Center for Air Resources Engineering and Science , Clarkson University , 8 Clarkson Avenue , Potsdam , New York 13699 , United States.
Institute for a Sustainable Environment , Clarkson University , 8 Clarkson Avenue , Potsdam , New York 13699 , United States.
Environ Sci Technol. 2018 Mar 6;52(5):2909-2917. doi: 10.1021/acs.est.7b05999. Epub 2018 Feb 12.
The U.S. Environmental Protection Agency's Great Lakes Fish Monitoring and Surveillance Program (GLFMSP) has traced the fate and transport of anthropogenic chemicals in the Great Lakes region for decades. Isolating and identifying halogenated species in fish is a major challenge due to the complexity of the biological matrix. A nontargeted screening methodology was developed and applied to lake trout using a 2-dimensional gas chromatograph coupled to a high resolution time-of-flight mass spectrometer (GC×GC-HR-ToF MS). Halogenated chemicals were identified using a combination of authentic standards and library spectral matching, with molecular formula estimations provided by exact mass spectral interpretation. In addition to the halogenated chemicals currently being targeted by the GLFMSP, more than 60 nontargeted halogenated species were identified. Most appear to be metabolites or breakdown products of larger halogenated organics. The most abundant compound class was halomethoxyphenols accounting for more than 60% of the total concentration of halogenated compounds in top predator fish from all five Great Lakes illustrating the need and utility of nontargeted halogenated screening of aquatic systems using this platform.
美国环境保护署的大湖鱼类监测和监视计划（GLFMSP）几十年来一直在追踪大湖地区人为化学物质的命运和迁移。由于生物基质的复杂性，从鱼类中分离和鉴定卤代物种是一项重大挑战。本研究采用二维气相色谱-高分辨飞行时间质谱联用仪（GC×GC-HR-ToF MS）建立并应用于湖鳟鱼的非靶向筛选方法。通过使用真实标准品和库光谱匹配的组合，以及通过精确质量谱解释提供的分子公式估算，鉴定了卤代化学品。除了 GLFMSP 目前正在针对的卤代化学品外，还鉴定了 60 多种非靶向卤代物质。大多数似乎是较大卤代有机物的代谢物或分解产物。最丰富的化合物类别是卤代苯氧基苯酚，占所有五大湖顶级捕食鱼类中卤代化合物总浓度的 60%以上，这说明了使用该平台对水生系统进行非靶向卤代筛选的必要性和实用性。
