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Martin R. Risch

Publications and source records attributed to Martin R. Risch.

At least 19 recordsLinked to original sources

Spatial patterns and temporal changes in atmospheric-mercury deposition for the midwestern USA, 2001–2016

Spatial patterns and temporal changes in atmospheric-mercury (Hg) deposition were examined in a five-state study area in the Midwestern USA where 32% of the stationary sources of anthropogenic Hg emissions in the continental USA were located. An extensive monitoring record for wet and dry Hg deposition was compiled for 2001–2016, including 4666 weekly precipitation samples at 13 sites and 27 annual litterfall-Hg samples at 7 sites. This study is the first to examine these Hg data for the Midwestern USA. The median annual precipitation-Hg deposition at the study sites was 10.4 micrograms per square meter per year (ug/m2/year) and ranged from 5.8 ug/m2/year to 15.0 ug/m2/year. The median annual Hg concentration was 9.4 ng/L. Annual litterfall-Hg deposition had a median of 16.1 ug/m2/year and ranged from 9.7 to 23.4 ug/m2/year. Isopleth maps of annual precipitation-Hg deposition indicated a recurring spatial pattern similar to one revealed by statistical analysis of weekly precipitation-Hg deposition. In that pattern, high Hg deposition in southeastern Indiana was present each year, frequently extending to southern Illinois. Most of central Indiana and central Illinois had similar Hg deposition. Areas with comparatively lower annual Hg deposition were observed in Michigan and Ohio for many years and frequently included part of northern Indiana. The area in southern Indiana where high Hg deposition predominated had the highest number of extreme episodes of weekly Hg deposition delivering up to 15% of the annual Hg load from precipitation in a single week. Modeled 48-h back trajectories indicated air masses for these episodes often arrived from the south and southwest, crossing numerous stationary sources of Hg emissions releasing from 23 to more than 300 kg Hg per year. This analysis suggests that local and regional, rather than exclusively continental or global Hg emissions were likely contributing to the extreme episodes and at least in part, to the spatial patterns of precipitation-Hg deposition in the study area. Statistically significant temporal decreases in weekly precipitation-Hg concentrations in the study area between the periods 2001–2013 and 2014–2016 were observed, coinciding with reported reductions in Hg emissions in the USA required by implementation of national Hg emissions-control rules. These decreases in atmospheric-Hg concentrations are believed to have resulted in the reduced atmospheric-Hg deposition recorded because precipitation depths between the two periods were not significantly different. The Hg-monitoring data for the study area identified an atmospheric deposition response to decreased local and regional Hg emissions.

Illinois, Indiana, Kentucky, Michigan, Ohio

Atmospheric deposition to forests in the eastern USA

Atmospheric mercury (Hg) deposition to forests is important because half of the land cover in the eastern USA is forest. Mercury was measured in autumn litterfall and weekly precipitation samples at a total of 27 National Atmospheric Deposition Program (NADP) monitoring sites in deciduous and mixed deciduous-coniferous forests in 16 states in the eastern USA during 2007–2014. These simultaneous, uniform, repeated, annual measurements of forest Hg include the broadest area and longest time frame to date. The autumn litterfall-Hg concentrations and litterfall mass at the study sites each year were combined with annual precipitation-Hg data. Rates of litterfall-Hg deposition were higher than or equal to precipitation-Hg deposition rates in 70% of the annual data, which indicates a substantial contribution from litterfall to total atmospheric-Hg deposition. Annual litterfall-Hg deposition in this study had a median of 11.7 μg per square meter per year (μg/m 2 /yr) and ranged from 2.2 to 23.4 μg/m 2 /yr. It closely matched modeled dry-Hg deposition, based on land cover at selected NADP Hg-monitoring sites. Mean annual atmospheric-Hg deposition at forest study sites exhibited a spatial pattern partly explained by statistical differences among five forest-cover types and related to the mapped density of Hg emissions. Forest canopies apparently recorded changes in atmospheric-Hg concentrations over time because litterfall-Hg concentrations decreased year to year and litterfall-Hg concentrations were significantly higher in 2007–2009 than in 2012–2014. These findings reinforce reported decreases in Hg emissions and atmospheric elemental-Hg concentrations during this same time period. Methylmercury (MeHg) was detected in all litterfall samples at all sites, compared with MeHg detections in less than half the precipitation samples at selected sites during the study. These results indicate MeHg in litterfall is a pathway into the terrestrial food web where it can accumulate in the prey of songbirds, bats, and raptors.

Environmental Pollution

The estimated six-year mercury dry deposition across North America

Dry deposition of atmospheric mercury (Hg) to various land covers surrounding 24 sites in North America was estimated for the years 2009 to 2014. Depending on location, multiyear mean annual Hg dry deposition was estimated to range from 5.1 to 23.8 μg m –2 yr –1 to forested canopies, 2.6 to 20.8 μg m –2 yr –1 to nonforest vegetated canopies, 2.4 to 11.2 μg m –2 yr –1 to urban and built up land covers, and 1.0 to 3.2 μg m –2 yr –1 to water surfaces. In the rural or remote environment in North America, annual Hg dry deposition to vegetated surfaces is dominated by leaf uptake of gaseous elemental mercury (GEM), contrary to what was commonly assumed in earlier studies which frequently omitted GEM dry deposition as an important process. Dry deposition exceeded wet deposition by a large margin in all of the seasons except in the summer at the majority of the sites. GEM dry deposition over vegetated surfaces will not decrease at the same pace, and sometimes may even increase with decreasing anthropogenic emissions, suggesting that Hg emission reductions should be a long-term policy sustained by global cooperation.

