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Michael T. Tate

Publications and source records attributed to Michael T. Tate.

At least 37 records · Page 2Linked to original sources

Decadal trends of mercury cycling and bioaccumulation within Everglades National Park

Mercury (Hg) contamination has been a persistent concern in the Florida Everglades for over three decades due to elevated atmospheric deposition and the system's propensity for methylation and rapid bioaccumulation. Given declines in atmospheric Hg concentrations in the conterminous United States and efforts to mitigate nutrient release to the greater Everglades ecosystem, it was vital to assess how Hg dynamics responded on temporal and spatial scales. This study used a multimedia approach (water and biota) to examine Hg and methylmercury (MeHg) dynamics across a 76-site network within the southernmost portion of the region, Everglades National Park (ENP), from 2008 to 2018. Atmospheric Hg deposition was evaluated over time using a long-term monitoring station. Hg concentrations across matrices showed that air, water, and biota from the system were inextricably linked. Temporal patterns across matrices were driven primarily by hydrologic and climatic changes in the park and no evidence of a decline in atmospheric Hg deposition from 2008 to 2018 was observed, unlike other regions of the United States. In the Shark River Slough (SRS), excess dissolved organic carbon and sulfate were also consistently delivered from upgradient canals and showed no evidence of decline over the study period. Within the SRS a strong positive correlation was observed between MeHg concentrations in surface water and resident fish. Within distinct geographic regions of ENP (SRS, Marsh, Coastal), the geochemical controls on MeHg dynamics differed and highlighted regions susceptible to higher MeHg bioaccumulation, particularly in the SRS and Coastal regions. This study demonstrates the strong influence that dissolved organic carbon and sulfate loads have on spatial and temporal distributions of MeHg across the ENP. Importantly, improved water quality and flow rates are two key restoration targets of the nearly 30-year Everglades restoration program, which if achieved, this study suggests would lead to reduced MeHg production and exposure.

Florida

Surface-air mercury fluxes and a watershed mass balance in forested and harvested catchments

Forest soils are among the world’s largest repositories for long-term accumulation of atmospherically deposited mercury (Hg), and understanding the potential for remobilization through gaseous emissions, aqueous dissolution and runoff, or erosive particulate transport to down-gradient aquatic ecosystems is critically important for projecting ecosystem recovery. Forestry operations, especially clear-cut logging where most of the vegetaiton is removed, can influence Hg mobility/fluxes, foodweb dynamics, and bioaccumulation processes. This paper measured surface-air Hg fluxes from catchments in the Pacific Northwest, USA, to determine if there is a difference between forested and logged catchments. These measurements were conducted as part of a larger project on the impact of forestry operations on Hg cycling which include measurements of water fluxes as well as impacts on biota. Surface-air Hg fluxes were measured using a commonly applied dynamic flux chamber (DFC) method that incorporated diel and seasonal variability in elemental Hg (Hg 0 ) fluxes at multiple forested and harvested catchments. The results showed that the forested ecosystem had depositional Hg 0 fluxes throughout most of the year (annual mean: −0.26 ng/m 2 /h). In contrast, the harvested catchments showed mostly emission of Hg 0 (annual mean: 0.63 ng/m 2 /h). Differences in solar radiation reaching the soil was the primary driver resulting in a shift from net deposition to emission in harvested catchments. The surface-air Hg fluxes were larger than the fluxes to water as runoff and accounted for 97% of the differences in Hg sequestered in forested versus harvested catchments.

