School of Environmental Science and Engineering , Tianjin University , Tianjin 300072 , China.
Institute of Surface-Earth System Science , Tianjin University , Tianjin 300072 , China.
Environ Sci Technol. 2019 Aug 6;53(15):9024-9033. doi: 10.1021/acs.est.9b00749. Epub 2019 Jul 15.
Monochloramine (NHCl) can be irradiated by UV to create an advanced oxidation condition (i.e., UV/NHCl) for the elimination of organic micropollutants (OMPs) from source water. However, information in retrospective studies was scarce on how UV/NHCl performance would be affected by the water matrix and OMP molecular structures. In this study, the degradation of five representative OMPs, including triclosan, carbamazepine, sulfamethoxazole, estradiol (E2), and ethinylestradiol (EE2), was examined in different water matrices. All OMPs were rapidly removed by UV/NHCl but exhibited different degradation mechanisms. Although •OH, •Cl, and direct photolysis mainly contributed to the overall degradation of OMPs in buffered nanopure water, the contribution of reactive nitrogen species (RNS) generated from the photolysis of NHCl was not negligible in the degradation of E2 and EE2. A phenolic group was identified as the moiety reactive toward RNS. Based on quantitative analysis of the impact on OMP degradation from cosolutes (including Cl, HCO, NOM) as well as pH and NHCl doses, we developed a kinetic model for the prediction of OMP degradation in complex water matrices. In environmental water matrices, the performance and radical contributions in UV/NHCl and UV/HO systems were taken into comparison, which showed faster degradation of OMPs and a more significant contribution of CO in the UV/NHCl process.
一氯胺(NHCl)可被紫外线照射生成高级氧化条件(即 UV/NHCl),从而去除水源中的有机微污染物(OMPs)。然而,关于水基质和 OMP 分子结构如何影响 UV/NHCl 性能的回顾性研究信息很少。在本研究中,在不同的水基质中考察了五种代表性 OMPs(三氯生、卡马西平、磺胺甲恶唑、雌二醇(E2)和乙炔雌二醇(EE2))的降解情况。所有 OMPs 均被 UV/NHCl 迅速去除,但表现出不同的降解机制。尽管 •OH、•Cl 和直接光解主要有助于缓冲超纯水中原位 OMPs 的整体降解,但 NHCl 光解生成的活性氮物种(RNS)对 E2 和 EE2 降解的贡献不可忽视。鉴定出酚基是与 RNS 反应的部分。基于对共溶质(包括 Cl、HCO3-、NOM)以及 pH 值和 NHCl 剂量对 OMP 降解影响的定量分析,我们开发了一个用于预测复杂水基质中 OMP 降解的动力学模型。在环境水中,比较了 UV/NHCl 和 UV/HO 体系中的性能和自由基贡献,结果表明 UV/NHCl 过程中 OMPs 的降解速度更快,CO 的贡献更显著。