radical generation after activation. Herein, we report PMS-promoted rapid degradation of histamine H-2-receptor antagonists (HRAs) through non-radical process for the first time. Five commonly used HRAs, i.e., ranitidine (RNTD), cimetidine (CMTD), famotidine (FMTD), nizatidine (NZTD) and roxatidine (RXTD), were examined their reactivity towards PMS. Results show that HRAs (except RXTD) exhibit high reactivity towards PMS, with apparent second-order rate constants from 403 to 872 M(-1)s(-1) at pH 7.0. Radical scavenging experiments excluded the contribution of radicals to PMS-promoted degradation of HRAs, and this non-radical process was unaffected by the real water matrices. Structure-activity assessment and theoretical calculation indicated that the thioether sulfur in HRAs (except RXTD) was the main reactive site for PMS oxidation. Transformation product analysis further elucidated oxidation of the thioether sulfur to sulfoxide product through an oxygen atom transfer process. Moreover, the thioether sulfur on the straight chain was more susceptible to oxygen transfer with PMS than that on the thiazole ring of HRAs. Toxicity evaluation indicated the ecotoxicity of HRAs could be remarkably reduced after PMS oxidation. Hence, this work provides a promising strategy to rapidly remove HRAs and significantly reduce their toxicity in water treatment. (C) 2020 Elsevier Ltd. All rights reserved.