Modeling global-scale fate and transport of perfluorooctanoate emitted from direct sources

被引:196
作者
Armitage, James
Cousins, Ian T. [1 ]
Buck, Robert C.
Prevedouros, Konstantinos
Russell, Mark H.
MacLeod, Matthew
Korzeniowski, Stephen H.
机构
[1] Univ Stockholm, Dept Appl Environm Sci, SE-10691 Stockholm, Sweden
[2] EI Pont Nemours & Co Inc, Wilmington, DE 19805 USA
[3] ETH, Inst Chem & Bioengn, CH-8093 Zurich, Switzerland
关键词
FLUOROTELOMER ALCOHOL BIODEGRADATION; ALPHA-HEXACHLOROCYCLOHEXANE; PERFLUORINATED CHEMICALS; ATMOSPHERIC CHEMISTRY; ARCTIC-OCEAN; FLUOROCHEMICALS; ACIDS; FRACTIONATION; CONTAMINANTS; RESIDENTS;
D O I
10.1021/es0614870
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The long-term (1950-2050) global fate of perfluorooctanoate (PFO) is investigated using the global distribution model, GloboPOP. The model is used to test the hypotheses that direct PFO emissions can account for levels observed in the global oceans and that ocean water transport to the Arctic is an important global distribution pathway. The model emission scenarios are derived from historical and projected PFO emissions solely from direct sources. Modeled ocean water concentrations compare favorably to observed PFO concentrations in the world's oceans and thus ocean inventories can be accounted for by direct sources. The model results support the hypothesis that long-range ocean transport of PFO to the Arctic is important and estimate a net PFO influx of approximately 8-23 tons per year flowing into the model's Northern Polar zone in 2005, an amount at least 1 order of magnitude greater than estimated PFO flux to the Arctic from potential indirect sources such as atmospheric transport and degradation of fluorotelomer alcohols. Modeled doubling times of ocean water concentrations in the Arctic between 1975 and 2005 of approximately 7.5-10 years are in good agreement with doubling times of PFO in Arctic biota estimated from monitoring data. The model is further applied to predict future trends in PFO contamination levels using forecasted (2005-2050) direct emissions, including substantial reductions committed to by industry. Modeled ocean water concentrations in zones near to sources decline markedly after 2005, whereas modeled concentrations in the Arctic are predicted to continue to increase until approximately 2030 and show no significant decrease for the remaining 20 years of the model simulation. Since water is the primary exposure medium for Arctic biota, these model results suggest that concentrations in Arctic biota may continue to rise long after direct emissions have been substantially reduced or eliminated.
引用
收藏
页码:6969 / 6975
页数:7
相关论文
共 52 条
[1]  
*3M COMP, 2000, AR2260600
[2]   Anthropogenic iodine-129 in the Arctic Ocean and Nordic Seas: Numerical modeling and prognoses [J].
Alfimov, V. ;
Possnert, G. ;
Aldahan, A. .
MARINE POLLUTION BULLETIN, 2006, 52 (04) :380-385
[4]  
BRICE TJ, 1950, FLUORINE CHEM
[5]  
BUCK RC, 2006, UNPUB ESTIMATED HIST
[6]   Perfluorinated chemicals in selected residents of the American continent [J].
Calafat, AM ;
Needham, LL ;
Kuklenyik, Z ;
Reidy, JA ;
Tully, JS ;
Aguilar-Villalobos, M ;
Naeher, LP .
CHEMOSPHERE, 2006, 63 (03) :490-496
[7]   Perfluorochemicals in pooled serum samples from United States residents in 2001 and 2002 [J].
Calafat, AM ;
Kuklenyik, Z ;
Caudill, SP ;
Reidy, JA ;
Needham, LL .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (07) :2128-2134
[8]  
Caliebe C., 2005, Fluoros
[9]   Changes in temperature and tracer distributions within the Arctic Ocean: Results from the 1994 Arctic Ocean section [J].
Carmack, EC ;
Aagaard, K ;
Swift, JH ;
MacDonald, RW ;
McLaughlin, FA ;
Jones, EP ;
Perkin, RG ;
Smith, JN ;
Ellis, KM ;
Killius, LR .
DEEP-SEA RESEARCH PART II-TOPICAL STUDIES IN OCEANOGRAPHY, 1997, 44 (08) :1487-+
[10]   Atmospheric chemistry of N-methyl perfluorobutane sulfonamidoethanol, C4F9SO2N(CH3)CH2CH2OH:: Kinetics and mechanism of reaction with OH [J].
D'Eon, JC ;
Hurley, MD ;
Wallington, TJ ;
Mabury, SA .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (06) :1862-1868