Oregon

The influence of legacy contamination on the transport and bioaccumulation of mercury within the Mobile River Basin

Past industrial use and subsequent release of mercury (Hg) into the environment have resulted in severe cases of legacy contamination that still influence contemporary Hg levels in biota. While the bioaccumulation of legacy Hg is commonly assessed via concentration measurements within fish tissue, this practice becomes difficult in regions of high productivity and methylmercury (MeHg) production, like the Mobile River Basin, Alabama in the southeastern United States. This study applied Hg stable isotope tracers to distinguish legacy Hg from regional deposition sources in sediments, waters, and fish within the Mobile River. Sediments and waters displayed differences in δ 202 Hg between industrial and background sites, which corresponded to drastic differences in Hg concentration. Sites that were affected by legacy Hg, as defined by δ 202 Hg, produced largemouth bass with lower MeHg content (59–70%) than those captured in the main rivers (>85%). Direct measurements of Hg isotopes and mathematical estimates of MeHg isotope pools in fish displayed similar distinctions between legacy and watershed sources as observed in other matrices. These results indicate that legacy Hg can accumulate directly into fish tissue as the inorganic species and may also be available for methylation within contaminated zones decades after the initial release.

Alabama

Examining historical mercury sources in the Saint Louis River estuary: How legacy contamination influences biological mercury levels in Great Lakes coastal regions

Industrial chemical contamination within coastal regions of the Great Lakes can pose serious risks to wetland habitat and offshore fisheries, often resulting in fish consumption advisories that directly affect human and wildlife health. Mercury (Hg) is a contaminant of concern in many of these highly urbanized and industrialized coastal regions, one of which is the Saint Louis River estuary (SLRE), the second largest tributary to Lake Superior. The SLRE has legacy Hg contamination that drives high Hg concentrations within sediments, but it is unclear whether legacy-derived Hg actively cycles within the food web. To understand the relative contributions of legacy versus contemporary Hg sources in coastal zones, Hg, carbon, and nitrogen stable isotope ratios were measured in sediments and food webs of SLRE and the Bad River, an estuarine reference site. Hg stable isotope values revealed that legacy contamination of Hg was widespread and heterogeneously distributed in sediments of SLRE, even in areas lacking industrial Hg sources. Similar isotope values were found in benthic invertebrates, riparian spiders, and prey fish from SLRE, confirming legacy Hg reaches the SLRE food web. Direct comparison of prey fish from SLRE and the Bad River confirmed that Hg isotope differences between the sites were not attributable to fractionation associated with rapid Hg bioaccumulation at estuarine mouths, but due to the presence of industrial Hg within SLRE. The Hg stable isotope values of game fish in both estuaries were dependent on fish migration and diet within the estuaries and extending into Lake Superior. These results indicate that Hg from legacy contamination is actively cycling within the SLRE food web and, through migration, this Hg also extends into Lake Superior via game fish. Understanding sources and the movement of Hg within the estuarine food web better informs restoration strategies for other impaired Great Lakes coastal zones.

Minnesota, Wisconsin

Isolation of methylmercury using distillation and anion-exchange chromatography for isotopic analyses in natural matrices

The development of mercury (Hg) stable isotope measurements has enhanced the study of Hg sources and transformations in the environment. As a result of the mixing of inorganic Hg (iHg) and methylmercury (MeHg) species within organisms of the aquatic food web, understanding species-specific Hg stable isotopic compositions is of significant importance. The lack of MeHg isotope measurements is due to the analytical difficulty in the separation of the MeHg from the total Hg pool, with only a few methods having been tested over the past decade with varying degrees of success, and only a handful of environmentally relevant measurements. Here, we present a novel anion-exchange resin separation method using AG 1-X4 that further isolates MeHg from the sample matrix, following a distillation pretreatment, in order to obtain ambient MeHg stable isotopic compositions. This method avoids the use of organic reagents, does not require complex instrumentation, and is applicable across matrices. Separation tests across sediment, water, and biotic matrices showed acceptable recoveries (98 ± 5%, n = 54) and reproducible δ 202 Hg isotope results (2 SDs ≤ 0.15‰) down to 5 ng of MeHg. The measured MeHg pools in natural matrices, such as plankton and sediments, showed large deviations from the non-speciated total Hg measurement, indicating that there is an important isotopic shift during methylation that is not recorded by typical measurements, but is vital in order to assess sources of Hg during bioaccumulation.

