Semivolatile fluorinated organic compounds in Asian and western U.S air masses

Semivolatile fluorinated organic compounds in Asian and western U.S air masses
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DOI:
10.1021/es0713678
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发表时间:
2007-12-15
影响因子:
11.4
通讯作者:
Simonich, Staci
Simonich, Staci
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Piekarz, Arkadiusz M.;Primbs, Toby;Simonich, Staci

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从日本冲绳和美国俄勒冈州的合岛观测站(HSO)和美国俄勒冈州的芒特学士观测站(MBO)采集的空气样品中的半挥发性含氟有机化合物(FOCs)在2004年春季(MBO和HSO)和2006年春季(MBO)进行了测量。在亚洲和美国西部的气团中都测量到了氟调聚醇(FTOHs),尽管美国西部的气团浓度要高得多。首次报道了亚洲气团中的氟调聚烯烃和美国气团中8:2的氟调聚丙烯酸酯的浓度。在亚洲和美国西部的气团中也检测到了N-乙基全氟辛烷磺酰胺、N-甲基全氟辛烷磺胺乙醇和N-乙基全氟辛烷磺胺乙醇,但频率低于FTOHs。通过估算FTOHs在大气中的停留时间,计算FTOH浓度比,研究FTOH与非氟半挥发性有机化合物浓度的相关性,以及确定空气质量的反向轨迹,研究了FTOHs的大气来源和归宿。估算的6:2FTOH、8:2FTOH和10:2FTOH在大气中的停留时间分别为50、80和70d,2006年MBO时6:2FTOH、8:2FTOH和10:2FTOH的平均浓度比为1.0、5.0和2.5。这些大气停留时间的相对顺序可以解释观察到的MBO下8:2FTOH和10:2FTOH(相对于6:2FTOH)比北美室内空气(FTOH平均比率为1.0:2.0:1.0)增加的原因。美国西部气团中FTOH浓度与气相多环芳烃和多氯联苯浓度呈正相关(p<0.05),与农业农药浓度呈负相关(p<0.05)。与美国西部气团相比,跨太平洋气团没有这些化合物的高浓度,而经过美国西部城市地区的低边界层气团则含有高浓度的这些化合物。这表明半挥发性震源是从美国西部的城市地区排放的。
Semivolatile fluorinated organic compounds (FOCs) were measured in archived air sample extracts collected from Hedo Station Observatory (HSO) on Okinawa, Japan and Mount Bachelor Observatory (MBO), Oregon U.S. during the springs of 2004 (MBO and HSO) and 2006 (MBO). Fluorotelomer alcohols (FTOHs) were measured in both Asian and western U.S. air masses, though western U.S. air masses had significantly higher concentrations. Concentrations of fluorotelomer olefins in Asian air masses and 8:2 fluorotelomer acrylate in U.S. air masses were reported for the first time. N-ethyl perfluorooctane sulfonamide, N-methyl perfluorooctane sulfonamido ethanol, and N-ethyl perfluorooctane sulfonamido ethanol were also measured in Asian and western U.S. air masses but less frequently than FTOHs. The atmospheric sources and fate of FTOHs were investigated by estimating their atmospheric residence times, calculating FTOH concentration ratios, investigating FTOH correlations with nonfluorinated semivolatile organic compound concentrations, and determining air mass back trajectories. Estimated atmospheric residence times far 6:2 FTOH, 8:2 FTOH, and 10:2 FTOH were 50, 80, and 70 d, respectively, and the average concentration ratio of 6:2 FTOH to 8:2 FTOH to 10:2 FTOH at MBO in 2006 was 1.0 to 5.0 to 2.5. The relative order of these atmospheric residence times may explain the observed enhancement of 8:2 FTOH and 10:2 FTOH (relative to 6:2 FTOH) at MBO compared to North American indoor air (FTOH average ratio of 1.0 to 2.0 to 1.0). FTOH concentrations in western U.S. air masses were positively correlated (p < 0.05) with gas-phase polycyclic aromatic hydrocarbon and polychlorinated biphenyl concentrations and negatively correlated (p < 0.05) with agricultural pesticide concentrations. In comparison to western U.S. air masses, trans-Pacific air masses did not contain elevated concentrations of these compounds, whereas lower boundary layer air masses that passed over urban areas of the western U.S. did. This suggests that semivolatile FOCs are emitted from urban areas in the western U.S.