Three-year monitoring of atmospheric PCBs and PBDEs at the Chinese Great Wall Station, West Antarctica: Levels, chiral signature, environmental behaviors and source implication

Three-year monitoring of atmospheric PCBs and PBDEs at the Chinese Great Wall Station, West Antarctica: Levels, chiral signature, environmental behaviors and source implication
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南极洲西部中国长城站大气 PCBs 和 PBDEs 的三年监测:水平、手性特征、环境行为和来源影响

DOI:
10.1016/j.atmosenv.2016.11.036
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发表时间:
2017-02
影响因子:
5
通讯作者:
Jiang Guibin
Jiang Guibin
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Wang Pu;Li Yingming;Zhang Qinghua;Yang Qinghua;Zhang Lin;Liu Fubin;Fu Jianjie;Meng Wenying;Wang Dou;Sun Huizhong;Zheng Shucheng;Hao Yanfen;Liang Yong;Jiang Guibin

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2011年1月至2014年1月,在南极洲西部乔治国王岛的中国长长城站使用大容量空气采样器对多氯联苯(PCBs)和多溴联苯醚(PBDEs)进行了为期三年的监测活动。结果表明:Σ20PCB和Σ27PBDE(气体+颗粒)浓度分别为5.87 ~ 72.7 pg m−3和0.60 ~ 16.1 pg m−3;较轻的同系物,特别是PCB-11(非aroclor同系物)占主导地位Σ20PCBs,而BDE-209除了较轻的同系物(例如BDE-28和-17)外,对Σ27PBDEs也有重大贡献。手性特征表明,样品中存在手性多氯联苯的非消旋残基,表明空气-海水交换这一二次源可能对空气中手性多氯联苯的消旋体组成产生影响。较轻的多氯联苯(不包括PCB-11)在2011年和2012年表现出明显的温度依赖性,反映了局部地表旋转化辐射的影响。然而,持久性有机污染物气体浓度与温度倒数(1/T)的回归线的浅斜率表明,远距离大气输送(LRAT)是多氯联苯和多溴二苯醚进入南极环境的重要途径。此外,从技术配方中得出的不同特征同系物之间的相关性和比率表明,十溴二苯醚的本地来源和高溴二苯醚的光降解。对持久性有机污染物的气/颗粒分配进行了评价,结果表明,基于稳态的模型总体上优于基于平衡态的模型。然而,前者仍然低估了大多数pcb在颗粒相中的分配(logKOA<11),这意味着在对logKOA较低的化合物使用时需要进一步优化。
A three-year monitoring campaign (Jan 2011–2014) of polychlorinated biphenyl (PCBs) and polybrominated diphenyl ethers (PBDEs) was conducted using a high-volume air sampler at the Chinese Great Wall Station in King George Island, West Antarctica. The results showed that the Σ20PCB and Σ27PBDE concentrations (gas + particle) were 5.87–72.7 pg m−3and 0.60–16.1 pg m−3, respectively. The lighter congeners especially PCB-11 (a non-Aroclor congener) dominated Σ20PCBs, while BDE-209 made a significant contribution to Σ27PBDEs apart from the lighter congeners (e.g., BDE-28 and -17). The chiral signature indicated nonracemic residues of chiral PCBs in the samples, suggesting potential influence of the secondary source, i.e. air-seawater exchange, on the atropisomer composition of chiral PCBs in air. Lighter PCBs (excluding PCB-11) showed significant temperature dependence in 2011 and 2012, reflecting the influence of revolatilization emission from the local surface. However, the shallow slopes of the regression lines for gaseous concentrations of POPs against reciprocal temperature (1/T) suggested long-range atmospheric transport (LRAT) as an important pathway for both PCBs and PBDEs into the Antarctic environment. Furthermore, correlations and ratios between different signature congeners deriving from the technical formulations indicated a local source of Deca-BDE and photodegradation of higher brominated BDEs. The gas/particle partitioning of POPs was also evaluated and the newly developed steady-state-based model generally showed a better performance than the equilibrium-state-based model. However, the former still underestimated the partitioning of most PCBs (logKOA<11) in particle phase, implying that further optimization is necessary when using it for those compounds with lower logKOA.
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