Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 51, Issue 3, Pages 1441-1449Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.6b05484
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Funding
- U.S. EPA Great Lakes Restoration Initiative with Assistance [GL-00E00538]
- National Natural Science Foundation of China [21625702, 21407157]
- National Basic Research Program of China [2015CB453102]
- Strategic Priority Research Program of the Chinese Academy of Science [XDB14010400]
- Institute for Environmental Science and Policy at the University of Illinois at Chicago (UIC)
- Canada Research Chair program
- High Level Foreign Experts [GDT20143200016]
- State Administration of Foreign Experts Affairs
- P.R. China to Nanjing University
- Einstein Professor Program of the Chinese Academy of Sciences
- Distinguished Visiting Professorship in the School of Biological Sciences of the University of Hong Kong
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This is the first study on organophosphate ester (OPEs) flame retardants and plasticizers in the sediment of the Great Lakes. Concentrations of 14 OPEs were measured in three sediment cores and 88 Ponar surface grabs collected from Lakes Ontario, Michigan, and Superior of North America. The sum of these OPEs (Sigma 14OPEs) in Ponar grabs averaged 2.2, 4.7, and 16.6 ng g(-1)dw in Lakes Superior, Michigan, and Ontario, respectively. Multiple linear regression analyses demonstrated statistically significant associations between logarithm concentrations of Sigma 14OPEs as well as selected congeners in surface grab samples and sediment organic carbon content as well as a newly developed urban distance factor. Temporal trends observed in dated sediment cores from Lake Michigan demonstrated that the recent increase in depositional flux to sediment is dominated by chlorinated OPEs, particularly tris(2chloroisopropyl) phosphate (TCPP), which has a doubling time of about 20 years. Downward diffusion within sediment may have caused vertical fractionation of OPEs over time. Two relatively hydrophilic OPEs including TCPP had much higher concentrations in sediment than estimated based on equilibria between water and sediment organic carbon. Approximately a quarter (17 tonnes) of the estimated total OPE burden (63 tonnes) in Lake Michigan resides in sediment, which may act as a secondary source releasing OPEs to the water column for years to come.
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