Environmental Science & Technology

Groundwater quality from private domestic water-supply wells in the vicinity of petroleum production in southwestern Indiana

The U.S. Geological Survey provided technical support to the Agency for Toxic Substances and Disease Registry for site selection and sample collection and analysis in a 2012 investigation of groundwater quality from 29 private domestic water-supply wells in the vicinity of petroleum production in southwestern Indiana. Petroleum hydrocarbons, oil and grease, aromatic volatile organic compounds, methane concentrations greater than 8,800 micrograms per liter, chloride concentrations greater than 250 milligrams per liter, and gross alpha radioactivity greater than 15 picocuries per liter were reported in the analysis of groundwater samples from 11 wells.

Indiana

Geochemical legacies and the future health of cities: A tale of two neurotoxins in urban soils

The past and future of cities are inextricably linked, a linkage that can be seen clearly in the long-term impacts of urban geochemical legacies. As loci of population as well as the means of employment and industry to support these populations, cities have a long history of co-locating contaminating practices and people, sometimes with negative implications for human health. Working at the intersection between environmental processes, communities, and human health is critical to grapple with environmental legacies and to support healthy, sustainable, and growing urban populations. An emerging area of environmental health research is to understand the impacts of chronic exposures and exposure mixtures—these impacts are poorly studied, yet may pose a significant threat to population health. Acute exposure to lead (Pb), a powerful neurotoxin to which children are particularly susceptible, has largely been eliminated in the U.S. and other countries through policy-based restrictions on leaded gasoline and lead-based paints. But the legacy of these sources remains in the form of surface soil Pb contamination, a common problem in cities and one that has only recently emerged as a widespread chronic exposure mechanism in cities. Some urban soils are also contaminated with another neurotoxin, mercury (Hg). The greatest human exposure to Hg is through fish consumption, so eating fish caught in urban areas presents risks for toxic Hg exposure. The potential double impact of chronic exposure to these two neurotoxins is pronounced in cities. Overall, there is a paradigmatic shift from reaction to and remediation of acute exposures towards a more nuanced understanding of the dynamic cycling of persistent environmental contaminants with resultant widespread and chronic exposure of inner-city dwellers, leading to chronic toxic illness and disability at substantial human and social cost.

Indiana

Real-time, continuous water-quality monitoring in Indiana and Kentucky

Water-quality “super” gages (also known as “sentry” gages) provide real-time, continuous measurements of the physical and chemical characteristics of stream water at or near selected U.S. Geological Survey (USGS) streamgages in Indiana and Kentucky. A super gage includes streamflow and water-quality instrumentation and representative stream sample collection for laboratory analysis. USGS scientists can use statistical surrogate models to relate instrument values to analyzed chemical concentrations at a super gage. Real-time, continuous and laboratory-analyzed concentration and load data are publicly accessible on USGS Web pages.

Indiana, Kentucky

Mercury and methylmercury in reservoirs in Indiana

Mercury (Hg) is an element that occurs naturally, but evidence suggests that human activities have resulted in increased amounts being released to the atmosphere and land surface. When Hg is converted to methylmercury (MeHg) in aquatic ecosystems, MeHg accumulates and increases in the food web so that some fish contain levels which pose a health risk to humans and wildlife that consume these fish. Reservoirs unlike natural lakes, are a part of river systems that are managed for flood control. Data compiled and interpreted for six flood-control reservoirs in Indiana showed a relation between Hg transport, MeHg formation in water, and MeHg in fish that was influenced by physical, chemical, and biological differences among the reservoirs. Existing information precludes a uniform comparison of Hg and MeHg in all reservoirs in the State, but factors and conditions were identified that can indicate where and when Hg and MeHg levels in reservoirs could be highest. As part of a statewide monitoring network for Hg and MeHg in Indiana streams, 66 water samples were collected from four reservoir tailwater sites (downstream near the dams) on a quarterly schedule for 5 years. The reservoirs were Brookville Lake, Cagles Mill Lake, J. Edward Roush Lake, and Mississinewa Lake. Particulate-bound Hg concentrations were significantly lower in tailwater samples than in samples from free-flowing streams in the statewide network. (Free-flowing streams were not affected by dams and were not upstream from these reservoirs.) These data indicated the reduced flow velocity of water upstream from dams was allowing particulate-bound Hg to settle out of the water in the reservoir pools. The concentration ratios of MeHg to Hg were significantly higher in the tailwater samples than in samples from free-flowing streams, and the MeHg to Hg ratios were significantly higher in summer than in other seasons. To evaluate the conditions related to MeHg formation, pools of three reservoirs (Brookville Lake, Monroe Lake, and Patoka Lake) were investigated during summer hydrologic conditions. Water temperature and dissolved oxygen were measured from the water surface to the lake bottom at 10 to 17 transects across each reservoir to identify three thermal strata, defined by water temperature, dissolved oxygen concentration, and depth. Depth-specific water samples were collected from these thermal strata throughout each reservoir, from the headwaters to the dam and from the tailwater. Mercury concentrations higher than 0.04 nanogram per liter (ng/L) were detected in all 53 samples, and MeHg concentrations higher than 0.04 ng/L were detected in 53 percent of the samples. The investigation found a zone of water below 8 or 9 meters, with temperatures less than 18 degrees Celsius and dissolved oxygen less than 3.5 milligrams per liter, extending through nearly half the reservoir area in Monroe Lake and Patoka Lake. This zone had abundant dissolved MeHg and concentration ratios of dissolved MeHg to Hg that ranged from 25 to 82 percent. This zone also had water with pH less than 7 and decreased dissolved sulfate, conditions indicating sulfate reduction by microorganisms that promoted a high potential for the conversion of Hg to MeHg. Reservoir outflow came from this zone at Monroe Lake and contributed to a tailwater concentration ratio for dissolved MeHg to Hg of 56 percent. Reservoir outflow at Patoka Lake was not from this zone, and dissolved MeHg was not detected in the tailwater. In contrast, samples from the summer pool at Brookville Lake had no MeHg detections even though Hg was detected, probably because the water pH higher than 7 inhibited sulfate reduction and did not promote the conversion of Hg to MeHg. Mercury and MeHg concentrations and the concentration ratios of MeHg to Hg in water varied among the six reservoirs in Indiana, and the differences were related to a combination of factors that could apply to other reservoirs. In areas with moderate to high rates of atmospheric Hg wet and dry deposition, Hg runoff and transport to streams and reservoirs was potentially highest for reservoirs with heavily forested watersheds in steep terrains of near-surface bedrock. Methylmercury concentrations and concentration ratios of MeHg to Hg were highest for reservoirs with the longest summer pools and highest inflow-to-outflow retention times, where water-chemistry conditions favoring sulfate reduction promoted conversion of Hg to MeHg. Methylmercury (reported as Hg) in fish-tissue samples collected for the State fish consumption advisory program was used to describe MeHg food-web accumulation and magnification in the reservoirs. The highest percentages of fish-tissue samples with Hg concentrations that exceeded the criterion of 0.30 milligram per kilogram for protection of human health were from Monroe Lake (38 percent) and Patoka Lake (33 percent). A review of the number and size of fish species caught from these two reservoirs resulted in two implications for fish consumption by humans. First, the highest numbers of fish harvested for potential human consumption were species more likely to have MeHg concentrations lower than the human-health criterion (crappie, bluegill, and catfish). Second, although largemouth bass were likely to have MeHg concentrations higher than the human-health criterion, they were caught and released more often than they were harvested. However, the average size largemouth bass (in both reservoirs) and above-average size walleye (in Monroe Lake) that were harvested for potential human consumption were likely to have MeHg concentrations higher than the human-health criterion.