Analytical and Bioanalytical Chemistry

Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan

To understand the impact reduced mercury (Hg) loading and invasive species have had on methylmercury bioaccumulation in predator fish of Lake Michigan, we reconstructed bioaccumulation trends from a fish archive (1978 to 2012). By measuring fish Hg stable isotope ratios, we related temporal changes in Hg concentrations to varying Hg sources. Additionally, dietary tracers were necessary to identify food web influences. Through combined Hg, C, and N stable isotopic analyses, we were able to differentiate between a shift in Hg sources to fish and periods when energetic transitions (from dreissenid mussels) led to the assimilation of contrasting Hg pools (2000 to present). In the late 1980s, lake trout δ 202 Hg increased (0.4‰) from regulatory reductions in regional Hg emissions. After 2000, C and N isotopes ratios revealed altered food web pathways, resulting in a benthic energetic shift and changes to Hg bioaccumulation. Continued increases in δ 202 Hg indicate fish are responding to several United States mercury emission mitigation strategies that were initiated circa 1990 and continued through the 2011 promulgation of the Mercury and Air Toxics Standards rule. Unlike archives of sediments, this fish archive tracks Hg sources susceptible to bioaccumulation in Great Lakes fisheries. Analysis reveals that trends in fish Hg concentrations can be substantially affected by shifts in trophic structure and dietary preferences initiated by invasive species in the Great Lakes. This does not diminish the benefits of declining emissions over this period, as fish Hg concentrations would have been higher without these actions.

Lake Michigan

Chemical and physical controls on mercury source signatures in stream fish from the northeastern United States

Streams in the northeastern U.S. receive mercury (Hg) in varying proportions from atmospheric deposition and legacy point sources, making it difficult to attribute shifts in fish concentrations directly back to changes in Hg source management. Mercury stable isotope tracers were utilized to relate sources of Hg to co-located fish and bed sediments from 23 streams across a forested to urban-industrial land-use gradient within this region. Mass-dependent isotopes (δ202Hg) in prey and game fish at forested sites were depleted (medians -0.95 and -0.83 ‰, respectively) in comparison to fish from urban-industrial settings (medians -0.26 and -0.38 ‰, respectively); the forested site group also had higher prey fish Hg concentrations. The separation of Hg isotope signatures in fish was strongly related to in-stream and watershed land-use indicator variables. Fish isotopes were strongly correlated with bed sediment isotopes, but the comparison of isotopic composition between fish and sediment was variable due to differing ecosystem-specific drivers controlling the extent of MeHg formation. The multivariable approach of analyzing watershed characteristics and stream chemistry reveals that the Hg isotope composition in fish is linked to current and historic Hg sources in the northeastern U.S. and can be used to trace bioaccumulated Hg.

Environmental Science & Technology

Rapid pre-concentration of mercury in solids and water for isotopic analysis

The precise quantification of mercury (Hg) stable isotope compositions in low concentration or dilute samples poses analytical challenges due to Hg mass limitations. Common Hg pre-concentration procedures require extended processing times, making rapid Hg stable isotope measurements challenging. Here we present a modified pre-concentration method that combines commonly used Hg reduction and gold trap amalgamation followed by semi-rapid thermal desorption (less than 1 h) and chemical trapping. This custom designed system was demonstrated to perform adequately on multiple trapping matrices including a new bromine monochloride (BrCl) wet oxidant trap (40% 3HNO 3 :BrCl), capable of trapping consistently in 2 mL volume over a wide range of Hg masses (5–200 ng). The procedure was also shown to work effectively on natural matrices, waters and sediments, producing comparable isotope results to the direct digestion analyses. Here, we present a method that can effectively triple sample throughput in comparison to traditional procedures, and also access lower concentration matrices without compromising the accuracy or precision of Hg isotope measurements.

