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Perchlorate in The Great Lakes: Isotopic Composition and Origin

Poghosyan, Armen and Sturchio, Neil C. and Morrison, Candice G. and Beloso, Abelardo D., Jr. and Guan, Yunbin and Eiler, John M. and Jackson, W. Andrew and Hatzinger, Paul B. (2014) Perchlorate in The Great Lakes: Isotopic Composition and Origin. Environmental Science and Technology, 48 (19). pp. 11146-11153. ISSN 0013-936X. http://resolver.caltech.edu/CaltechAUTHORS:20141121-085345563

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Abstract

Perchlorate is a persistent and mobile contaminant in the environment with both natural and anthropogenic sources. Stable isotope ratios of oxygen (δ^(18)O, Δ^(17)O) and chlorine (δ^(37)Cl) along with the abundance of the radioactive isotope ^(36)Cl were used to trace perchlorate sources and behavior in the Laurentian Great Lakes. These lakes were selected for study as a likely repository of recent atmospheric perchlorate deposition. Perchlorate concentrations in the Great Lakes range from 0.05 to 0.13 μg per liter. Δ^(37)Cl values of perchlorate from the Great Lakes range from +3.0‰ (Lake Ontario) to +4.0‰ (Lake Superior), whereas δ^(18)O values range from −4.1‰ (Lake Superior) to +4.0‰ (Lake Erie). Great Lakes perchlorate has mass-independent oxygen isotopic variations with positive Δ^(17)O values (+1.6‰ to +2.7‰) divided into two distinct groups: Lake Superior (+2.7‰) and the other four lakes (∼+1.7‰). The stable isotopic results indicate that perchlorate in the Great Lakes is dominantly of natural origin, having isotopic composition resembling that measured for indigenous perchlorate from preindustrial groundwaters of the western USA. The ^(36)Cl/Cl ratio of perchlorate varies widely from 7.4 × 10^(–12) (Lake Ontario) to 6.7 × 10^(–11) (Lake Superior). These ^(36)ClO_4– abundances are consistent with an atmospheric origin of perchlorate in the Great Lakes. The relatively high ^(36)ClO_4– abundances in the larger lakes (Lakes Superior and Michigan) could be explained by the presence of ^(36)Cl-enriched perchlorate deposited during the period of elevated atmospheric ^(36)Cl activity following thermonuclear bomb tests in the Pacific Ocean.


Item Type:Article
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http://dx.doi.org/10.1021/es502796d DOIArticle
http://pubs.acs.org/doi/abs/10.1021/es502796dPublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/es502796dPublisherSupporting Information
Additional Information:© 2014 American Chemical Society. Received: June 8, 2014; Revised: August 20, 2014; Accepted: August 29, 2014; Published: August 29, 2014. This work was supported in part by the Strategic Environmental Research and Development Program (SERDP Project ER-1435) of the U.S. Department of Defense. The authors thank the captain and crew of EPA’s RV Lake Guardian for assistance in sampling the Great Lakes. The Great Lakes map in the TOC/abstract graphic is from NOAA, Great Lakes Environmental Research Laboratory.
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Funding AgencyGrant Number
Department of Defense (DOD)ER-1435
Record Number:CaltechAUTHORS:20141121-085345563
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20141121-085345563
Official Citation:Perchlorate in The Great Lakes: Isotopic Composition and Origin Armen Poghosyan, Neil C. Sturchio, Candice G. Morrison, Abelardo D. Beloso, Jr., Yunbin Guan, John M. Eiler, W. Andrew Jackson, and Paul B. Hatzinger Environmental Science & Technology 2014 48 (19), 11146-11153
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:52031
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:21 Nov 2014 17:26
Last Modified:21 Nov 2014 17:26

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