Indiana

A Great Lakes atmospheric mercury monitoring network: evaluation and design

As many as 51 mercury (Hg) wet-deposition-monitoring sites from 4 networks were operated in 8 USA states and Ontario, Canada in the North American Great Lakes Region from 1996 to 2010. By 2013, 20 of those sites were no longer in operation and approximately half the geographic area of the Region was represented by a single Hg-monitoring site. In response, a Great Lakes Atmospheric Mercury Monitoring (GLAMM) network is needed as a framework for regional collaboration in Hg-deposition monitoring. The purpose of the GLAMM network is to detect changes in regional atmospheric Hg deposition related to changes in Hg emissions. An optimized design for the network was determined to be a minimum of 21 sites in a representative and approximately uniform geographic distribution. A majority of the active and historic Hg-monitoring sites in the Great Lakes Region are part of the National Atmospheric Deposition Program (NADP) Mercury Deposition Network (MDN) in North America and the GLAMM network is planned to be part of the MDN. To determine an optimized network design, active and historic Hg-monitoring sites in the Great Lakes Region were evaluated with a rating system of 21 factors that included characteristics of the monitoring locations and interpretations of Hg data. Monitoring sites were rated according to the number of Hg emissions sources and annual Hg emissions in a geographic polygon centered on each site. Hg-monitoring data from the sites were analyzed for long-term averages in weekly Hg concentrations in precipitation and weekly Hg-wet deposition, and on significant temporal trends in Hg concentrations and Hg deposition. A cluster analysis method was used to group sites with similar variability in their Hg data in order to identify sites that were unique for explaining Hg data variability in the Region. The network design included locations in protected natural areas, urban areas, Great Lakes watersheds, and in proximity to areas with a high density of annual Hg emissions and areas with high average weekly Hg wet deposition. In a statistical analysis, relatively strong, positive correlations in the wet deposition of Hg and sulfate were shown for co-located NADP Hg-monitoring and acid-rain monitoring sites in the Region. This finding indicated that efficiency in regional Hg monitoring can be improved by adding new Hg monitoring to existing NADP acid-rain monitoring sites. Implementation of the GLAMM network design will require Hg-wet-deposition monitoring to be: (a) continued at 12 MDN sites active in 2013 and (b) restarted or added at 9 NADP sites where it is absent in 2013. Ongoing discussions between the states in the Great Lakes Region, the Lake Michigan Air Directors Consortium (a regional planning entity), the NADP, the U.S. Environmental Protection Agency, and the U.S. Geological Survey are needed for coordinating the GLAMM network.

Great Lakes

Water quality in Indiana: trends in concentrations of selected nutrients, metals, and ions in streams, 2000-10

