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J.A. Graydon

Publications and source records attributed to J.A. Graydon.

4 recordsLinked to original sources

Estimation of speciated and total mercury dry deposition at monitoring locations in eastern and central North America

Dry deposition of speciated mercury, i.e., gaseous oxidized mercury (GOM), particulate-bound mercury (PBM), and gaseous elemental mercury (GEM), was estimated for the year 2008–2009 at 19 monitoring locations in eastern and central North America. Dry deposition estimates were obtained by combining monitored two- to four-hourly speciated ambient concentrations with modeled hourly dry deposition velocities (V d ) calculated using forecasted meteorology. Annual dry deposition of GOM+PBM was estimated to be in the range of 0.4 to 8.1 μg m −2 at these locations with GOM deposition being mostly five to ten times higher than PBM deposition, due to their different modeled V d values. Net annual GEM dry deposition was estimated to be in the range of 5 to 26 μg m −2 at 18 sites and 33 μg m −2 at one site. The estimated dry deposition agrees very well with limited surrogate-surface dry deposition measurements of GOM and PBM, and also agrees with litterfall mercury measurements conducted at multiple locations in eastern and central North America. This study suggests that GEM contributes much more than GOM+PBM to the total dry deposition at the majority of the sites considered here; the only exception is at locations close to significant point sources where GEM and GOM+PBM contribute equally to the total dry deposition. The relative magnitude of the speciated dry deposition and their good comparisons with litterfall deposition suggest that mercury in litterfall originates primarily from GEM, which is consistent with the limited number of previous field studies. The study also supports previous analyses suggesting that total dry deposition of mercury is equal to, if not more important than, wet deposition of mercury on a regional scale in eastern North America.

Piney Reservoir;Beltsville;Grand Bay Nerr;Thompson↗

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↗

Investigation of mercury exchange between forest canopy vegetation and the atmosphere using a new dynamic chamber

This paper presents the design of a dynamic chamber system that allows full transmission of PAR and UV radiation and permits enclosed intact foliage to maintain normal physiological function while Hg(0) flux rates are quantified in the field. Black spruce and jack pine foliage both emitted and absorbed Hg(0), exhibiting compensation points near atmospheric Hg(0) concentrations of ∼2−3 ng m - 3 . Using enriched stable Hg isotope spikes, patterns of spike Hg(II) retention on foliage were investigated. Hg(0) evasion rates from foliage were simultaneously measured using the chamber to determine if the decline of foliar spike Hg(II) concentrations over time could be explained by the photoreduction and re-emission of spike Hg to the atmosphere. This mass balance approach suggested that spike Hg(0) fluxes alone could not account for the measured decrease in spike Hg(II) on foliage following application, implying that either the chamber underestimates the true photoreduction of Hg(II) to Hg(0) on foliage, or other mechanisms of Hg(II) loss from foliage, such as cuticle weathering, are in effect. The radiation spectrum responsible for the photoreduction of newly deposited Hg(II) on foliage was also investigated. Our spike experiments suggest that some of the Hg(II) in wet deposition retained by the forest canopy may be rapidly photoreduced to Hg(0) and re-emitted back to the atmosphere, while another portion may be retained by foliage at the end of the growing season, with some being deposited in litterfall. This finding has implications for the estimation of Hg dry deposition based on throughfall and litterfall fluxes.

Environmental Science & Technology↗