Piekarz Arkadiusz M, Primbs Toby, Field Jennifer A, Barofsky Douglas F, Simonich Staci
Department of Chemistry, Oregon State University, Corvallis, Oregon, USA.
Environ Sci Technol. 2007 Dec 15;41(24):8248-55. doi: 10.1021/es0713678.
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 for 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.
在2004年春季(位于美国俄勒冈州的巴彻勒山天文台[MBO]和日本冲绳的希多站天文台[HSO])和2006年春季(MBO)采集的存档空气样本提取物中,对半挥发性氟化有机化合物(FOCs)进行了测量。在亚洲和美国西部气团中均检测到了氟调聚物醇(FTOHs),不过美国西部气团中的浓度明显更高。首次报告了亚洲气团中氟调聚物烯烃以及美国气团中8:2氟调聚物丙烯酸酯的浓度。在亚洲和美国西部气团中还检测到了N - 乙基全氟辛烷磺酰胺、N - 甲基全氟辛烷磺酰胺基乙醇和N - 乙基全氟辛烷磺酰胺基乙醇,但出现频率低于FTOHs。通过估算FTOHs的大气停留时间、计算FTOH浓度比、研究FTOH与非氟化半挥发性有机化合物浓度的相关性以及确定气团后向轨迹,对FTOHs的大气来源和归宿进行了研究。6:2 FTOH、8:2 FTOH和10:2 FTOH的估算大气停留时间分别为50天、80天和70天,2006年MBO处6:2 FTOH与8:2 FTOH至10:2 FTOH的平均浓度比为1.0比5.0比2.5。这些大气停留时间的相对顺序或许可以解释与北美室内空气相比(FTOH平均比例为1.0比2.0比1.0),在MBO处观察到的8:2 FTOH和10:2 FTOH(相对于6:2 FTOH)的增强现象。美国西部气团中的FTOH浓度与气相多环芳烃和多氯联苯浓度呈正相关(p < 0.05),与农用农药浓度呈负相关(p < 0.05)。与美国西部气团相比,跨太平洋气团中这些化合物的浓度并未升高,而经过美国西部城市地区的近地面气团中则升高了。这表明半挥发性FOCs是从美国西部的城市地区排放出来的。