Water quality in Indiana streams generally improved during the 2000–10 study period, based on trends in selected nutrients, metals, and ions. This study combined water-quality data from the Indiana Fixed Station Monitoring Program (FSMP) with streamflow data from nearby U.S. Geological Survey streamgages. A parametric time-series model, QWTREND, was used to develop streamflow-adjusted constituent concentrations, to adjust for seasonal variance and serial correlation, and to identify trends independent of streamflow-related variability. This study examined 7,345 water samples from 57 FSMP sites for 11 years. Concentration trends were analyzed for 12 constituents—the nutrients nitrate, organic nitrogen, and phosphorus; suspended solids; the metals copper, iron, lead, and zinc; the ions chloride, and sulfate together with hardness as a measure of the calcium carbonate ion; and dissolved solids. Nutrient concentrations in this study generally were too high relative to standards and criteria. The national recommended criteria for the three ecoregions in Indiana were exceeded by more than one-half of the nitrate and most of the phosphorus concentrations. Copper, lead, zinc, chloride, sulfate, and dissolved solids concentrations were in acceptable ranges relative to standards and criteria in more than 97 percent of samples. The two Lake Michigan Basin sites had the highest concentrations and were in a unique statistical group for 10 of the 12 constituents, with concentrations many times higher than the statewide median and higher than the medians of most other basins. The two Ohio River Basin sites had the lowest concentrations and were in a unique statistical group for 6 of the 12 constituents. Statistically significant trends were identified that included 167 downward trends and 83 upward trends. The Kankakee River Basin had the most significant upward trends while the most significant downward trends were in the Whitewater River Basin, the Lake Michigan Basin, and the Patoka River Basin. For most constituents, a majority of sites had significant downward trends. Two streams in the Lake Michigan Basin have shown substantial decreases in most constituents. The West Fork White River near Indianapolis, Indiana, showed increases in nitrate and phosphorus and the Kankakee River Basin showed increases in copper, zinc, chloride, sulfate, and hardness. Upward trends in nutrients were identified at a few sites, but most nutrient trends were downward. Upward trends in metals corresponded with relatively small concentration increases while downward trends involved considerably larger concentration changes. Downward trends in chloride, sulfate, and suspended solids were observed statewide, but upward trends in hardness were observed in the northern half of Indiana.

Indiana

Organic wastewater compounds in water and sediment in and near restored wetlands, Great Marsh, Indiana Dunes National Lakeshore, 2009–11

A cooperative investigation between the U.S. Geological Survey and the National Park Service was completed from 2009 through 2011 to understand the occurrence, distribution, and environmental processes affecting concentrations of organic wastewater compounds in water and sediment in and near Great Marsh at the Indiana Dunes National Lakeshore in Beverly Shores, Indiana. Sampling sites were selected to represent hydrologic inputs to the restored wetlands from adjacent upstream residential and less developed areas and to represent discharge points of cascading cells within the restored wetland. A multiphase approach was used for the investigation. Discrete water samples and time-integrated passive samples were analyzed for 69 organic wastewater compounds. Continuous water-level information and periodic streamflow measurements characterized flow conditions at discharge points from restored wetland cells. Wetland sediments were collected and analyzed for sorptive losses of organic wastewater compounds and to evaluate of the potential for wetland sediments to biotransform organic wastewater compounds. A total of 52 organic wastewater compounds were detected in discrete water samples at 1 or more sites. Detections of organic wastewater compounds were widespread, but concentrations were generally low and 95 percent were less than 2.1 micrograms per liter. Six compounds were detected at concentrations greater than 2.1 micrograms per liter—four fecal sterols (beta-sitosterol, cholesterol, beta-stigmastanol, and 2-beta coprostanol), one plasticizer (bis-2-ethylhex ylphthalate), and a non-ionic detergent (4-nonylphenol diethoxylate). Two 1-month deployments of time-integrative passive samplers, called polar organic chemical integrative samplers, detected organic wastewater compounds at lower concentrations than were possible with discrete water samples. Isopropyl benzene (solvent), caffeine (plant alkaloid, stimulant), and hexahydrohexamethyl cyclopentabenzopyran (fragrance) were detected in more than half of the extracts from passive samplers, but they were not detected in any discrete water sample. The Yeast Estrogen Screen assay identified measurable estrogenicity in one passive sampler extract from the most downstream wetland site in both the April and November–December 2011 deployments and in passive sampler extracts from one residential and one upstream site in the November–December 2011 deployment only. Surface-water levels in the restored wetland cells were monitored continuously using submersible pressure transducers in hand-driven well points screened in the surface water. Surface-water levels in the wetland cells responded quickly to precipitation and substantially receded within 2 days following the largest rainfall events. Seasonal patterns in water levels generally showed higher and more variable surface-water levels in the wetland cells during spring and early summer. Water levels in the wetland cells fell below the elevation of the control structures and ceased to flow over the spillways during extended dry periods (primarily late summer and early fall). Daily loads of seven organic wastewater compounds, as indicators of septic system effluent, were estimated for samples collected at wetland outlet spillways when flow measurements could be made. Median daily loads of the indicator organic wastewater compounds increased in downstream order, and the largest median loads were measured at the most downstream site. Median daily loads were higher for samples collected in spring and summer than those collected in fall, as the higher seasonal water levels increased streamflow at the wetland outlet spillways. Wetland sediment samples were analyzed for 84 organic wastewater compounds, polycyclic aromatic hydrocarbons, and semivolatile organic compounds to investigate the fate of contaminants in Great Marsh. The top five detected compounds by total mass in wetland sediment samples were beta-sitosterol, beta-stigmastanol, cholesterol, bis(2-ethylhexyl) phthalate, and phenol. Polycyclic aromatic hydrocarbons also were frequently detected in wetland sediment samples. Source apportionment of polycyclic aromatic hydrocarbon detections indicated atmospheric sources of pyrogenic compounds, rather than residential sources. Comparisons of polycyclic aromatic hydrocarbon concentrations in wetland sediment samples to sediment quality target guidelines indicated the potential for harmful effects on sediment-dwelling organisms at several sites. Biodegradation of select endocrine-disrupting compounds (17α-ethinylestradiol, 4-nonylphenol, triclocarban, and bisphenol A) in shallow wetland sediments was evaluated in laboratory experiments by using carbon-14 radiolabeled model contaminants. Substantial biodegradation of certain organic wastewater compounds were demonstrated, primarily in oxic (oxygen containing) environments. One of four modeled compounds, bisphenol A, was biodegraded in anoxic (oxygen free) environments. Only sediments collected nearest residential areas exhibited degradation of the synthetic birth control pharmaceutical, 17α-ethinylestradiol, possibly owing to adaptation and acclimation of the indigenous microbial community to septic discharge and the resultant selection of a microbial capability for biodegradation of 17α-ethinylestradiol.

