Untargeted characterisation of dissolved organic matter contributions to rivers from anthropogenic point sources using direct-infusion and high-performance liquid chromatography/Orbitrap mass spectrometry.
Untargeted characterisation of dissolved organic matter contributions to rivers from anthropogenic point sources using direct-infusion and high-performance liquid chromatography/Orbitrap mass spectrometry.
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DOI：
10.1002/rcm.8618
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发表时间：
2020-09
期刊：
影响因子：
--
通讯作者：
Evershed RP
中科院分区：
文献类型：
--
作者：
Pemberton JA;Lloyd CEM;Arthur CJ;Johnes PJ;Dickinson M;Charlton AJ;Evershed RP
淡水中的人为有机输入会对水生生态系统产生有害影响，引起人们对环境保护和水安全的日益关注。欧盟水框架指令（欧盟，2000/60/EC）的现行法规通过监测选定的微污染物来涉及有机污染；然而，水生生态系统的反应需要全面了解溶解有机物（DOM）的组成。高分辨率质谱 (HRMS) 的引入将极大地增进我们对源自扩散源和点源的天然和人为来源的 DOM 成分的理解。使用固相萃取 (SPE) 从河流和处理后的污水中提取 DOM，并使用溶解有机碳分析、直接注入高分辨率质谱 (DI-HRMS) 和高效液相色谱 (HPLC)/HRMS 进行分析。使用单变量和多变量统计分析获得的数据，以证明背景 DOM、人为输入和河内混合的差异。根据在线数据库搜索的 MS2 谱图实现了化合物鉴定。 DI-HRMS 谱显示所有 DOM SPE 提取物的高度复杂性。使用主成分分析 (PCA) 和层次聚类分析实现了包含数千种单独化合物的提取物的分类和可视化。 Kruskal-Wallis 分析强调了源自污水处理厂的显着区分离子，以便通过 HPLC/HRMS 进行更深入的研究。 HPLC/HRMS 中 MS2 谱图的生成为识别人为化合物提供了基础，包括：药物、违禁药物、代谢物和低聚物，尽管仍有数千种化合物尚未鉴定。这种新方法可以对提取物中的 DOM 进行全面分析，而无需对可能存在的化合物有任何先入为主的想法。该方法有可能用作高通量、定性筛选方法，以确定点源的成分是否与接收水体的成分不同，从而为识别迄今为止尚未认识到的有机对水体的贡献提供了一种新方法。
Anthropogenic organic inputs to freshwaters can exert detrimental effects on aquatic ecosystems, raising growing concern for both environmental conservation and water security. Current regulation by the EU water framework directive (European Union, 2000/60/EC) relates to organic pollution by monitoring selected micropollutants; however, aquatic ecosystem responses require a comprehensive understanding of dissolved organic matter (DOM) composition. The introduction of high‐resolution mass spectrometry (HRMS) is set to greatly increase our understanding of the composition of DOM of both natural and anthropogenic origin derived from diffuse and point sources. DOM was extracted from riverine and treated sewage effluent using solid‐phase extraction (SPE) and analysed using dissolved organic carbon analysis, direct‐infusion high‐resolution mass spectrometry (DI‐HRMS) and high‐performance liquid chromatography (HPLC)/HRMS. The data obtained were analysed using univariate and multivariate statistics to demonstrate differences in background DOM, anthropogenic inputs and in‐river mixing. Compound identifications were achieved based on MS2 spectra searched against on‐line databases. DI‐HRMS spectra showed the highly complex nature of all DOM SPE extracts. Classification and visualisation of extracts containing many thousands of individual compounds were achieved using principal component analysis (PCA) and hierarchical cluster analysis. Kruskal‐Wallis analyses highlighted significant discriminating ions originating from the sewage treatment works for more in‐depth investigation by HPLC/HRMS. The generation of MS2 spectra in HPLC/HRMS provided the basis for identification of anthropogenic compounds including; pharmaceuticals, illicit drugs, metabolites and oligomers, although many thousands of compounds remain unidentified. This new approach enables comprehensive analysis of DOM in extracts without any preconceived ideas of the compounds which may be present. This approach has the potential to be used as a high throughput, qualitative, screening method to determine if the composition of point sources differs from that of the receiving water bodies, providing a new approach to the identification of hitherto unrecognised organic contribution to water bodies.
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