The impact of lime additions on mercury dynamics in stream chemistry and macroinvertebrates: a comparison of watershed and direct stream addition management strategies.

Acid deposition has declined across eastern North America and northern Europe due to reduced emissions of sulfur and nitrogen oxides. Ecosystem recovery has been slow with limited improvement in surface water chemistry. Delayed recovery has encouraged acid-neutralization strategies to accelerate recovery of impaired biological communities. Lime application has been shown to increase pH and dissolved organic carbon (DOC), which could also drive increased mobilization of mercury (Hg) to surface waters. A four-year study was conducted within Honnedaga Lake's watershed in the Adirondack region of New York to compare the effects of watershed and direct channel lime additions on Hg in stream water and macroinvertebrates. All treatments sharply increased stream pH and DOC concentrations, but large differences in the duration of impacts were apparent. The watershed treatment resulted in multi-year increases in concentrations and loads of total Hg (150%; 390%), DOC (190%; 350%) and nutrients, whereas total Hg and DOC increased for short periods (72-96 h) after channel treatments. No response of Hg in macroinvertebrates was evident following the watershed treatment, but a potential short-term and spatially constrained increase occurred after the channel treatment. Our observations indicate that both treatment approaches mobilize Hg, but that direct channel liming mobilizes considerably less than watershed liming over any period longer than a few days. During the final study year, increased methyl Hg concentrations were observed across reference and treated streams, which may reflect an extended dry period, highlighting that climate variation may also affect Hg dynamics.

Response of mercury in an Adirondack (NY, USA) forest stream to watershed lime application.

Surface waters in Europe and North America previously impacted by acid deposition are recovering in conjunction with declining precursor emissions since the 1980s. Lime has been applied to some impacted watersheds to accelerate recovery. The response to liming can be considered a proxy for future recovery from acid deposition. Increases in dissolved organic carbon concentrations have been observed in surface waters in response to increased pH associated with recovery from acid deposition. Although not previously described, recovery-related increases in dissolved organic carbon could drive increases in mercury concentrations and loads because of the affinity of mercury for dissolved organic matter. We used a before-after impact-response approach to describe the response of stream mercury cycling to the application of lime to the watershed of a small stream in the Adirondack Mountains of New York, USA. Dissolved organic carbon, total mercury and methylmercury concentrations increased significantly in streamwater within two weeks of treatment, to previously unobserved concentrations. After six months, post-treatment before-after impact-control (BACI) tests indicate that mean dissolved organic carbon concentrations and total mercury to dissolved organic carbon ratios remained significantly higher and limed site fluxes of methylmercury were lower than those at the reference stream. This pattern suggests total mercury is leaching at elevated levels from the limed watershed, but limitations in production and transport to the stream channel likely resulted in increases in methylmercury concentration that were of limited duration.