Experimental evidence for recovery of mercury-contaminated fish populations.

Anthropogenic releases of mercury (Hg)1-3 are a human health issue4 because the potent toxicant methylmercury (MeHg), formed primarily by microbial methylation of inorganic Hg in aquatic ecosystems, bioaccumulates to high concentrations in fish consumed by humans5,6. Predicting the efficacy of Hg pollution controls on fish MeHg concentrations is complex because many factors influence the production and bioaccumulation of MeHg7-9. Here we conducted a 15-year whole-ecosystem, single-factor experiment to determine the magnitude and timing of reductions in fish MeHg concentrations following reductions in Hg additions to a boreal lake and its watershed. During the seven-year addition phase, we applied enriched Hg isotopes to increase local Hg wet deposition rates fivefold. The Hg isotopes became increasingly incorporated into the food web as MeHg, predominantly from additions to the lake because most of those in the watershed remained there. Thereafter, isotopic additions were stopped, resulting in an approximately 100% reduction in Hg loading to the lake. The concentration of labelled MeHg quickly decreased by up to 91% in lower trophic level organisms, initiating rapid decreases of 38-76% of MeHg concentration in large-bodied fish populations in eight years. Although Hg loading from watersheds may not decline in step with lowering deposition rates, this experiment clearly demonstrates that any reduction in Hg loadings to lakes, whether from direct deposition or runoff, will have immediate benefits to fish consumers.

Investigation of uptake and retention of atmospheric Hg(II) by boreal forest plants using stable Hg isotopes.

Although there is now a general consensus among mercury (Hg) biogeochemists that increased atmospheric inputs of inorganic Hg(II) to lakes and watersheds can result in increased methylmercury (MeHg) concentrations in fish, researchers still lack kinetic data describing the movement of Hg from the atmosphere, through watershed and lake ecosystems, and into fish. The use of isotopically enriched Hg species in environmental studies now allows experimentally applied new Hg to be distinguished from ambient Hg naturally present in the system. Four different enriched stable Hg(II) isotope "spikes" were applied sequentially over four years to the ground vegetation of a microcatchment at the Experimental Lakes Area (ELA) in the remote boreal forest of Canada to examine retention of Hg(II) following deposition. Areal masses of the spikes and ambient THg (all forms of Hg in a sample) were monitored for eight years, and the pattern of spike retention was used to estimate retention of newly deposited ambient Hg within the ground vegetation pool. Fifty to eighty percent of applied spike Hg was initially retained by ground vegetation. The areal mass of spike Hg declined exponentially over time and was best described by a first-order process with constants(k) ranging between 9.7 x 10(-40 day(-1) and 11.6 x 10(-4) day(-1). Average halflife (t1/2) of spike Hg within the ground vegetation pool (+/-S.D.) was 704 +/- 52 days. This retention of new atmospheric Hg(II) by vegetation delays movement of new Hg(II) into soil, runoff, and finally into adjacent lakes. Ground-applied Hg(II) spikes were not detected in tree foliage and litterfall, indicating that stomatal and/or root uptake of previously deposited Hg (i.e., "recycled" from ground vegetation or soil Hg pools) were likely not large sources of foliar Hg under these experimental conditions.

Long-term wet and dry deposition of total and methyl mercury in the remote boreal ecoregion of Canada.

Although a positive relationship between atmospheric loadings of inorganic mercury (Hg(II)) to watersheds and concentrations of methyl mercury (MeHg) in fish has now been established, net wet and dry deposition of Hg(II) and MeHg to watersheds remains challenging to quantify. In this study, concentrations and loadings of total mercury (THg; all forms of Hg in a sample) and MeHg in open area wet deposition, throughfall, and litterfall were quantified atthe remote Experimental Lakes Area in the boreal ecoregion, NW Ontario, Canada. Between 1992 and 2006, mean annual THg and MeHg loadings in the open were 36 +/- 17 and 0.5 +/- 0.2 mg ha(-1), respectively. Throughfall THg and MeHg loadings were generally 2-4 times and 0.8-2 times higher, respectively, than loadings in the open. Loadings of both THg and MeHg were highest under an old growth spruce/fir canopy and lowest under a deciduous maple canopy, whereas loadings under young jack pine and wetland spruce/pine/alder canopies were intermediate. Litterfall generally represented the largest input of THg (86-105 mg ha(-1)) and MeHg (0.7-0.8 mg ha(-1)) to the landscape on an annual basis. Using the "direct" method of estimating dry deposition (thoughfall + litterfall - open loadings), we calculated that annual dry deposition of THg and MeHg under forest canopies ranged from 105 to 201 mg ha(-1), whereas dry deposition of MeHg ranged from 0.7 to 1.2 mg ha(-1). Photoreduction and emission of wet-deposited Hg(ll) from canopy foliage were accounted for, resulting in 3-5% (5-6 mg ha(-1)) higher annual estimates of dry deposition than via the direct method alone. NetTHg and MeHg loadings to this remote landscape were lower than at any other previously studied forested site globally. This study shows that THg and MeHg loading can be extremely variable within a heterogeneous boreal landscape and that processes such as Hg photoreduction and emission from foliage should be considered when estimating dry deposition of Hg.

Whole-ecosystem study shows rapid fish-mercury response to changes in mercury deposition.

Methylmercury contamination of fisheries from centuries of industrial atmospheric emissions negatively impacts humans and wildlife worldwide. The response of fish methylmercury concentrations to changes in mercury deposition has been difficult to establish because sediments/soils contain large pools of historical contamination, and many factors in addition to deposition affect fish mercury. To test directly the response of fish contamination to changing mercury deposition, we conducted a whole-ecosystem experiment, increasing the mercury load to a lake and its watershed by the addition of enriched stable mercury isotopes. The isotopes allowed us to distinguish between experimentally applied mercury and mercury already present in the ecosystem and to examine bioaccumulation of mercury deposited to different parts of the watershed. Fish methylmercury concentrations responded rapidly to changes in mercury deposition over the first 3 years of study. Essentially all of the increase in fish methylmercury concentrations came from mercury deposited directly to the lake surface. In contrast, <1% of the mercury isotope deposited to the watershed was exported to the lake. Steady state was not reached within 3 years. Lake mercury isotope concentrations were still rising in lake biota, and watershed mercury isotope exports to the lake were increasing slowly. Therefore, we predict that mercury emissions reductions will yield rapid (years) reductions in fish methylmercury concentrations and will yield concomitant reductions in risk. However, a full response will be delayed by the gradual export of mercury stored in watersheds. The rate of response will vary among lakes depending on the relative surface areas of water and watershed.