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在紫外光照射下水中特戊酰基三酮的光降解:转化产物的鉴定和光降解途径的阐明。

Photodegradation of tefuryltrione in water under UV irradiation: Identification of transformation products and elucidation of photodegradation pathway.

机构信息

College of Agriculture, Northeast Agricultural University, Harbin, 150030, Heilongjiang, China; Safety and Quality Institute of Agricultural Products, Heilongjiang Academy of Agricultural Sciences, Harbin, 150086, China.

Safety and Quality Institute of Agricultural Products, Heilongjiang Academy of Agricultural Sciences, Harbin, 150086, China.

出版信息

Chemosphere. 2019 Jul;227:133-141. doi: 10.1016/j.chemosphere.2019.03.174. Epub 2019 Apr 6.

Abstract

Photodegradation is an important abiotic degradation process in the aquatic environment. In this study, the photodegradation of tefuryltrione in aqueous solution was investigated under UV-Visible irradiation. Effects of carbonate (CO), bicarbonate (HCO), nitrate (NO), hydrogen phosphate (HPO), potassium (K), and ammonium (NH) on the photodegradation kinetics of tefuryltrione were evaluated. Results showed that tefuryltrione photodegradation was increased by HCO, CO, and NO in the range of 0.1-10 mmol L; decreased by HPO; and insignificantly affected by K and NH. Twelve main transformation products (TPs) were separated and identified on the basis of mass spectrum data assigned by elemental-composition calculations, comparison of structural analogs, and available literature. A tentative photodegradation pathway was further proposed depending on the identified TPs and their kinetic evolutions. Results indicated that TP 1 was generated by the hydroxyl that substituted for chlorine, TP 2 was formed by the cleavage of the ether bond of tefuryltrione, and TPs 3-6 were formed by the breakage of the CC bond of the keto moiety of tefuryltrione. Further, TPs 9-12 were formed by the rearrangement of tefuryltrione-photodegradation products. These findings are highly important for elucidating the environmental fate of tefuryltrione in aquatic ecosystems.

摘要

光降解是水生环境中一种重要的非生物降解过程。本研究采用紫外-可见辐射,考察了四氟苯甲酮在水溶液中的光降解行为。研究了碳酸盐(CO)、碳酸氢盐(HCO)、硝酸盐(NO)、氢磷酸盐(HPO)、钾(K)和铵(NH)对四氟苯甲酮光降解动力学的影响。结果表明,HCO、CO 和 NO 在 0.1-10mmol/L 范围内促进了四氟苯甲酮的光降解;HPO 则抑制了四氟苯甲酮的光降解;K 和 NH 对四氟苯甲酮的光降解影响不显著。基于元素组成计算、结构类似物比较和文献报道分配的质谱数据,分离和鉴定了 12 种主要转化产物(TPs)。根据鉴定的 TPs 及其动力学演变,进一步提出了光降解途径的假设。结果表明,TP1 是由取代氯的羟基生成的,TP2 是由四氟苯甲酮的醚键断裂生成的,TPs3-6 是由四氟苯甲酮酮式部分的 CC 键断裂生成的。此外,TPs9-12 是由四氟苯甲酮光降解产物的重排生成的。这些发现对于阐明四氟苯甲酮在水生生态系统中的环境归宿具有重要意义。

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