Spatial and Temporal Trends of Polyhalogenated Carbazoles in Sediments of Upper Great Lakes: Insights into Their Origin

Jiehong Guo; Zhuona Li; Prabha Ranasinghe; Solidea Bonina; Soheil Hosseini; Margaret B. Corcoran; Colin Smalley; Karl J. Rockne; Neil C. Sturchio; John P. Giesy; An Li

doi:10.1021/acs.est.6b06128

Spatial and Temporal Trends of Polyhalogenated Carbazoles in Sediments of Upper Great Lakes: Insights into Their Origin

Jiehong Guo, Zhuona Li, Prabha Ranasinghe, Solidea Bonina, Soheil Hosseini, Margaret B. Corcoran, Colin Smalley, Karl J. Rockne, Neil C. Sturchio, John P. Giesy, An Li

Research output: Contribution to journal › Article › peer-review

54 Scopus citations

Abstract

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 (BDE209). The 27 individual analytes differ in spatial distribution and temporal trend. Our results showed that PHCZs with substitution patterns of -Br_2-5, -Cl_1-2Br_2-4, 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.

Original language	English (US)
Pages (from-to)	89-97
Number of pages	9
Journal	Environmental Science and Technology
Volume	51
Issue number	1
DOIs	https://doi.org/10.1021/acs.est.6b06128
State	Published - Jan 3 2017
Externally published	Yes

Bibliographical note

Funding Information:
This research was part of the Great Lakes Sediment Surveillance Program (GLSSP) funded by a Cooperative Agreement from the U.S. EPA Great Lakes Restoration Initiative with Assistance No. GL-00E00538 (EPA Program Officer Todd Nettesheim). J.G. and S.H. were also supported by Predoctoral Fellowships from the Institute for Environmental Science and Policy at the University of Illinois at Chicago.

Publisher Copyright:
© 2016 American Chemical Society.

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title = "Spatial and Temporal Trends of Polyhalogenated Carbazoles in Sediments of Upper Great Lakes: Insights into Their Origin",

abstract = "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 (BDE209). 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.",

author = "Jiehong Guo and Zhuona Li and Prabha Ranasinghe and Solidea Bonina and Soheil Hosseini and Corcoran, {Margaret B.} and Colin Smalley and Rockne, {Karl J.} and Sturchio, {Neil C.} and Giesy, {John P.} and An Li",

note = "Funding Information: This research was part of the Great Lakes Sediment Surveillance Program (GLSSP) funded by a Cooperative Agreement from the U.S. EPA Great Lakes Restoration Initiative with Assistance No. GL-00E00538 (EPA Program Officer Todd Nettesheim). J.G. and S.H. were also supported by Predoctoral Fellowships from the Institute for Environmental Science and Policy at the University of Illinois at Chicago. Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

year = "2017",

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doi = "10.1021/acs.est.6b06128",

language = "English (US)",

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T1 - Spatial and Temporal Trends of Polyhalogenated Carbazoles in Sediments of Upper Great Lakes

T2 - Insights into Their Origin

AU - Guo, Jiehong

AU - Li, Zhuona

AU - Ranasinghe, Prabha

AU - Bonina, Solidea

AU - Hosseini, Soheil

AU - Corcoran, Margaret B.

AU - Smalley, Colin

AU - Rockne, Karl J.

AU - Sturchio, Neil C.

AU - Giesy, John P.

AU - Li, An

N1 - Funding Information: This research was part of the Great Lakes Sediment Surveillance Program (GLSSP) funded by a Cooperative Agreement from the U.S. EPA Great Lakes Restoration Initiative with Assistance No. GL-00E00538 (EPA Program Officer Todd Nettesheim). J.G. and S.H. were also supported by Predoctoral Fellowships from the Institute for Environmental Science and Policy at the University of Illinois at Chicago. Publisher Copyright: © 2016 American Chemical Society.

PY - 2017/1/3

Y1 - 2017/1/3

N2 - 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 (BDE209). 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.

AB - 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 (BDE209). 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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VL - 51

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JO - Environmental Science & Technology

JF - Environmental Science & Technology

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Spatial and Temporal Trends of Polyhalogenated Carbazoles in Sediments of Upper Great Lakes: Insights into Their Origin

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