Indiana

Spatial patterns and temporal trends in mercury concentrations, precipitation depths, and mercury wet deposition in the North American Great Lakes region, 2002-2008

Annual and weekly mercury (Hg) concentrations, precipitation depths, and Hg wet deposition in the Great Lakes region were analyzed by using data from 5 monitoring networks in the USA and Canada for a 2002-2008 study period. High-resolution maps of calculated annual data, 7-year mean data, and net interannual change for the study period were prepared to assess spatial patterns. Areas with 7-year mean annual Hg concentrations higher than the 12 ng per liter water-quality criterion were mapped in 4 states. Temporal trends in measured weekly data were determined statistically. Monitoring sites with significant 7-year trends in weekly Hg wet deposition were spatially separated and were not sites with trends in weekly Hg concentration. During 2002-2008, Hg wet deposition was found to be unchanged in the Great Lakes region and its subregions. Any small decreases in Hg concentration apparently were offset by increases in precipitation.

Great Lakes Region

Litterfall mercury dry deposition in the eastern USA

Mercury (Hg) in autumn litterfall from predominately deciduous forests was measured in 3 years of samples from 23 Mercury Deposition Network sites in 15 states across the eastern USA. Annual litterfall Hg dry deposition was significantly higher (median 12.3 micrograms per square meter (μg/m 2 ), range 3.5–23.4 μg/m 2 ) than annual Hg wet deposition (median 9.6 μg/m 2 , range 4.4–19.7 μg/m 2 ). The mean ratio of dry to wet Hg deposition was 1.3–1. The sum of dry and wet Hg deposition averaged 21 μg/m 2 per year and 55% was litterfall dry deposition. Methylmercury was a median 0.8% of Hg in litterfall and ranged from 0.6 to 1.5%. Annual litterfall Hg and wet Hg deposition rates differed significantly and were weakly correlated. Litterfall Hg dry deposition differed among forest-cover types. This study demonstrated how annual litterfall Hg dry deposition rates approximate the lower bound of annual Hg dry fluxes.

