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J.W.M. Rudd

Publications and source records attributed to J.W.M. Rudd.

4 recordsLinked to original sources

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 × 10 −4 day −1 and 11.6 × 10 −4 day −1 . Average half-life ( t 1/2 ) 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.

Environmental Science & Technology↗

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 wild-life 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.

Proceedings of the National Academy of Sciences of↗

Speciation and transport of newly deposited mercury in a boreal forest wetland: A stable mercury isotope approach

As part of the Mercury Experiment to Assess Atmospheric Loadings in Canada and the United States (METAALICUS) the fate and transport of contemporary mercury (Hg) deposition in a boreal wetland was investigated using an experimentally applied stable mercury isotope. We applied high purity (99.2% ± 0.1) 202 Hg(II) to a wetland plot to determine if (1) the 202 Hg was detectable above the pool of native Hg, (2) the 202 Hg migrated vertically and/or horizontally in peat and pore waters, and (3) the 202 Hg was converted to methylmercury (MeHg) in situ. The 202 Hg was easily detected by ICP/MS in both solid peat and pore waters. Over 3 months, the 202 Hg migrated vertically downward in excess of 15 cm below the water table and traveled several meters horizontally beyond the experimental plot to the lake margin along the dominant vector of groundwater flow. Importantly, at one location, 6% of aqueous 202 Hg was detected as Me 202 Hg after only 1 day. These results indicate that new inorganic Hg in atmospheric deposition can be readily methylated and transported lakeward by shallow groundwater flow, confirming the important role of wetlands as contributors of Hg to aquatic ecosystems.

Water Resources Research↗

Reactivity and mobility of new and old mercury deposition in a boreal forest ecosystem during the first year of the METAALICUS study

The METAALICUS (Mercury Experiment To Assess Atmospheric Loading In Canada and the US) project is a whole ecosystem experiment designed to study the activity, mobility, and availability of atmospherically deposited mercury. To investigate the dynamics of mercury newly deposited onto a terrestrial ecosystem, an enriched stable isotope of mercury ( 202 Hg) was sprayed onto a Boreal forest subcatchment in an experiment that allowed us, for the first time, to monitor the fate of “new” mercury in deposition and to distinguish it from native mercury historically stored in the ecosystem. Newly deposited mercury was more reactive than the native mercury with respect to volatilization and methylation pathways. Mobility through runoff was very low and strongly decreased with time because of a rapid equilibration with the large native pool of “bound” mercury. Over one season, only ∼8% of the added 202 Hg volatilized to the atmosphere and less than 1% appeared in runoff. Within a few months, approximately 66% of the applied 202 Hg remained associated with above ground vegetation, with the rest being incorporated into soils. The fraction of 202 Hg bound to vegetation was much higher than seen for native Hg (<5% vegetation), suggesting that atmospherically derived mercury enters the soil pool with a time delay, after plants senesce and decompose. The initial mobility of mercury received through small rain events or dry deposition decreased markedly in a relatively short time period, suggesting that mercury levels in terrestrial runoff may respond slowly to changes in mercury deposition rates.

Environmental Science & Technology↗