Resolving Atmospheric Mercury Loading and Source Trends from Isotopic Records of Remote North American Lake Sediments.

The strongest evidence for anthropogenic alterations to the global mercury (Hg) cycle comes from historical records of mercury deposition preserved in lake sediments. Hg isotopes have added a new dimension to these sedimentary archives, promising additional insights into Hg source apportionment and biogeochemical processing. Presently, most interpretations of historical changes are constrained to a small number of locally contaminated ecosystems.

Global and Local Sources of Mercury Deposition in Coastal New England Reconstructed from a Multiproxy, High-Resolution, Estuarine Sediment Record.

Historical reconstruction of mercury (Hg) accumulation in natural archives, especially lake sediments, has been essential to understanding human perturbation of the global Hg cycle. Here we present a high-resolution chronology of Hg accumulation between 1727 and 1996 in a varved sediment core from the Pettaquamscutt River Estuary (PRE), Rhode Island. Mercury accumulation is examined relative to (1) historic deposition of polycyclic aromatic hydrocarbons (PAHs) and lead (Pb) and its isotopes (Pb/Pb) in the same core, and (2) other reconstructions of Hg deposition in urban and remote settings.

Spatiotemporal patterns of mercury accumulation in lake sediments of western North America.

For the Western North America Mercury Synthesis, we compiled mercury records from 165 dated sediment cores from 138 natural lakes across western North America. Lake sediments are accepted as faithful recorders of historical mercury accumulation rates, and regional and sub-regional temporal and spatial trends were analyzed with descriptive and inferential statistics. Mercury accumulation rates in sediments have increased, on average, four times (4×) from 1850 to 2000 and continue to increase by approximately 0.

Atmospheric Hg emissions from preindustrial gold and silver extraction in the Americas: a reevaluation from lake-sediment archives.

Human activities over the last several centuries have transferred vast quantities of mercury (Hg) from deep geologic stores to actively cycling earth-surface reservoirs, increasing atmospheric Hg deposition worldwide. Understanding the magnitude and fate of these releases is critical to predicting how rates of atmospheric Hg deposition will respond to future emission reductions. The most recently compiled global inventories of integrated (all-time) anthropogenic Hg releases are dominated by atmospheric emissions from preindustrial gold/silver mining in the Americas.

Methylmercury accumulation in plankton on the continental margin of the northwest Atlantic Ocean.

Accumulation of monomethylmercury (MMHg) by plankton is a key process influencing concentrations of this toxic mercury species in marine food webs and seafood. We examined bioaccumulation and biomagnification of MMHg in microseston and four size fractions of zooplankton on the continental shelf, slope, and rise of the northwest Atlantic Ocean. The bioaccumulation factor (BAF, L/kg) for MMHg in microseston averaged 10(4.

Apportioning global and non-global components of mercury deposition through (210)Pb indexing.

Our previous work has documented a correlation between Hg concentrations and (210)Pb activity measured in wet deposition that might be used to help apportion sources of Hg in precipitation. Here we present the results of a 27-month precipitation collection effort using co-located samplers for Hg and (210)Pb designed to assess this hypothesis. Study sites were located on the east and west coasts of North America, in the continental interior, and on the Florida Peninsula.

Mercury biogeochemical cycling in the ocean and policy implications.

Anthropogenic activities have enriched mercury in the biosphere by at least a factor of three, leading to increases in total mercury (Hg) in the surface ocean. However, the impacts on ocean fish and associated trends in human exposure as a result of such changes are less clear. Here we review our understanding of global mass budgets for both inorganic and methylated Hg species in ocean seawater.

Iron-mediated photochemical decomposition of methylmercury in an arctic Alaskan lake.

Sunlight-induced decomposition is the principal sink for methylmercury (CH(3)Hg(+)) in arctic Alaskan lakes and reduces its availability for accumulation in aquatic food webs. However, the mechanistic chemistry of this process in natural waters is unknown. We examined experimentally the mechanism of photochemical CH(3)Hg(+) decomposition in filter-sterilized epilimnetic waters of Toolik Lake in arctic Alaska (68 degrees 38'N, 149 degrees 36'W), a region illuminated by sunlight almost continuously during the summer.

Methylmercury in freshwater fish linked to atmospheric mercury deposition.

A connection between accumulation of methylmercury (MeHg) in wild fish populations and atmospheric mercury deposition has not been made. Large databases for both MeHg in fish and atmospheric mercury deposition have been assimilated from monitoring efforts spanning the contiguous United States. Here, we compare results of these data sets and show that state-wide average concentrations of MeHg in a cosmopolitan freshwater fish, the largemouth bass Micropterus salmoides, are related positively to wet atmospheric Hg fluxes among most of the 25 states that are analyzed, which span a 5-fold range in Hg deposition.

Bioaccumulation and trophic transfer of methylmercury in Long Island Sound.

