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J.M. Benoit

Publications and source records attributed to J.M. Benoit.

3 recordsLinked to original sources

Constants for mercury binding by organic matter isolates from the Florida Everglades

Dissolved organic matter (DOM) has been implicated as an important complexing agent for Hg that can affect its mobility and bioavailability in aquatic ecosystems. However, binding constants for natural Hg-DOM complexes are not well known. We employed a competitive ligand approach to estimate conditional stability constants for Hg complexes with DOM isolates collected from Florida Everglades surface waters. The isolates examined were the hydrophobic fraction of DOM from a eutrophic, sulfidic site (F1-HPoA) and the hydrophilic fraction from an oligotrophic, low-sulfide site (2BS-HPiA). Our experimental determinations utilized overall octanol-water partitioning coefficients (D ow ) for 203 Hg at 0.01 M chloride and across pH and DOM concentration gradients. Use of this radioisotope allowed rapid determinations of Hg concentrations in both water and octanol phases without problems of matrix interference. Conditional stability constants (I = 0.06, 23°C) were log K′ = 11.8 for F1-HPoA and log K′ = 10.6 for 2BS-HPiA. These are similar to previously published stability constants for Hg binding to low-molecular-weight thiols. Further, F1-HPoA showed a pH-dependent decline in D ow that was consistent with models of Hg complexation with thiol groups as the dominant Hg binding sites in DOM. These experiments demonstrate that the DOM isolates are stronger ligands for Hg than chloride ion or ethylenediamine-tetraacetic acid. Speciation calculations indicate that at the DOM concentrations frequently measured in Everglades, 20 to 40 μM, significant complexation of Hg by DOM would be expected in aerobic (sulfide-free) surface waters.

Florida↗

Methyl mercury dynamics in littoral sediments of a temperate seepage lake

The sites and rates of methyl mercury (MeHg) production and transport in littoral zone sediments were investigated at Pallette Lake in northern Wisconsin. In littoral areas where groundwater inflow occurs, sulfate supply from groundwater creates profiles of electron acceptors (sulfate) and donors (methane, sulfide) that are reversed from those found in sediments whose sulfate supply is delivered from overlying water. The highest MeHg concentrations in porewaters and the maximal advective MeHg flux rates (4.5-61.7 ng ·m -2 ·day -1 ) were observed in the spring, while highest bulk phase concentrations occur later in the summer. These estimated MeHg fluxes are greater than the mean areal production rates estimated previously for the water column and are similar to the atmospheric flux. Gross MeHg production was measured using the addition of 203 Hg as a tracer to sediments. The depth at which maximal 203 Hg methylation occurred coincided with the observed maximums in solid-phase and porewater MeHg concentrations. Because input, advection, and accumulation of MeHg in these sediments were measured directly, an independent estimate of MeHg production could be made and compared with 203 Hg-derived rates. This comparison suggests that that the 203 Hg tracer method provides reasonable estimates of gross methylation rates and that a substantial fraction of solid-phase Hg is available for methylation

Canadian Journal of Fisheries and Aquatic Sciences↗

Mercury cycling in the Allequash Creek watershed, northern Wisconsin

Although there have been recent significant gains in our understanding of mercury (Hg) cycling in aquatic environments, few studies have addressed Hg cycling on a watershed scale in particular, attention to Hg species transfer between watershed components (upland soils, groundwater, wetlands, streams, and lakes) has been lacking. This study describes spatial and temporal distributions of total Hg and MeHg among watershed components of the Allequash Creek watershed (northern Wisconsin, USA). Substantial increases in total Hg and MeHg were observed as groundwater discharged through peat to form springs that flow into the stream, or rivulets that drain across the surface of the wetland. This increase was concomitant with increases in DOC. During fall, when the Allequash Creek wetland released a substantial amount of DOC to the stream, a 23 fold increase in total Hg concentrations was observed along the entire length of the stream. Methylmercury, however, did not show a similar response. Substantial variability was observed in total Hg (0.9 to 6.3) and MeHg (<0.02 to 0.33) concentrations during synoptic surveys of the entire creek. For the Allequash Creek watershed, the contributing groundwater basin is about 50% larger than the topographic drainage basin. Total Hg concentrations in groundwater, the area of the groundwater basin, and annual stream flow data give a watershed-yield rate of 12 mg/km2/d, which equates to a retention rate of 96%. The calculated MeHg yield rate for the wetland area is 0.6 to 1.5 mg/km2/d, a value that is 3-6 fold greater than the atmospheric deposition rate.

Water, Air, & Soil Pollution↗