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莠去津的光氧化及其对氯后消毒副产物形成的影响:溶液 pH 值的影响及机制。

Photooxidation of atrazine and its influence on disinfection byproducts formation during post-chlorination: effect of solution pH and mechanism.

机构信息

School of Civil Engineering, Yantai University, Yantai, 264005, China.

Shandong Provincial Key Laboratory of Water and Soil Conservation and Environmental Protection, College of Resources and Environment, Linyi University, Linyi, 276000, China.

出版信息

Sci Rep. 2020 Nov 23;10(1):20355. doi: 10.1038/s41598-020-77006-0.

Abstract

Partial photooxidation of micropollutants may lead to various degradation intermediates, obviously affecting disinfection byproducts (DBPs) formation during the post-chlorination process. The photooxidation of atrazine (ATZ) in aqueous solutions with low-pressure mercury UV lamps in UV, UV/HO and UV/TiO treatment system and the formation of chlorinated disinfection byproducts (DBPs) during subsequent chlorination processes including dichloroacetic acid (DCAA), trichloroacetic acid (TCAA), 1,1,1-trichloro-2-propanone (TCP), trichloromethane (TCM) and chloropicrin (CHP) were investigated in this study. The effect of solution pH on the oxidation pathway of ATZ in three UV photooxidation treatment process and the impact of photooxidation on the DBPs formations were assessed. Based on UPLC-ESI-MS/MS analyses, identification of main oxidation intermediates was performed and the plausible degradation pathways of ATZ in photooxidation system were proposed, indicating that photooxidation of ATZ in UV/HO and UV/TiO process system was significantly pH-dependent processes. Dichloroacetic acid (DCAA), trichloroacetic acid (TCAA), 1,1,1-trichloro-2-propanone (TCP), trichloromethane (TCM) and chloropicrin (CHP) were detected in photooxidized ATZ solutions. Compared to the other three DBPs, TCM and TCP were the main DBPs formed. The DBPs formations were greatly promoted in oxidized ATZ solutions. Solution pH and UV irradiation time exhibited obvious impact on the DBPs formation on the basis of DBP species. The variation tendency of DBPs observed relates to the combustion of ATZ in photooxidation system and the production oxidation intermediates.

摘要

部分微污染物的光氧化作用可能导致各种降解中间产物的形成,这显然会影响后续氯化过程中消毒副产物(DBPs)的形成。本研究采用低压汞紫外灯在 UV、UV/HO 和 UV/TiO 处理系统中对水中莠去津(ATZ)进行光氧化,并考察了后续氯化过程中形成的氯化消毒副产物(DBPs),包括二氯乙酸(DCAA)、三氯乙酸(TCAA)、1,1,1-三氯-2-丙酮(TCP)、三氯甲烷(TCM)和氯仿(CHP)。考察了溶液 pH 值对三种 UV 光氧化处理过程中 ATZ 氧化途径的影响以及光氧化对 DBPs 形成的影响。基于 UPLC-ESI-MS/MS 分析,对主要氧化中间产物进行了鉴定,并提出了 ATZ 在光氧化体系中的可能降解途径,表明 UV/HO 和 UV/TiO 体系中 ATZ 的光氧化过程明显依赖于 pH 值。在光氧化 ATZ 溶液中检测到二氯乙酸(DCAA)、三氯乙酸(TCAA)、1,1,1-三氯-2-丙酮(TCP)、三氯甲烷(TCM)和氯仿(CHP)。与其他三种 DBPs 相比,TCM 和 TCP 是主要形成的 DBPs。与未氧化的 ATZ 溶液相比,氧化后的 ATZ 溶液中 DBPs 的形成大大增加。基于 DBP 种类,溶液 pH 值和紫外辐照时间对 DBPs 的形成有明显的影响。观察到的 DBPs 变化趋势与 ATZ 在光氧化体系中的燃烧和产生的氧化中间产物有关。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6417/7684306/ecd495c45f67/41598_2020_77006_Fig1_HTML.jpg

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