School of Environment and Guangdong Key Laboratory of Environmental Pollution and Health , Jinan University , Guangzhou , 510632 , China.
Cooperative Wildlife Research Laboratory and Department of Zoology , Southern Illinois University , Carbondale , Illinois 62901 , United States.
Environ Sci Technol. 2019 Feb 19;53(4):1786-1796. doi: 10.1021/acs.est.8b05300. Epub 2019 Feb 11.
Following the phase-out of polybrominated diphenyl ether (PBDE) and hexabromocyclododecane (HBCDD) flame retardants (FRs) from North American markets, the use of alternative FRs has increased. In this study the occurrence and spatiotemporal distributions of 18 dechlorane analogues (collectively referred to as DECs) and 20 alternative brominated FRs (referred to as ABFRs, i.e., brominated FRs other than PBDEs and HBCDD) were investigated in top predator fish megacomposites (i.e., a composite of all 50 fish) collected yearly from each of the Great Lakes from 2004 to 2016. Frequently detected substances include dechlorane 602, 603, 604 Component B, anti- and syn-dechlorane plus, and chlordene plus, as well as several brominated benzene FRs (i.e., hexabromobenzene, pentabromotoluene, and tetrabromo- o-chlorotoluene). Concentrations of ΣDECs and ΣABFRs ranged from 0.33-31.9 ng/g lipid weight (lw) (0.01-8.3 ng/g wet weight or ww) and 0.91-54.7 ng/g lw (0.09-7.1 ng/g ww), respectively. Flame retardant contamination exhibited chemical-specific spatial variations across the five lakes. Concentrations of ΣABFRs in Lake Erie fish were generally lower than those from other lakes. By contrast, fish ΣDEC concentrations were highest in Lake Ontario and the composition of dechlorane analogues differed significantly between Lake Ontario and the other lakes, indicating likely point-source influences. Temporal analyses revealed declining trends of ΣDECs and ΣABFRs in most lakes except Lake Erie, with age corrected trend slopes of -13.5% to -8.8% and -20.1% to -7.0% per year, respectively.
继北美市场逐步淘汰多溴二苯醚 (PBDE) 和六溴环十二烷 (HBCDD) 阻燃剂 (FR) 之后,替代 FR 的使用有所增加。在这项研究中,于 2004 年至 2016 年期间,每年从五大湖的每个湖泊中采集顶级掠食性鱼类复合样本(即所有 50 种鱼类的组合),检测了 18 种脱氯类似物(统称 DECs)和 20 种替代溴化 FR(简称 ABFRs,即除 PBDE 和 HBCDD 以外的溴化 FR)的出现情况和时空分布。经常检测到的物质包括脱氯类似物 602、603、604B 成分、反式和顺式脱氯类似物加合物以及氯丹加合物,以及几种溴化苯 FR(即六溴苯、五溴甲苯和四溴邻氯甲苯)。ΣDECs 和 ΣABFRs 的浓度范围分别为 0.33-31.9ng/g 脂重(lw)(0.01-8.3ng/g 湿重或 ww)和 0.91-54.7ng/g lw(0.09-7.1ng/g ww)。五种湖泊中,阻燃剂污染表现出化学物质的特定空间变化。伊利湖鱼类中的 ΣABFRs 浓度一般低于其他湖泊。相比之下,安大略湖鱼类的 ΣDEC 浓度最高,安大略湖和其他湖泊的脱氯类似物组成也有显著差异,表明可能存在点源影响。时间分析表明,除伊利湖外,大多数湖泊中的 ΣDECs 和 ΣABFRs 呈下降趋势,每年的年龄校正趋势斜率分别为-13.5%至-8.8%和-20.1%至-7.0%。