Hunan Engineering Research Center of Water Security Technology and Application, College of Civil Engineering, Hunan University, Changsha 410082, China; Key Laboratory of Building Safety and Energy Efficiency, Ministry of Education, Hunan University, Changsha 410082, China.
State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092, China.
Sci Total Environ. 2022 Sep 10;838(Pt 1):155894. doi: 10.1016/j.scitotenv.2022.155894. Epub 2022 May 13.
Organic chloramines posed significant risks to drinking water safety. However, the formation mechanism of algae-derived organic chloramines remained unclear. In this study, it was observed that pre-oxidation of algal suspensions increased organic chloramine formation during chlorination. Compared to KMnO pre-oxidation, O significantly increased the organic chloramine formation potential of algal suspensions. Characterization was performed with size exclusion chromatography-multiple detectors (SEC-MDs) to better understand the organic chloramine formation mechanism. The results revealed that low molecular weight proteins (AMW ≤ 0.64 kDa) were the main precursors of organic chloramines after conventional water treatment processes. We then focused on 14 essential amino acids involved in protein formation. Their concentrations and organic chloramine formation potentials were determined, based on which the theoretical organic chloramine formation potentials of the studied samples were evaluated. However, dramatic gaps between theoretical and experimental organic chloramine formations were observed, which suggested that not all organic nitrogen could react with chlorine to form organic chloramine. The condensed dual descriptor (CDD) was calculated to predict the electrophilic substitution reaction sites on peptides. Furthermore, the activation barrier of each proposed reaction was computed to confirm that the reaction sites for chlorine were located on amino groups. This study clarified the formation mechanism of algal-derived organic chloramines, which could provide a powerful theoretical foundation for controlling organic chloramine formation in drinking water processes.
有机氯胺对饮用水安全构成了重大威胁。然而,藻类衍生的有机氯胺的形成机制仍不清楚。本研究观察到藻类悬浮液的预氧化会增加氯化过程中有机氯胺的形成。与 KMnO4 预氧化相比,O3 显著增加了藻类悬浮液的有机氯胺形成潜力。采用尺寸排阻色谱-多检测器(SEC-MDs)进行了表征,以更好地理解有机氯胺的形成机制。结果表明,经过常规水处理工艺后,低分子量蛋白质(AMW ≤ 0.64 kDa)是有机氯胺的主要前体。然后,我们专注于参与蛋白质形成的 14 种必需氨基酸。根据它们的浓度和有机氯胺形成潜力,评估了所研究样品的理论有机氯胺形成潜力。然而,理论和实验有机氯胺形成之间存在显著差距,这表明并非所有有机氮都能与氯反应形成有机氯胺。计算了凝聚双描述符(CDD)以预测肽上的亲电取代反应位点。此外,计算了每个提议反应的活化能垒,以确认氯的反应位点位于氨基上。本研究阐明了藻类衍生的有机氯胺的形成机制,可为控制饮用水处理过程中有机氯胺的形成提供有力的理论基础。