Analytica Chimica Acta

Timber harvest alters mercury bioaccumulation and food web structure in headwater streams

Timber harvest has many effects on aquatic ecosystems, including changes in hydrological, biogeochemical, and ecological processes that can influence mercury (Hg) cycling. Although timber harvest’s influence on aqueous Hg transformation and transport are well studied, the effects on Hg bioaccumulation are not. We evaluated Hg bioaccumulation, biomagnification, and food web structure in 10 paired catchments that were either clear-cut in their entirety, clear-cut except for an 8-m wide riparian buffer, or left unharvested. Average mercury concentrations in aquatic biota from clear-cut catchments were 50% higher than in reference catchments and 165% higher than in catchments with a riparian buffer. Mercury concentrations in aquatic invertebrates and salamanders were not correlated with aqueous THg or MeHg concentrations, but rather treatment effects appeared to correspond with differences in the utilization of terrestrial and aquatic basal resources in the stream food webs. Carbon and nitrogen isotope data suggest that a diminished shredder niche in the clear-cut catchments contributed to lower basal resource diversity compared with the reference of buffered treatments, and that elevated Hg concentrations in the clear-cut catchments reflect an increased reliance on aquatic resources in clear-cut catchments. In contrast, catchments with riparian buffers had higher basal resource diversity than the reference catchments, indicative of more balanced utilization of terrestrial and aquatic resources. Further, following timber harvest THg concentrations in riparian songbirds were elevated, suggesting an influence of timber harvest on Hg export to riparian food webs. These data, coupled with comparisons of individual feeding guilds, indicate that changes in organic matter sources and associated effects on stream food web structure are important mechanisms by which timber harvest modifies Hg bioaccumulation in headwater streams and riparian consumers.

Oregon

Factors affecting mercury stable isotopic distribution in piscivorous fish of the Laurentian Great Lakes

Identifying the sources of methylmercury (MeHg) and tracing the transformations of mercury (Hg) in the aquatic food web are important components of effective strategies for managing current and legacy Hg sources. In our previous work, we measured stable isotopes of Hg (δ 202 Hg, Δ 199 Hg, and Δ 200 Hg) in the Laurentian Great Lakes and estimated source contributions of Hg to bottom sediment. Here, we identify isotopically distinct Hg signatures for Great Lakes trout ( Salvelinus namaycush ) and walleye ( Sander vitreus ), driven by both food-web and water-quality characteristics. Fish contain high values for odd-isotope mass independent fractionation (MIF) with averages ranging from 2.50 (western Lake Erie) to 6.18‰ (Lake Superior) in Δ 199 Hg. The large range in odd-MIF reflects variability in the depth of the euphotic zone, where Hg is most likely incorporated into the food web. Even-isotope MIF (Δ 200 Hg), a potential tracer for Hg from precipitation, appears both disconnected from lake sedimentary sources and comparable in fish among the five lakes. We suggest that similar to the open ocean, water-column methylation also occurs in the Great Lakes, possibly transforming recently deposited atmospheric Hg deposition. We conclude that the degree of photochemical processing of Hg is controlled by phytoplankton uptake rather than by dissolved organic carbon quantity among lakes.

Environmental Science & Technology

Stream mercury export in response to contemporary timber harvesting methods (Pacific Coastal Mountains, Oregon, USA)