Humans are exposed to methylmercury (MeHg) principally by consumption of marine fish. The coastal zone supports the majority of marine fish production, and may therefore be an important source of MeHg to humans; however, little is known about the bioaccumulation of MeHg in near-shore marine ecosystems. We examined MeHg in microseston, zooplankton, a decapod crustacean, and four representative species of finfish that differ in trophic status and/or prey selection in Long Island Sound (LIS), a large coastal embayment in the northeastern United States.

Photodecomposition of methylmercury in an Arctic Alaskan lake.

Sunlight-induced decomposition of monomethylmercury (MMHg) reduces its availability for accumulation in aquatic food webs. We examined MMHg degradation in epilimnetic waters of Toolik Lake (68 degrees 38' N, 149 degrees 36' W) in arctic Alaska, a region illuminated by sunlight almost continuously during the summer. MMHg decomposition in surface water of Toolik Lake is exclusively abiotic and mediated by sunlight; comparable rates of MMHg decomposition were observed in filter-sterilized and unfiltered surface waters incubated under in situ sunlight and temperature conditions, and no MMHg was degraded in unfiltered aliquots incubated in the dark.

Biogeochemical cycling of methylmercury in lakes and tundra watersheds of Arctic Alaska.

The fate of atmospherically deposited and environmentally active Hg is uncertain in the Arctic, and of greatest toxicological concern is the transformation to monometh-ylmercury (MMHg). Lake/watershed mass balances were developed to examine MMHg cycling in four northern Alaska lakes near the ecological research station at Toolik Lake (68 degrees 38' N, 149 degrees 36' W). Primary features of the cycle are watershed runoff, sedimentary production and mobilization, burial, and photodecomposition in the water column.

Methylmercury in mosquitoes related to atmospheric mercury deposition and contamination.

A connection between loadings of inorganic Hg, especially from the atmosphere, and accumulation of methylmercury (MeHg) in aquatic biota has not been firmly established. Mosquitoes (Diptera: Culicidae) may be a useful indictor of Hg contamination or MeHg accumulation in aquatic ecosystems because they have aquatic life stages, and their ubiquitous distribution permits sampling across wide ranges of climate, biological productivity, and atmospheric Hg deposition. We examined MeHg in adult mosquitoes from subtropical (Florida), maritime (California), continental (Michigan), and arctic (Alaska) regions of North America that span a range in wet atmospheric Hg deposition (1.

Modern and historic atmospheric mercury fluxes in northern Alaska: Global sources and Arctic depletion.

We reconstruct from lake-sediment archives atmospheric Hg deposition to Arctic Alaska over the last several centuries and constrain a contemporary lake/watershed mass-balance with real-time measurement of Hg fluxes in rainfall, runoff, and evasion. Results indicate that (a) anthropogenic Hg impact in the Arctic is of similar magnitude to that at temperate latitudes; (b) whole-lake Hg sedimentation determined from 55 210Pb-dated cores from the five small lakes demonstrates a 3-fold increase in atmospheric Hg deposition since the advent of the Industrial Revolution; (c) because of high soil Hg concentrations and relatively low atmospheric deposition fluxes, erosional inputs to these lakes are more significant than in similar temperate systems; (d) volatilization accounts for about 20% of the Hg losses (evasion and sedimentation); and (e) another source term is needed to balance the evasional and sedimentation sinks. This additional flux (1.

Determination of methylmercury in environmental matrixes by on-line flow injection and atomic fluorescence spectrometry.

The precision and bias of monomethylmercury (MMHg) determinations in environmental samples can be improved by directly coupling and automating the numerous steps involved with analysis of this toxic Hg species. We developed a simple and robust mercury speciation analyzer (MSA) for measurement of MMHg in environmental matrixes. This on-line hyphenated system couples the main analytical steps, including sample introduction, aqueous-phase ethylation, Tenax preconcentration, and gas chromatographic separation, to cold vapor atomic fluorescence detection and data acquisition.

Geochemical controls on the production and distribution of methylmercury in near-shore marine sediments.

We examined temporal differences in sedimentary production of monomethylmercury (MMHg) at three sites in Long Island Sound (LIS). Sediment-phase concentrations of Hg species decreased from west to east in LIS surface sediments, following the trend of organic matter. However, Hg methylation potentials, measured by incubation with an isotopic tracer (200Hg), increased from west to east.

Determination of the mercury complexation characteristics of dissolved organic matter in natural waters with "reducible Hg" titrations.

A new method for the determination of the concentration and conditional stability constant of dissolved organic matter that binds mercury (Hg) has been developed using an in vitro assay of reducible Hg. The technique is a wet chemical analogue to electrochemical approaches now in use for ligand studies of many other trace transition metals in natural waters. Ligand characteristics are obtained from additions of ionic Hg to buffered lake, river water, and seawater and determination of the wet chemically reducible fraction following equilibration of the spike.