Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 51, Issue 1, Pages 89-97Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.6b06128
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Funding
- U.S. EPA Great Lakes Restoration Initiative [GL-00E00538]
- Institute for Environmental Science and Policy at the University of Illinois at Chicago
- program of High Level Foreign Experts - State Administration of Foreign Experts Affairs, the P.R. China [GDT20143200016]
- 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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Polyhalogenated carbazoles (PHCZs) have been increasingly detected in the environment. Their similarities in chemical structure with legacy pollutants and their potential toxicity have caused increasing concern. In this work, 112 Ponar grab and 28 core sediment samples were collected from Lakes Michigan, Superior, and Huron, and a total of 26 PHCZs were analyzed along with unsubstituted carbazole using gas chromatography coupled with single- or triple-quadrupole mass spectrometry. Our results show that the total accumulation of PHCZs in the sediments of the upper Great Lakes is >3000 tonnes, orders,of magnitude greater than those of polychlorinated biphenyls (PCBs) and deCabromodiphenyl ether (BDt209). The 27 individual analytes differ in spatial distribution and temporal trend. Our results showed that PHCZs with-substitution patterns of -Br2-5, -Cl1-2Br2-4, or having iodine, were more abundant in sediment of Lake Michigan deposited before 1900 than those deposited more recently, implying a natural origin. Some emerging PHCZs have been increasingly deposited into the sediment in recent decades, and deserve further environmental monitoring and research. Other PHCZs with low halogen-substitution may form from in situ dehalogenation of PHCZs having more halogens. Anthropogenic sources of PHCZs may exist, particularly for the emerging and low molecular mass congeners.
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