Land-use activities can alter hydrological and biogeochemical processes that can affect the fate, transformation, and transport of mercury (Hg). Previous studies in boreal forests have shown that forestry operations can have profound, but variable effects on Hg export and methylmercury (MeHg) formation. The Pacific Northwest is an important timber producing region that receives large atmospheric Hg loads, but the impact of forest harvesting on Hg mobilization has not been directly studied and was the focus of our investigation. Stream discharge was measured continuously and Hg and MeHg concentrations measured monthly for 1.5 years following logging in three paired harvested and un-harvested catchments. There was no significant difference in particulate-bound Hg concentrations or loads in the harvested and unharvested catchments which may have resulted from the best management practices aimed at minimizing erosion. However, the harvested catchments had significantly higher discharge (32%), filtered Hg concentrations (28%), filtered Hg loads (80%), and dissolved organic carbon (DOC) loads (40%) compared to forested catchments. MeHg concentrations were low (mostly <0.05 ng L-1) in both harvested, un-harvested and downstream samples due to well-drained/unsaturated soil conditions and steep slopes with high energy eroding stream channels that were not conducive to the development of anoxic conditions. These results have important implications for the role forestry operations have in affecting catchment retention and export of Hg pollution.

Oregon

Assessing potential health risks to fish and humans using mercury concentrations in inland fish from across western Canada and the United States

Fish represent high quality protein and nutrient sources, but Hg contamination is ubiquitous in aquatic ecosystems and can pose health risks to fish and their consumers. Potential health risks posed to fish and humans by Hg contamination in fish were assessed in western Canada and the United States. A large compilation of inland fish Hg concentrations was evaluated in terms of potential health risk to the fish themselves, health risk to predatory fish that consume Hg contaminated fish, and to humans that consume Hg contaminated fish. The probability that a fish collected from a given location would exceed a Hg concentration benchmark relevant to a health risk was calculated. These exceedance probabilities and their associated uncertainties were characterized for fish of multiple size classes at multiple health-relevant benchmarks. The approach was novel and allowed for the assessment of the potential for deleterious health effects in fish and humans associated with Hg contamination in fish across this broad study area. Exceedance probabilities were relatively common at low Hg concentration benchmarks, particularly for fish in larger size classes. Specifically, median exceedances for the largest size classes of fish evaluated at the lowest Hg concentration benchmarks were 0.73 (potential health risks to fish themselves), 0.90 (potential health risk to predatory fish that consume Hg contaminated fish), and 0.97 (potential for restricted fish consumption by humans), but diminished to essentially zero at the highest benchmarks and smallest fish size classes. Exceedances of benchmarks are likely to have deleterious health effects on fish and limit recommended amounts of fish humans consume in western Canada and the United States. Results presented here are not intended to subvert or replace local fish Hg data or consumption advice, but provide a basis for identifying areas of potential health risk and developing more focused future research and monitoring efforts.

Science of the Total Environment

Mercury and methylmercury in aquatic sediment across western North America

Large-scale assessments are valuable in identifying primary factors controlling total mercury (THg) and monomethyl mercury (MeHg) concentrations, and distribution in aquatic ecosystems. Bed sediment THg and MeHg concentrations were compiled for > 16,000 samples collected from aquatic habitats throughout the West between 1965 and 2013. The influence of aquatic feature type (canals, estuaries, lakes, and streams), and environmental setting (agriculture, forest, open-water, range, wetland, and urban) on THg and MeHg concentrations was examined. THg concentrations were highest in lake (29.3 ± 6.5 μg kg − 1 ) and canal (28.6 ± 6.9 μg kg − 1 ) sites, and lowest in stream (20.7 ± 4.6 μg kg − 1 ) and estuarine (23.6 ± 5.6 μg kg − 1 ) sites, which was partially a result of differences in grain size related to hydrologic gradients. By environmental setting, open-water (36.8 ± 2.2 μg kg − 1 ) and forested (32.0 ± 2.7 μg kg − 1 ) sites generally had the highest THg concentrations, followed by wetland sites (28.9 ± 1.7 μg kg − 1 ), rangeland (25.5 ± 1.5 μg kg − 1 ), agriculture (23.4 ± 2.0 μg kg − 1 ), and urban (22.7 ± 2.1 μg kg − 1 ) sites. MeHg concentrations also were highest in lakes (0.55 ± 0.05 μg kg − 1 ) and canals (0.54 ± 0.11 μg kg − 1 ), but, in contrast to THg, MeHg concentrations were lowest in open-water sites (0.22 ± 0.03 μg kg − 1 ). The median percent MeHg (relative to THg) for the western region was 0.7%, indicating an overall low methylation efficiency; however, a significant subset of data (n > 100) had percentages that represent elevated methylation efficiency (> 6%). MeHg concentrations were weakly correlated with THg (r 2 = 0.25) across western North America. Overall, these results highlight the large spatial variability in sediment THg and MeHg concentrations throughout western North America and underscore the important roles that landscape and land-use characteristics have on the MeHg cycle.

