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B.A. Branfireun

Publications and source records attributed to B.A. Branfireun.

4 recordsLinked to original sources

Response of a macrotidal estuary to changes in anthropogenic mercury loading between 1850 and 2000

Methylmercury (MeHg) bioaccumulation in marine food webs poses risks to fish-consuming populations and wildlife. Here we develop and test an estuarine mercury cycling model for a coastal embayment of the Bay of Fundy, Canada. Mass budget calculations reveal that MeHg fluxes into sediments from settling solids exceed losses from sediment-to-water diffusion and resuspension. Although measured methylation rates in benthic sediments are high, rapid demethylation results in negligible net in situ production of MeHg. These results suggest that inflowing fluvial and tidal waters, rather than coastal sediments, are the dominant MeHg sources for pelagic marine food webs in this region. Model simulations show water column MeHg concentrations peaked in the 1960s and declined by almost 40% by the year 2000. Water column MeHg concentrations respond rapidly to changes in mercury inputs, reaching 95% of steady state in approximately 2 months. Thus, MeHg concentrations in pelagic organisms can be expected to respond rapidly to mercury loading reductions achieved through regulatory controls. In contrast MeHg concentrations in sediments have steadily increased since the onset of industrialization despite recent decreases in total mercury loading. Benthic food web MeHg concentrations are likely to continue to increase over the next several decades at present-day mercury emissions levels because the deep active sediment layer in this system contains a large amount of legacy mercury and requires hundreds of years to reach steady state with inputs.

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↗

Application of ultrafiltration and stable isotopic amendments to field studies of mercury partitioning to filterable carbon in lake water and overland runoff

Results from pilot studies on colloidal phase transport of newly deposited mercury in lake water and overland runoff demonstrate that the combination of ultrafiltration, and stable isotope amendment techniques is a viable tool for the study of mercury partitioning to filterable carbon. Ultrafiltration mass balance calculations were generally excellent, averaging 97.3, 96.1 and 99.8% for dissolved organic carbon (DOC), total mercury (Hg T ), and methylmercury (MeHg), respectively. Sub nanogram per liter quantities of isotope were measurable, and the observed phase distribution from replicate ultrafiltration separations on lake water agreed within 20%. We believe the data presented here are the first published colloidal phase mercury data on lake water and overland runoff from uncontaminated sites. Initial results from pilot-scale lake amendment experiments indicate that the choice of matrix used to dissolve the isotope did not affect the initial phase distribution of the added mercury in the lake. In addition there was anecdotal evidence that native MeHg was either recently produced in the system, or at a minimum, that this ‘old’ MeHg partitions to the same subset of DOC that binds the amended mercury. Initial results from pilot-scale overland runoff experiments indicate that less than 20% of newly deposited mercury was transported in the filterable fraction (<0.7 μm). There is some indication of colloidal phase enrichment of mercury in runoff compared to the phase distribution of organic carbon, but the mechanism of this enrichment is unclear. The phase distribution of newly deposited mercury can differ from that of organic carbon and native mercury, suggesting that the quality of the carbon (available ligands), not the quantity of carbon, regulates partitioning. Further characterization of DOC is needed to clarify the underlying mechanisms.

Science of the Total Environment↗