Environmental Pollution

Mercury in Indiana watersheds: Retrospective for 2001–2006

Information about total mercury and methylmercury concentrations in water samples and mercury concentrations in fish-tissue samples was summarized for 26 watersheds in Indiana that drain most of the land area of the State. Mercury levels were interpreted with information on streamflow, atmospheric mercury deposition, mercury emissions to the atmosphere, mercury in wastewater, and landscape characteristics. Unfiltered total mercury concentrations in 411 water samples from streams in the 26 watersheds had a median of 2.32 nanograms per liter (ng/L) and a maximum of 28.2 ng/L. When these concentrations were compared to Indiana water-quality criteria for mercury, 5.4 percent exceeded the 12-ng/L chronic-aquatic criterion, 59 percent exceeded the 1.8-ng/L Great Lakes human-health criterion, and 72.5 percent exceeded the 1.3-ng/L Great Lakes wildlife criterion. Mercury concentrations in water were related to streamflow, and the highest mercury concentrations were associated with the highest streamflows. On average, 67 percent of total mercury in streams was in a particulate form, and particulate mercury concentrations were significantly lower downstream from dams than at monitoring stations not affected by dams. Methylmercury is the organic fraction of total mercury and is the form of mercury that accumulates and magnifies in food chains. It is made from inorganic mercury by natural processes under specific conditions. Unfiltered methylmercury concentrations in 411 water samples had a median of 0.10 ng/L and a maximum of 0.66 ng/L. Methylmercury was a median 3.7 percent and maximum 64.8 percent of the total mercury in 252 samples for which methylmercury was reported. The percentages of methylmercury in water samples were significantly higher downstream from dams than at other monitoring stations. Nearly all of the total mercury detected in fish tissue was assumed to be methylmercury. Fish-tissue samples from the 26 watersheds had wet-weight mercury concentrations that exceeded the 0.3 milligram per kilogram (mg/kg) U.S. Environmental Protection Agency (USEPA) methylmercury criterion in 12.4 percent of the 1,731 samples. The median wet-weight concentration in the fish-tissue samples was 0.13 mg/kg, and the maximum was 1.07 mg/kg. A coarse-scale analysis of all fish-tissue data in each watershed and a fine-scale analysis of data within 5 kilometers (km) of the downstream end of each watershed showed similar results overall. Mercury concentrations in fish-tissue samples were highest in the White River watershed in southern Indiana and the Fall Creek watershed in central Indiana. In fish-tissue samples within 5 km of the downstream end of a watershed, the USEPA methylmercury criterion was exceeded by 45 percent of mercury concentrations from the White River watershed and 40 percent of the mercury concentration from the Fall Creek watershed. A clear relation between mercury concentrations in fish-tissue samples and methylmercury concentrations in water was not observed in the data from watersheds in Indiana. Average annual atmospheric mercury wet-deposition rates were mapped with data at 156 locations in Indiana and four surrounding states for 2001–2006. These maps revealed an area in southeastern Indiana with high mercury wet-deposition rates—from 15 to 19 micrograms per square meter per year (µg/m 2 /yr). Annual atmospheric mercury dry-deposition rates were estimated with an inferential method by using concentrations of mercury species in air samples at three locations in Indiana. Mercury dry deposition-rates were 5.6 to 13.6 µg/m 2 /yr and were 0.49 to 1.4 times mercury wet-deposition rates. Total mercury concentrations were detected in 96 percent of 402 samples of wastewater effluent from 50 publicly owned treatment works in the watersheds; the median concentration was 3.0 ng/L, and the maximum was 88 ng/L. When these concentrations were compared to Indiana water-quality criteria for mercury, 12 percent exceeded the 12-ng/L chronic-aquatic criterion, 68 percent exceeded the 1.8-ng/L Great Lakes human-health criterion, and 81 percent exceeded the 1.3-ng/L Great Lakes wildlife criterion. Annual stream mercury yields were calculated with a model by using the mercury concentrations in water samples and daily average streamflows for 2002–2006, normalized to the watershed drainage areas. The average annual total mercury stream yields ranged from 0.73 to 45.2 µg/m 2 /yr and were highest in two White River watersheds in central Indiana. Median methylmercury stream yield was 1.9 percent of the median total mercury stream yield. In most watersheds, average annual stream yields of total mercury were a fraction of the combined average annual atmospheric mercury wet-deposition and estimated annual dry-deposition loading rates, indicating that much of the stream mercury was attributable to atmospheric deposition. In two watersheds, average annual stream yields of total mercury were approximately twice the atmospheric mercury loading, indicating that some of the stream mercury apparently was not attributable to atmospheric deposition. Rather, some of the stream mercury yield potentially was contributed by mercury in wastewater discharges. Land-cover type corresponded with the mercury levels in three watersheds: (1) A watershed of the White River in central Indiana with a high percentage of urban land cover had some of the highest total mercury concentrations and stream mercury yields. The urban land cover and numerous permitted wastewater outfalls with mercury in treated effluent potentially contributed mercury to this watershed. (2) A monitoring station on the Maumee River in northeastern Indiana, downstream from a large area of urban land cover, recorded the highest stream mercury concentrations. The urban land cover and mercury detected in treated effluent potentially contributed to the high mercury concentrations at this station. (3) A watershed of the Patoka River in southern Indiana with a high percentage of forest land cover had the highest atmospheric mercury dry-deposition rate. The high dry-deposition rate from the forest land cover potentially contributed to the high mercury concentrations in this watershed. From a retrospective view, mercury concentrations in Indiana watersheds routinely exceeded criteria protective of humans and commonly exceeded criteria protective of wildlife. Atmospheric mercury wet deposition was a predominant factor, but not the single factor, affecting mercury in Indiana watersheds. Mercury in wastewater discharges and atmospheric mercury dry deposition apparently contributed a substantial part of the mercury yield from some watersheds. Dams and impoundments increased the percentage of methylmercury in downstream waters. Long-term monitoring of mercury in wet and dry atmospheric deposition, and in streams and reservoirs, coordinated with monitoring of mercury in fish, will be needed to detect whether mercury levels in Indiana watersheds change in the future.

