In Silico Supported Nontarget Analysis of Contaminants of Emerging Concern: Increasing Confidence in Unknown Identification in Wastewater and Surface Waters
In Silico Supported Nontarget Analysis of Contaminants of Emerging Concern: Increasing Confidence in Unknown Identification in Wastewater and Surface Waters
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DOI：
10.1021/acsestwater.1c00105
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发表时间：
2021-08-01
期刊：
影响因子：
--
通讯作者：
Aga, Diana S.
中科院分区：
文献类型：
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作者：
Angeles, Luisa F.;Halwatura, Lahiruni M.;Aga, Diana S.
利用液相色谱-高分辨质谱联用技术（LC-HRMS）进行非目标分析是一种有价值的方法，用于表征环境中的新兴关注污染物（CEC）。在这项研究中，废水和地表水样品在菲律宾马尼拉的三个地点进行了分析CEC使用非目标分析方法与LC-Orbitrap。先前优化的半自动化工作流程用于化合物发现者的数据处理。共鉴定了157种化合物，其中21种用参比标准品确认，83种用质谱库（mzCloud）的证据确认，53种使用计算机碎片（MetFrag）初步鉴定。这些化合物包括药物如抗生素、抗真菌和抗高血压化合物、人类代谢物、天然产物、杀虫剂和工业化学品。用参比标准品确认的化合物包括抗生素环丙沙星、克拉霉素、乙酰磺胺甲恶唑和甲氧苄啶（2 - 19 ng/L），以及抗真菌化合物多菌灵和氯咪巴唑（3-47 ng/L）。还检测到杀虫剂避蚊胺和敌草隆（37纳克/升）。初步的多变量线性回归质量结构保留关系（QSRR）模型的基础上量子化学分子描述符的实用程序进行了演示。本研究证明了使用有助于注释HRMS数据和根据标准化分类系统报告检测的工具和软件的重要性。废水和地表水样品中几种CEC的检测表明，在确定环境中CEC的发生时进行非目标分析的重要性。
Nontarget analysis using liquid chromatography-high resolution mass spectrometry (LC-HRMS) is a valuable approach in characterizing for contaminants of emerging concern (CECs) in the environment. In this study, wastewater and surface water samples from three locations in Manila, Philippines were analyzed for CECs using a nontarget analysis approach with an LC-Orbitrap. A previously optimized semiautomated workflow was used for data processing with Compound Discoverer. A total of 157 compounds were identified, with 21 confirmed with reference standards, 83 confirmed with evidence from a mass spectral library (mzCloud), and 53 tentatively identified using in silico fragmentation (MetFrag). These compounds include pharmaceuticals such as antibiotics, antifungal, and antihypertensive compounds, human metabolites, natural products, pesticides, and industrial chemicals. Compounds confirmed with reference standards include antibiotics ciprofloxacin, clarithromycin, acetyl-sulfamethoxazole, and trimethoprim (2 to 19 ng/L), and antifungal compounds carbendazim and climbazole (3-47 ng/L). The pesticides diethyltoluamide (DEET) and diuron were also detected (37 ng/L). The utility of a preliminary multivariable linear regression quality structure-retention relationship (QSRR) model based on quantum chemical molecular descriptors is demonstrated. This study demonstrates the importance of using tools and software that are helpful for annotating HRMS data and reporting detections according to a standardized classification system. The detection of several CECs in wastewater and surface water samples show the importance of performing nontarget analysis in determining occurrence of CECs in the environment.