Enhancing the Detectable Chemical Space in an Effluent-Dominated Stream: Non-Target Analysis Reveals Potential Rapid In Situ Product Formation

IF 8.8 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Alyssa L. Mianecki,  and , Gregory H. LeFevre*, 
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引用次数: 0

Abstract

Effluent-dominated streams are increasingly common in temperate regions and have potential for adverse ecological and human health effects. Nontarget analysis (NTA) using high resolution mass spectrometry (HRMS) is an emerging approach to examine complex chemical mixtures in the environment. Here, we leveraged archived samples previously analyzed for 154 target contaminants in a well-studied temperate region effluent-dominated stream and compared target results with suspected compounds from NTA. NTA enhanced the detectable chemical space by 20 times compared to target analysis alone. Target analysis was biased toward larger mass contaminants compared to the compounds detected with NTA, indicating that target analysis was not fully representative of the compound distribution for the effluent-impacted waters. Hierarchical cluster analysis exposed clusters of compounds significantly upregulated at the effluent/stream mixing zone, revealing evidence of a novel phenomenon wherein transformation product and/or metabolite formation appears to occur rapidly in situ. Additionally, an exposure-driven NTA retrospective analysis uncovered upregulation of 7endocrine-disrupting compounds that may explain prior bioassay results. These findings have urgent implications for ecosystems and downstream communities experiencing de facto wastewater reuse conditions. NTA offers enhanced characterization of complex mixtures in effluent-dominated streams and can reveal novel mixture dynamics otherwise masked when employing target analysis alone.

在以流出物为主的流中增强可检测的化学空间:非目标分析揭示了潜在的快速原位产物形成
以污水为主的河流在温带地区越来越普遍,可能对生态和人类健康造成不利影响。使用高分辨率质谱(HRMS)的非目标分析(NTA)是一种新兴的检测环境中复杂化学混合物的方法。在这里,我们利用了之前在一个研究充分的温带地区以流出物为主的溪流中分析的154种目标污染物的存档样本,并将目标结果与NTA的可疑化合物进行了比较。与单独的目标分析相比,NTA将可检测的化学空间提高了20倍。与NTA检测到的化合物相比,目标分析偏向于更大质量的污染物,这表明目标分析不能完全代表污水影响水域的化合物分布。分层聚类分析揭示了在流出/流混合区显著上调的化合物簇,揭示了一种新现象的证据,其中转化产物和/或代谢物的形成似乎在原地迅速发生。此外,一项暴露驱动的NTA回顾性分析揭示了7种内分泌干扰化合物的上调,这可能解释了先前的生物测定结果。这些发现对生态系统和下游社区具有迫切的意义。NTA提供了在以流出物为主的溪流中复杂混合物的增强表征,并且可以揭示新的混合物动力学,否则单独使用目标分析时就会被掩盖。
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来源期刊
Environmental Science & Technology Letters Environ.
Environmental Science & Technology Letters Environ. ENGINEERING, ENVIRONMENTALENVIRONMENTAL SC-ENVIRONMENTAL SCIENCES
CiteScore
17.90
自引率
3.70%
发文量
163
期刊介绍: Environmental Science & Technology Letters serves as an international forum for brief communications on experimental or theoretical results of exceptional timeliness in all aspects of environmental science, both pure and applied. Published as soon as accepted, these communications are summarized in monthly issues. Additionally, the journal features short reviews on emerging topics in environmental science and technology.
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