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Mercury stable isotope abundances were used to trace transport of Hg-impacted river sediment near a coal ash spill at Harriman, Tennessee, USA. δ202Hg values for Kingston coal ash released into the Emory River in 2008 are significantly negative (-1.78 ± 0.35‰), whereas sediments of the Clinch River, into which the Emory River flows, are contaminated by an additional Hg source (potentially from the Y-12 complex near Oak Ridge, Tennessee) with near-zero values (-0.23 ± 0.16‰). Nominally uncontaminated Emory River sediments (12 miles upstream from the Emory-Clinch confluence) have intermediate values (-1.17 ± 0.13‰) and contain lower Hg concentrations. Emory River mile 10 sediments, possibly impacted by an old paper mill has δ202Hg values of -0.47 ± 0.04‰. A mixing model, using δ202Hg values and Hg concentrations, yielded estimates of the relative contributions of coal ash, Clinch River, and Emory River sediments for a suite of 71 sediment samples taken over a 30 month time period from 13 locations. Emory River samples, with two exceptions, are unaffected by Clinch River sediment, despite occasional upstream flow from the Clinch River. As expected, Clinch River sediment below its confluence with the Emory River are affected by Kingston coal ash; however, the relative contribution of the coal ash varies among sampling sites [ABSTRACT FROM AUTHOR]

The Tennessee Valley Authority Kingston coal ash spill in December 2008 deposited approximately 4.1 million m(3) of fly ash and bottom ash into the Emory and Clinch River system (Harriman, Tennessee, U.S.A.). The objective of this study was to investigate the impact of the ash on surface water and sediment quality over an eighteen month period after the spill, with a specific focus on mercury and methylmercury in sediments. Our results indicated that surface water quality was not impaired with respect to total mercury concentrations. However, in the sediments of the Emory River near the coal ash spill, total mercury concentrations were 3- to 4-times greater than sediments several miles upstream of the ash spill. Similarly, methylmercury content in the Emory and Clinch River sediments near the ash spill were slightly elevated (up to a factor of 3) at certain locations compared to upstream sediments. Up to 2% of the total mercury in sediments containing coal ash was present as methylmercury. Mercury isotope composition and sediment geochemical data suggested that elevated methylmercury concentrations occurred in regions where native sediments were mixed with coal ash (e.g., less than 28% as coal ash in the Emory River). This coal ash may have provided substrates (such as sulfate) that stimulated biomethylation of mercury. The production of methylmercury in these areas is a concern because this neurotoxic organomercury compound can be highly bioaccumulative. Future risk assessments of coal ash spills should consider not only the leaching potential of mercury from the wastes but also the potential for methylmercury production in receiving waters.