College of Environment, Zhejiang University of Technology, 18 Chao-wang Road, Hangzhou, 310014, China; Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, University of Chinese Academy of Sciences, Chinese Academy of Sciences, 18 Shuang-qing Road, Beijing, 100085, China.
College of Environment, Zhejiang University of Technology, 18 Chao-wang Road, Hangzhou, 310014, China.
Water Res. 2019 Jul 1;158:417-423. doi: 10.1016/j.watres.2019.03.056. Epub 2019 Mar 29.
This study investigated the VUV/UV photodegradation of three iodinated disinfection byproducts (I-DBPs), namely, triiodomethane (TIM), diiodoacetamide (DIAcAm) and triiodoacetic acid (TIAA), based on a mini-fluidic VUV/UV photoreaction system (MVPS). The pseudo-first-order rate constants (k) of TIM, DIAcAm and TIAA under VUV/UV irradiation (1769, 1301 and 1174 m einstein, respectively) were higher than those under UV irradiation (1003, 832 and 766 m einstein, respectively). The enhancement of photodegradation could be attributed to the indirect HO oxidation rather than the direct VUV photolysis. As a whole, compared with the indirect HO oxidation, the direct UV photolysis had a relatively greater contribution to the degradation of the three I-DBPs, especially DIAcAm and TIAA (ca. 57% and 60%, respectively). The two electron-withdrawing groups in DIAcAm and TIAA (i.e., acylamino and carboxyl) decreased the electron density of the C-I bonds, thus weakening the electrophilic attack of HO. The iodine in the three I-DBPs was released to form I and a small fraction (< 6%) of I was oxidized to IO, indicating that HO preferred to break the C-I bonds rather than oxidize I. The direct UV photolysis proceeded via HO-catalyzed deiodination reactions, while the indirect HO oxidation proceeded via deiodination reactions along with HO addition. The VUV/UV photodegradation of the three I-DBPs was more favored at an acidic pH but inhibited by the water matrix components (i.e., NOM, Cl and alkalinity) to different extents.
本研究基于微型流动态 VUV/UV 光反应系统(MVPS),考察了三种碘代消毒副产物(I-DBPs),即三碘甲烷(TIM)、二碘乙酰胺(DIAcAm)和三碘乙酸(TIAA)的 VUV/UV 光降解。在 VUV/UV 辐照下(分别为 1769、1301 和 1174 m einstein),TIM、DIAcAm 和 TIAA 的准一级速率常数(k)高于在 UV 辐照下(分别为 1003、832 和 766 m einstein)。光降解增强可归因于间接的 HO 氧化而非直接的 VUV 光解。总的来说,与间接的 HO 氧化相比,直接的 UV 光解对三种 I-DBPs 的降解有相对更大的贡献,特别是 DIAcAm 和 TIAA(分别约为 57%和 60%)。DIAcAm 和 TIAA 中的两个吸电子基团(即酰氨基和羧基)降低了 C-I 键的电子密度,从而削弱了 HO 的亲电攻击。三种 I-DBPs 中的碘释放形成 I,一小部分(<6%)I 被氧化成 IO,表明 HO 优先断裂 C-I 键而不是氧化 I。直接的 UV 光解通过 HO 催化的脱碘反应进行,而间接的 HO 氧化则通过脱碘反应以及 HO 加成进行。三种 I-DBPs 的 VUV/UV 光降解在酸性 pH 下更有利,但不同程度地受到水基质成分(即 NOM、Cl 和碱度)的抑制。