Decadal Differences in Emerging Halogenated Contaminant Profiles in Great Lakes Top Predator Fish
Decadal Differences in Emerging Halogenated Contaminant Profiles in Great Lakes Top Predator Fish
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DOI：
10.1021/acs.est.0c03825
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发表时间：
2020-11-17
影响因子：
11.4
通讯作者：
Crimmins, Bernard S.
中科院分区：
文献类型：
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作者：
Baygi, Sadjad Fakouri;Fernando, Sujan;Crimmins, Bernard S.
几十年来一直在监测五大湖中遗留的卤化污染物，但还有许多其他未知的卤化污染物可能影响五大湖的生态系统。为了解决这一问题，在2005/2006年和2015/2016年从每个湖泊收集了湖鳟鱼（Salvelinus namaycush），并筛选了先前未识别的化合物。使用大气压气相色谱-四极杆飞行时间质谱仪在正和负模式下操作产生的高分辨率质谱数据文件，使用同位素轮廓去卷积色谱算法分离未知的卤化组分。新检测到的特征的时间和空间差异被用来隔离新的潜在污染物。将未知卤代化合物（或特征）的十年差异与多氯联苯总浓度趋势进行了比较。检测到超过2000个未知的卤化特征。正如预期的那样，上级湖包含的未知卤化特征数量最少，而安大略湖包含的数量最多。与通常监测的传统遗留污染物特征相比，未知特征倾向于具有较少的Cl和/或Br原子。湖泊之间的未知卤代化合物的不同模式表明，在五大湖中仍然存在目前监测计划所遗漏的不明卤代污染物来源。
Legacy halogenated contaminants have been monitored in the Great Lakes for decades, but there are many additional unknown halogenated contaminants potentially affecting the Great Lakes ecosystem. To address this concern, lake trout (Salvelinus namaycush) were collected in 2005/2006 and 2015/2016 from each lake and screened for previously unidentified compounds. The isotopic profile deconvoluted chromatogram algorithm was used to isolate unknown halogenated components using high-resolution mass spectrometry data files generated by an atmospheric pressure gas chromatography-quadrupole time-of-flight mass spectrometer operated in positive and negative modes. The temporal and spatial differences in the newly detected features were used to isolate new potential contaminants. Decadal differences in the unknown halogenated compounds (or features) were compared with the total polychlorinated biphenyl concentration trends. Greater than 2000 unknown halogenated features were detected. As expected, Lake Superior contained the lowest number of unknown halogenated features, whereas Lake Ontario contained the highest. Unknown features tended to have fewer Cl and/or Br atoms compared to traditional legacy contaminant features typically monitored. Diverse patterns of unknown halogenated compounds between lakes suggested that there continues to be unidentified sources of halogenated contaminants in the Great Lakes missed by current monitoring programs.