Science of the Total Environment

Reservoirs and water management influence fish mercury concentrations in the western United States and Canada

Anthropogenic manipulation of aquatic habitats can profoundly alter mercury (Hg) cycling and bioaccumulation. The impoundment of fluvial systems is among the most common habitat manipulations and is known to increase fish Hg concentrations immediately following impoundment. However, it is not well understood how Hg concentrations differ between reservoirs and lakes at large spatial and temporal scales or how reservoir management influences fish Hg concentrations. This study evaluated total Hg (THg) concentrations in 64,386 fish from 883 reservoirs and 1387 lakes, across the western United States and Canada, to assess differences between reservoirs and lakes, as well as the influence of reservoir management on fish THg concentrations. Fish THg concentrations were 1.4-fold higher in reservoirs (0.13 &plusmn; 0.011 &mu;g/g wet weight &plusmn; standard error) than lakes (0.09 &plusmn; 0.006), though this difference varied among ecoregions. Fish THg concentrations were 1.5- to 2.6-fold higher in reservoirs than lakes of the North American Deserts, Northern Forests, and Mediterranean California ecoregions, but did not differ between reservoirs and lakes in four other ecoregions. Fish THg concentrations peaked in three-year-old reservoirs then rapidly declined in 4&ndash;12 year old reservoirs. Water management was particularly important in influencing fish THg concentrations, which were up to 11-times higher in reservoirs with minimum water storage occurring in May, June, or July compared to reservoirs with minimum storage occurring in other months. Between-year changes in maximum water storage strongly influenced fish THg concentrations, but within-year fluctuations in water levels did not influence fish THg concentrations. Specifically, fish THg concentrations increased up to 3.2-fold over the range of between-year changes in maximum water storage in all ecoregions except Mediterranean California. These data highlight the role of reservoir creation and management in influencing fish THg concentrations and suggest that water management may provide an effective means of mitigating Hg bioaccumulation in some reservoirs.

Science of the Total Environment

Spatial and temporal patterns of mercury concentrations in freshwater fish across the Western United States and Canada

Methylmercury contamination of fish is a global threat to environmental health. Mercury (Hg) monitoring programs are valuable for generating data that can be compiled for spatially broad syntheses to identify emergent ecosystem properties that influence fish Hg bioaccumulation. Fish total Hg (THg) concentrations were evaluated across the Western United States (US) and Canada, a region defined by extreme gradients in habitat structure and water management. A database was compiled with THg concentrations in 96,310 fish that comprised 206 species from 4262 locations, and used to evaluate the spatial distribution of fish THg across the region and effects of species, foraging guilds, habitats, and ecoregions. Areas of elevated THg exposure were identified by developing a relativized estimate of fish mercury concentrations at a watershed scale that accounted for the variability associated with fish species, fish size, and site effects. THg concentrations in fish muscle ranged between 0.001 and 28.4 (&mu;g/g wet weight (ww)) with a geometric mean of 0.17. Overall, 30% of individual fish samples and 17% of means by location exceeded the 0.30 &mu;g/g ww US EPA fish tissue criterion. Fish THg concentrations differed among habitat types, with riverine habitats consistently higher than lacustrine habitats. Importantly, fish THg concentrations were not correlated with sediment THg concentrations at a watershed scale, but were weakly correlated with sediment MeHg concentrations, suggesting that factors influencing MeHg production may be more important than inorganic Hg loading for determining fish MeHg exposure. There was large heterogeneity in fish THg concentrations across the landscape; THg concentrations were generally higher in semi-arid and arid regions such as the Great Basin and Desert Southwest, than in temperate forests. Results suggest that fish mercury exposure is widespread throughout Western US and Canada, and that species, habitat type, and region play an important role in influencing ecological risk of mercury in aquatic ecosystems.