Indiana

Mercury in precipitation in Indiana, January 2004–December 2005

Mercury in precipitation was monitored during 2004–2005 at five locations in Indiana as part of the National Atmospheric Deposition Program–Mercury Deposition Network (NADP–MDN). Monitoring stations were operated at Roush Lake near Huntington, Clifty Falls State Park near Madison, Fort Harrison State Park near Indianapolis, Monroe County Regional Airport near Bloomington, and Indiana Dunes National Lakeshore near Porter. At these monitoring stations, precipitation amounts were measured continuously and weekly samples were collected for analysis of mercury by methods achieving detection limits as low as 0.05 ng/L (nanograms per liter). Wet deposition was computed as the product of mercury concentration and precipitation. The data were analyzed for seasonal patterns, temporal trends, and geographic differences. In the 2 years, 520 weekly samples were collected at the 5 monitoring stations and 448 of these samples had sufficient precipitation to compute mercury wet deposition. The 2-year mean mercury concentration at the five monitoring stations (normalized to the sample volume) was 10.6 ng/L. As a reference for comparison, the total mercury concentration in 41 percent of the samples analyzed was greater than the statewide Indiana water-quality standard for mercury (12 ng/L, protecting aquatic life) and 99 percent of the concentrations exceeded the most conservative Indiana water-quality criterion (1.3 ng/L, protecting wild mammals and birds). The normalized annual mercury concentration at Clifty Falls in 2004 was the fourth highest in the NADP–MDN in eastern North America that year. In 2005, the mercury concentrations at Clifty Falls and Indiana Dunes were the ninth highest in the NADP–MDN in eastern North America. At the five monitoring stations during the study period, the mean weekly total mercury deposition was 0.208 µg/m 2 (micrograms per square meter) and mean annual total mercury deposition was 10.8 µg/m 2 . The annual mercury deposition at Clifty Falls in 2004 and 2005 was in the top 25 percent of the NADP–MDN stations in eastern North America. Mercury concentrations and deposition varied at the five monitoring stations during 2004–2005. Mercury concentrations in wet-deposition samples ranged from 1.2 to 116.6 ng/L and weekly mercury deposition ranged from 0.002 to 1.74 µg/m 2 . Data from weekly samples exhibited seasonal patterns. During April through September, total mercury concentrations and deposition were higher than the median for all samples. Annual precipitation at four of the five monitoring stations was within 10 percent of normal both years, with the exception of Indiana Dunes, where precipitation was 23 percent below normal in 2005. Episodes of high mercury deposition, which were the top 10 percent of weekly mercury deposition at the five monitoring stations, contributed 39 percent of all mercury deposition during 2004–2005. Mercury deposition more than 1.04 µg/m 2 (5 times the mean weekly deposition) was recorded for 12 samples. These episodes of highest mercury deposition were recorded at all five monitoring stations, but the most (7 of 12) were at Clifty Falls and contributed 34.4 percent of the total deposition at that station during 2004–2005. Weekly samples with high mercury deposition may help to explain the differences in annual mercury deposition among the five monitoring stations in Indiana. A statistical evaluation of the monitoring data for 2001–2005 indicated several statistically significant temporal trends. A statewide (5-station) decrease (p = 0.007) in mercury deposition and a statewide decrease (p = 0.059) in mercury concentration were shown. Decreases in mercury deposition (p = 0.061 and p = 0.083) were observed at Roush Lake and Bloomington. A statistically significant trend was not observed for precipitation at the five monitoring stations during this 5-year period. A potential explanation for part of the statewide decrease in mercury concentration and mercury deposition was a 28 percent decrease in the total estimated annual mercury emissions in Indiana between 2002 and 2005. Mercury deposition statistically was correlated most closely to precipitation in the 448 samples, 2004–2005, and this relation was demonstrated by statewide maps of annual precipitation and annual mercury deposition based on precipitation data from 127 National Weather Service Cooperative Observer Program stations. However, one area in southeastern Indiana in the vicinity of Clifty Falls exhibited high mercury deposition that might be related more to mercury concentration than to precipitation. This is because areas with the same range of precipitation as southeastern Indiana were mapped with less mercury deposition. Other data demonstrate a geographic difference for mercury in precipitation in the vicinity of the Clifty Falls monitoring station. The weekly mercury concentrations at Clifty Falls were statistically higher than concentrations at Roush Lake, Fort Harrison, and Bloomington. Clifty Falls data ranked highest among the five monitoring stations for mercury concentration and mercury deposition, 2004–2005, and in the previous 3 years. Episodes of high mercury deposition were recorded most often at Clifty Falls in 2004–2005 and in the previous 3 years. Statistical trends in mercury concentration or mercury deposition were not observed for the Clifty Falls data. A potential explanation for this geographic difference is that annual mercury emissions from sources in the vicinity of Clifty Falls were higher than those at the other stations. Other factors may help explain the differences in total mercury concentrations, such as the types of mercury emissions, mercury transport from stationary sources outside Indiana, and meteorological conditions. Additional data are needed to assign a localized or regional boundary to the area affected by high deposition of mercury near Clifty Falls.

Indiana

Total mercury and methylmercury in Indiana streams, August 2004-September 2006

Total mercury and methylmercury were determined by use of low (subnanogram per liter) level analytical methods in 225 representative water samples collected following ultraclean protocols at 25 Indiana monitoring stations in a statewide network, on a seasonal schedule, August 2004-September 2006. The highest unfiltered total mercury concentrations were at six monitoring stations - five that are downstream from urban and industrial wastewater discharges and that have upstream drainage areas more than 1,960 square miles and one that is downstream from active and abandoned mine lands and that has an upstream drainage area of 602 square miles. Total mercury concentrations in unfiltered samples ranged from 0.24 to 26.9 nanograms per liter (ng/L), with a median of 2.35 ng/L. The highest concentrations of total mercury, those in the 90th percentile and above, were more than 9.05 ng/L, and most were in samples collected during winter and spring 2006 during changing streamflow hydrograph conditions. Seasonal medians for unfiltered total mercury were highest during winter and spring. Instantaneous streamflow and turbidity at the time of sample collection also were highest in winter and spring and potentially indicate conditions for the most particulate mercury transport. Samples with the highest total mercury concentrations were from water that had the highest turbidity at the time of sample collection. Unfiltered total mercury concentrations were significantly lower in samples collected at five stations downstream from dams. Values for particulate total mercury and streamflow also were significantly lower at these five stations. Total mercury concentrations equaled or exceeded the 2007 Indiana chronic aquatic criterion of 12 ng/L in 5.8 percent of samples and at 10 monitoring stations. Most of the total mercury in these 13 samples was estimated to be particulate. Most of the samples with mercury concentrations that equaled or exceeded the 12 ng/L criterion were collected during winter and spring 2006 during changing streamflow hydrograph conditions and in streamflow that was high for 2004-2006. Methylmercury was detected in 83 percent of unfiltered samples; reported concentrations ranged from 0.04 to 0.57 ng/L, with a median of 0.09 ng/L. The highest concentrations of methylmercury, those in the 90th percentile and above, were more than 0.25 ng/L, and most were in samples collected during spring and summer. Methylation efficiency in most samples was less than 5.8 percent, but was as much as 24.6 percent. Seasonal medians for methylmercury were highest during spring and summer. Seasonal medians for water temperatures at the time of sample collection were highest during these seasons and potentially indicate conditions for the most formation of methylmercury. The low streamflow statistical category had the significantly highest methylation efficiency.

