Novel brominated flame retardants in West Antarctic atmosphere (2011–2018): Temporal trends, sources and chiral signature
Novel brominated flame retardants in West Antarctic atmosphere (2011–2018): Temporal trends, sources and chiral signature
复制标题
南极西部大气中的新型溴化阻燃剂（2011-2018）：时间趋势、来源和手性特征
DOI：
10.1016/j.scitotenv.2020.137557
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发表时间：
2020
影响因子：
9.8
通讯作者：
Guibin Jiang
中科院分区：
文献类型：
--
作者：
Junpeng Zhao;Pu Wang;Chu Wang;Min Fu;Yingming Li;Ruiqiang Yang;Jianjie Fu;Yanfen Hao;Julius Matsiko;Qinghua Zhang;Guibin Jiang
2011 - 2018年，利用高容量主动式空气采样器（HV-AAS）对西南极长城站乔治王岛的气相和颗粒相样品中的新型溴化阻燃剂（NBFR）进行了全面调查。∑ 12 NBFR的浓度范围为0.27至3.0 pg m−3，平均值为1.1 ± 0.50 pg m− 3，在过去八年中呈轻微上升趋势。十溴二苯乙烷是主要的非溴化阻燃剂，平均相对贡献率为50%。所研究的NBFR大部分倾向于分布在气相中，平均比例为72 ± 16%，而logKOA值较高的NBFR在颗粒相中的比例较高。采用气体/颗粒分配模型对NBFR的环境行为进行了评价。与基于平衡态的模型相比，基于稳态的模型更好地预测了西南极大气中NBFR的气体/颗粒分配。除（1 R，2 R，5 R，6 R）-1，2，5，6-四溴环辛烷（β-TBCO）外，其它NBFR均无温度依赖性。∑ 12 NBFR的年平均浓度与东南偏东的频率呈显著负相关（ESE，112.5°）风和静风（~0 m s−1）（p< 0.05），且与西北风频率呈显著正相关（西至西北偏北，270°至337.5°）（p< 0.05），表明来自海洋区域的气团的显著影响。此外，NBFR的手性特征通常显示在大气中的非外消旋残留物。反式-（1 R，2 R）-1，2-二溴-（4S）-4-（（1 R）-1，2-二溴乙基）环己烷（α-TBECH）和β-TBCO的对映体分数（EF）分别为0.115-0.962和0.281-0.795，揭示了NBFR的次级来源，例如，来源地区的海水-空气交换和/或非外消旋残留物。据我们所知，这是对南极大气中NBFR的极少数研究之一。
Novel brominated flame retardants (NBFRs) were comprehensively investigated in both gaseous and particle phase samples collected using a high-volume active air sampler (HV-AAS) at the Chinese Great Wall Station in King George Island, West Antarctica from 2011 to 2018. The concentrations of ∑12NBFRs ranged from 0.27 to 3.0 pg m−3, with a mean value of 1.1 ± 0.50 pg m−3and the levels showed a slightly increasing trend over the eight years. Decabromodiphenyl ethane (DBDPE) was the predominant NBFR with a relative contribution of 50% on average. Most of the studied NBFRs tended to distribute in gaseous phase with an average ratio of 72 ± 16% while NBFRs with higher logKOAvalues had higher proportions in particle phase. The gas/particle partitioning models were employed to evaluate the environmental behavior of NBFRs. Compared to the equilibrium-state-based model, the steady-state-based model performed much better to predict the gas/particle partitioning of NBFRs in the West Antarctic atmosphere. Additionally, no temperature dependence was found for NBFRs exceptrac-(1R,2R,5R,6R)-1,2,5,6-tetrabromocyclooctane (β-TBCO). The annual mean concentrations of ∑12NBFRs showed a significantly negative correlation with the frequency of east-southeast (ESE, 112.5°) wind and calm wind (~0 m s−1) (p< 0.05), and a significantly positive correlation with the frequency of wind from northwest interval (west to north-northwest, 270° to 337.5°) (p< 0.05), suggesting a significant effect of air mass from the ocean area. Furthermore, the chiral signature of NBFRs showed commonly non-racemic residue in the atmosphere. The enantiomer fractions (EF) ofrac-(1R,2R)-1,2-dibromo-(4S)-4-((1R)-1,2-dibromoethly)cyclohexane (α-TBECH) and β-TBCO were 0.115–0.962 and 0.281–0.795, revealing secondary sources of NBFRs, e.g., seawater-air exchange and/or non-racemic residue in the source regions. As far as we know, this is one of very few studies on NBFRs in the Antarctic atmosphere.