Institute for a Sustainable Environment, Clarkson University, Potsdam, NY, United States of America.
Civil and Environmental Engineering, Clarkson University, Potsdam, NY, United States of America; Center for Air and Aquatic Resources Engineering and Science, Clarkson University, Potsdam, NY, United States of America.
Sci Total Environ. 2021 Jul 15;778:146151. doi: 10.1016/j.scitotenv.2021.146151. Epub 2021 Mar 5.
This work presents the first assessment of temporal trends (2005-2016) for perfluoroalkyl acids (PFAAs) in top predator fish of the Laurentian Great Lakes except Lake Ontario, for which we provide a post-2008 update. Lake trout (Salvelinus namaycush) or walleye (Sander vitreus; Lake Erie only) collected annually from 2005 to 2016 were analyzed for 12 perfluoroalkyl carboxylic acids (PFCAs) and 4 perfluoroalkyl sulfonic acids (PFSAs) with carbon chain lengths between 4 and 16 (C4-C16). Individual analyte concentrations generally decreased in fish basin-wide between 2005 and 2016, including Lake Ontario lake trout previously found to lack declining PFAA concentrations up until 2008. Declining fish PFAA burden reflects a positive response to the industrial phase-outs of these chemicals. Notable exceptions to this general decline included most analytes in lake trout collected from Lake Superior near Keweenaw Point and C6 and C8 PFSAs and C9 PFCAs in Lake Erie lake trout and walleye, which exhibited constant or increasing concentrations in recent years. Recent increases in Lake Superior shoreline development and mobilization from increased sediment resuspension and contamination from biosolids-amended agricultural soils in the Lake Erie watershed are plausible explanations for these cases. However, data scarcity prohibits confirmation of these suspected causes. The lingering lack of declining concentrations noted in this study together with the ongoing evolution of the fluorinated chemical industry emphasize the vigilance needed to better understand how past and future emissions will affect the Great Lakes and global ecosystems.
本研究首次评估了除安大略湖以外的北美五大湖顶级捕食性鱼类中全氟烷基酸（PFAAs）的时间趋势（2005-2016 年），我们还提供了 2008 年后的安大略湖数据更新。2005 年至 2016 年，每年从安大略湖采集湖鳟（Salvelinus namaycush）或大眼梭鲈（Sander vitreus；仅在伊利湖），分析了 12 种全氟烷基羧酸（PFCAs）和 4 种全氟烷基磺酸（PFSAs），其碳链长度在 4 到 16 之间（C4-C16）。在整个流域范围内，鱼类中各个分析物的浓度普遍在 2005 年至 2016 年之间下降，包括之前发现的安大略湖湖鳟，其 PFAA 浓度在 2008 年之前并未下降。鱼类中 PFAAs 负担的下降反映了这些化学物质的工业淘汰取得了积极成效。但也有一些明显的例外，包括在基威诺半岛附近的苏必利尔湖采集的湖鳟中的大多数分析物，以及伊利湖湖鳟和大眼梭鲈中的 C6 和 C8 PFSAs 和 C9 PFCAs，这些物质近年来的浓度保持不变或呈上升趋势。最近苏必利尔湖沿岸开发活动增加，以及伊利湖流域的生物固体处理过的农业土壤导致沉积物再悬浮和污染增加，这些可能是造成这些情况的原因。然而，数据的缺乏限制了对这些可疑原因的确认。本研究中注意到的浓度持续下降，以及氟化学工业的持续发展，都强调了需要保持警惕，以更好地了解过去和未来的排放将如何影响五大湖和全球生态系统。
