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环境样品中抗菌剂转化产物的可疑筛查 开发在伪 MRM 过渡中运行的 LC-QTrap 方法。

Suspect screening of antimicrobial agents transformation products in environmental samples development of LC-QTrap method running in pseudo MRM transitions.

机构信息

Silesian University of Technology, Faculty of Chemistry, Department of Inorganic, Analytical Chemistry and Electrochemistry, 6 B. Krzywoustego Str., 44-100 Gliwice, Poland.

University of Warmia and Mazury in Olsztyn, Faculty of Geoengineering, Department of Engineering of Water Protection and Environmental Microbiology, 1 Prawocheńskiego Str., 10-720 Olsztyn, Poland.

出版信息

Sci Total Environ. 2022 Feb 20;808:152114. doi: 10.1016/j.scitotenv.2021.152114. Epub 2021 Dec 3.

Abstract

The aim of the work was to develop a new HPLC-MS/MS method that allows for the simultaneous detection of antimicrobials agents (targeted analysis) and their transformation products (non-targeted analysis), which enabled the elucidation of their transformation pathways in the environment. Targeted analysis was performed for 16 selected antimicrobials agents (AMs) in wastewater collected at different stages of the treatment process and river water from sections before and after wastewater discharge. The samples were collected in the Łyna sewage treatment plant (Olsztyn, Poland) in three measuring periods at different seasons. Analytes were selected from tetracyclines, fluoroquinolones, β-lactams, macrolides, glycopeptides, lincosamides and synthetic antibiotics. As a part of the targeted analysis, 13 AMs were detected in wastewater samples, and 7 of them in river water samples. However, their presence and concentrations were closely related to the type of the sample and the season in which the sample was taken. The highest concentrations of AMs were detected in samples collected in September (max. 1643.7 ng L TRI), while the lowest AMs concentrations were found in samples collected in June (max. 136.1 ng L CLR). The total content of AMs in untreated wastewater was in the range of 1.42-1644 ng L, while in the river water was for upstream 1.22-48.73 ng L and for downstream 2.24-149 ng L. In the non-target analysis, 33 degradation products of the selected AMs were identified, and the transformation pathways of their degradation were speculated. In the course of the research, it was found that as a result of the processes taking place in wastewater treatment plant, the parent substances are transformed into a number of stable transformation products. Transformation products resulted from hydroxylation, ring opening, oxidation, methylation or demethylation, carboxylation, or cleavage of the CN bond of the parent AMs.

摘要

本工作旨在开发一种新的 HPLC-MS/MS 方法,该方法可同时检测抗菌剂(靶向分析)及其转化产物(非靶向分析),从而阐明其在环境中的转化途径。靶向分析针对污水处理过程不同阶段采集的废水和废水排放前后的河流水中的 16 种选定抗菌剂(AMs)进行。样品于不同季节在三个测量期内在波兰奥尔什丁的林那污水处理厂(Łyna sewage treatment plant)采集。分析物选自四环素类、氟喹诺酮类、β-内酰胺类、大环内酯类、糖肽类、林可酰胺类和合成抗生素。作为靶向分析的一部分,在废水样品中检测到 13 种 AMs,在河水样品中检测到 7 种 AMs。然而,它们的存在和浓度与样品类型以及采样季节密切相关。在 9 月采集的样品中检测到 AMs 的浓度最高(最大值为 1643.7 ng/L TRI),而在 6 月采集的样品中 AMs 的浓度最低(最大值为 136.1 ng/L CLR)。未经处理的废水中 AMs 的总含量在 1.42-1644 ng/L 范围内,而在河水中上游为 1.22-48.73 ng/L,下游为 2.24-149 ng/L。在非靶向分析中,鉴定出了选定 AMs 的 33 种降解产物,并推测了其降解的转化途径。在研究过程中发现,由于污水处理厂中发生的过程,母体物质转化为许多稳定的转化产物。转化产物来自母体 AMs 的羟基化、开环、氧化、甲基化或脱甲基化、羧化或 CN 键的断裂。

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