Science of the Total Environment

Atmospheric mercury and fine particulate matter in coastal New England: implications for mercury and trace element sources in the northeastern United States

Intensive sampling of ambient atmospheric fine particulate matter was conducted at Woods Hole, Massachusetts over a four-month period from 3 April to 29 July, 2008, in conjunction with year-long deployment of the USGS Mobile Mercury Lab. Results were obtained for trace elements in fine particulate matter concurrently with determination of ambient atmospheric mercury speciation and concentrations of ancillary gasses (SO 2 , NO x , and O 3 ). For particulate matter, trace element enrichment factors greater than 10 relative to crustal background values were found for As, Bi, Cd, Cu, Hg, Pb, Sb, V, and Zn, indicating contribution of these elements by anthropogenic sources. For other elements, enrichments are consistent with natural marine (Na, Ca, Mg, Sr) or crustal (Ba, Ce, Co, Cs, Fe, Ga, La, Rb, Sc, Th, Ti, U, Y) sources, respectively. Positive matrix factorization was used together with concentration weighted air-mass back trajectories to better define element sources and their locations. Our analysis, based on events exhibiting the 10% highest PM 2.5 contributions for each source category, identifies coal-fired power stations concentrated in the U.S. Ohio Valley, metal smelting in eastern Canada, and marine and crustal sources showing surprisingly similar back trajectories, at times each sampling Atlantic coastal airsheds. This pattern is consistent with contribution of Saharan dust by a summer maximum at the latitude of Florida and northward transport up the Atlantic Coast by clockwise circulation of the summer Bermuda High. Results for mercury speciation show diurnal production of RGM by photochemical oxidation of Hg° in a marine environment, and periodic traverse of the study area by correlated RGM-SO 2 (NO x ) plumes, indicative of coal combustion sources.

Massachusetts

Comparison of atmospheric mercury speciation and deposition at nine sites across central and eastern North America

This study presents >5 cumulative years of tropospheric mercury (Hg) speciation measurements, over the period of 2003–2009, for eight sites in the central and eastern United States and one site in coastal Puerto Rico. The purpose of this research was to identify local and regional processes that impact Hg speciation and deposition (wet + dry) across a large swath of North America. Sites sampled were selected to represent both a wide range of mercury exposure and environmental conditions. Seasonal mean concentrations of elemental Hg (1.27 ± 0.31 to 2.94 ± 1.57 ng m−3; x ± s), reactive gaseous mercury (RGM; 1.5 ± 1.6 to 63.3 ± 529 pg m−3), and fine particulate Hg (1.2 ± 1.4 to 37.9 ± 492 pg m−3) were greatest at sites impacted by Hg point sources. Diel bin plots of Hgo and RGM suggest control by a variety of local/regional processes including impacts from Hg point sources and boundary layer/free tropospheric interactions as well as from larger‐scale processes affecting Hg speciation (i.e., input of the global Hg pool, RGM formed from oxidation of Hgo by photochemical compounds at coastal sites, and elemental Hg depletion during periods of dew formation). Comparison of wet Hg deposition (measured), RGM and fine particulate Hg dry deposition (calculated using a multiple resistance model), and anthropogenic point source emissions varied significantly between sites. Significant correlation between emission sources and dry deposition was observed but was highly dependant upon inclusion of data from two sites with exceptionally high deposition. Findings from this study highlight the importance of environmental setting on atmospheric Hg cycling and deposition rates.

Journal of Geophysical Research