Indiana

Environmental Assessment of the Muscatatuck Urban Training Center near Butlerville, Indiana, October and November 2005

An environmental assessment of the Muscatatuck Urban Training Center near Butlerville in Jennings County, Indiana, was completed during October and November 2005. As part of the Department of Defense Earth Science Program, the U.S. Geological Survey collected information about environmental conditions at the 825-acre former State of Indiana mental health facility prior to its conversion by the Indiana National Guard into an urban training center. The assessment was designed to investigate the type and extent of potential contamination associated with historical activities in selected areas of the facility. Samples of surface water, ground water, surface soil, and buried sediment were collected for the assessment in seven geographic study areas. Surface-water samples were collected from flowing and pooled surface water, as well as seeps and springs where ground water discharged at the land surface. Ground-water samples were collected from temporary wells installed in boreholes drilled to bedrock. Surface-soil samples were collected near sites of possible contamination. Buried-sediment samples were taken from core material collected near the top of bedrock at depths of 6.4 to 26 feet. For the assessment, 59 environmental, 22 quality-assurance, and 46 laboratory-blank samples were analyzed for as many as 65 volatile organic compounds, 62 semivolatile organic compounds, 20 trace elements, 10 inorganic cations and anions, 3 nutrients, and 4 water-quality characteristics. Concentrations of constituents detected in these samples were compared with regulatory standards (the Indiana Surface-Water-Quality Standards and Indiana Ground-Water-Quality Standards) and guidance criteria from the Indiana Department of Environmental Management's Risk Integrated System of Closures for contaminated soil and ground water. Standards or criteria were exceeded by 17 constituent concentrations in 11 environmental samples from 5 of the 7 geographic study areas. Standards or criteria were exceeded for 10 constituents: ammonia, arsenic, benzo(a)pyrene, beryllium, chloride, chloroform, copper, lead, sulfate, and zinc.

Indiana

Mercury in precipitation in Indiana, January 2001–December 2003

Mercury in precipitation was monitored during 2001 through 2003 at four locations in Indiana as part of the National Atmospheric Deposition Program-Mercury Deposition Network (NADP-MDN). Monitoring stations were operated at Roush Lake near Huntington, Clifty Falls State Park near Madison, Monroe County Regional Airport near Bloomington, and Indiana Dunes National Lakeshore near Porter. At these monitoring stations, precipitation amounts were measured and weekly samples were collected for analysis of total mercury and methylmercury by low-level methods. Wet deposition was computed with the total mercury and methylmercury concentrations and the precipitation amounts. In 3 years of weekly samples collected at the four monitoring stations, the volume-weighted total mercury concentration was 11.5 ng/L (nanograms per liter). As a reference for comparison, the total mercury concentration in 47 percent of the samples analyzed was greater than the Indiana water-quality standard for mercury (12 ng/L, protecting aquatic life) and nearly all of the concentrations exceeded the Indiana water-quality standards for mercury in the Great Lakes system (1.8 ng/L, protecting human health, and 1.3 ng/L, protecting wild mammals and birds). The precipitation-weighted concentrations at three of the monitoring stations in Indiana in 2003 were in the top 40 percent of all monitoring stations in the NADP-MDN and the concentration at Indiana Dunes was the eighth highest in the NADP-MDN for 2003. At the four monitoring stations during the study period, the mean weekly total mercury deposition was 243 ng/m 2 (nanograms per square meter) and mean annual total mercury deposition was 12,623 ng/m 2 . The annual mercury deposition at the four monitoring stations in Indiana in 2003 was in the top 40 percent of all monitoring stations in the NADP-MDN and the annual mercury deposition at the Clifty Falls station was the tenth highest in the NADP-MDN for 2003. For the 3-year period, the median methylmercury concentration in weekly samples was 0.058 ng/L with a maximum of 5.77 ng/L. Normalized methylmercury deposition was 2.09 ng/m 2 per inch of precipitation and methylmercury deposition was 0.7 percent of the total mercury deposition. The annual and mean weekly methylmercury deposition was highest at the Roush Lake station. Among the monitoring stations in the NADP-MDN with methylmercury data, methylmercury deposition at the monitoring stations in Indiana appeared to be higher than at eight stations in Wisconsin and Minnesota for that same time period, although methylmercury concentrations in Indiana were similar to or lower than those in Wisconsin and Minnesota. Geographically, the weekly total mercury concentrations at Indiana Dunes and Clifty Falls were statistically higher than concentrations at Bloomington, although a statistical difference in weekly total mercury deposition was not found among the four monitoring stations. Annual mercury emissions from sources in the vicinity of Indiana Dunes and Clifty Falls in 2001 were more than 10 times those at Bloomington, although other factors may help explain the differences in total mercury concentrations, such as the types of mercury emissions, mercury transport from sources outside Indiana, and meteorological conditions. Mercury concentrations and deposition varied at the four monitoring stations during the 3-year period. Total mercury concentrations in weekly samples ranged from 1.54 to 77 ng/L and weekly mercury deposition ranged from 0.8 to 2,456 ng/m 2 . Data from weekly samples exhibited seasonal patterns. Total mercury concentrations and deposition were highest in spring and summer and lowest in winter. Methylmercury concentrations were highest in winter and methylmercury deposition was highest in spring. Annual precipitation at the four monitoring stations was highest in 2003, exceeding the precipitation normals in spring and summer 2003. Annual mercury deposition in 2003 at the Roush Lake, Clifty Falls, and Indiana Dunes was as much as 41 to 67 percent higher in 2003 than in 2001 or in 2002 at those stations. Total mercury deposition that was more than 10 percent of the mean annual deposition (1,262 ng/m 2 ) was recorded in 11 of 551 weekly samples from the study period. These samples contained approximately 3 inches or more of rain and most were collected in spring and summer 2003. The highest deposition (2,456 ng/m 2 in a sample from Roush Lake) was 15.7 percent of the annual deposition at that station and approximately 10 times the mean weekly deposition for Indiana. High deposition recorded in three weekly samples at Clifty Falls contributed 31 percent of the annual deposition at that station in 2003. Weekly samples with high mercury deposition may help to explain the differences in annual mercury deposition among the four monitoring stations in Indiana.

Indiana