Paul F. Schuster

Comparison of total mercury and methylmercury cycling at five sites using the small watershed approach

The small watershed approach is well-suited but underutilized in mercury research. We applied the small watershed approach to investigate total mercury (THg) and methylmercury (MeHg) dynamics in streamwater at the five diverse forested headwater catchments of the US Geological Survey Water, Energy, and Biogeochemical Budgets (WEBB) program. At all sites, baseflow THg was generally less than 1ng L(-1) and MeHg was less than 0.2ng L(-1). THg and MeHg concentrations increased with streamflow, so export was primarily episodic. At three sites, THg and MeHg concentration and export were dominated by the particulate fraction in association with POC at high flows, with maximum THg (MeHg) concentrations of 94 (2.56)ng L(-1) at Sleepers River, Vermont; 112 (0.75)ng L(-1) at Rio Icacos, Puerto Rico; and 55 (0.80)ng L(-1) at Panola Mt., Georgia. Filtered (<0.7microm) THg increased more modestly with flow in association with the hydrophobic acid fraction (HPOA) of DOC, with maximum filtered THg concentrations near 5ng L(-1) at both Sleepers and Icacos. At Andrews Creek, Colorado, THg export was also episodic but was dominated by filtered THg, as POC concentrations were low. MeHg typically tracked THg so that each site had a fairly constant MeHg/THg ratio, which ranged from near zero at Andrews to 15% at the low-relief, groundwater-dominated Allequash Creek, Wisconsin. Allequash was the only site with filtered MeHg consistently above detection, and the filtered fraction dominated both THg and MeHg. Relative to inputs in wet deposition, watershed retention of THg (minus any subsequent volatilization) was 96.6% at Allequash, 60% at Sleepers, and 83% at Andrews. Icacos had a net export of THg, possibly due to historic gold mining or frequent disturbance from landslides. Quantification and interpretation of Hg dynamics was facilitated by the small watershed approach with emphasis on event sampling.

Hydrological and chemical estimates of the water balance of a closed-basin lake in north central Minnesota

Chemical mass balances for sodium, magnesium, chloride, dissolved organic carbon, and oxygen 18 were used to estimate groundwater seepage to and from Williams Lake, Minnesota, over a 15-month period, from April 1991 through June 1992. Groundwater seepage to the lake and seepage from the lake to groundwater were determined independently using a flow net approach using data from water table wells installed as part of the study. Hydrogeological analysis indicated groundwater seepage to the lake accounted for 74% of annual water input to the lake; the remainder came from atmospheric precipitation, as determined from a gage in the watershed and from nearby National Weather Service gages. Seepage from the lake accounted for 69% of annual water losses from the lake; the remainder was removed by evaporation, as determined by the energy budget method. Calculated annual water loss exceeded calculated annual water gain, and this imbalance was double the value of the independently measured decrease in lake volume. Seepage to the lake determined from oxygen 18 was larger (79% of annual water input) than that determined from the flow net approach and made the difference between calculated annual water gain and loss consistent with the independently measured decrease in lake volume. Although the net difference between volume of seepage to the lake and volume of seepage from the lake was 1% of average lake volume, movement of water into and out of the lake by seepage represented an annual exchange of groundwater with the lake equal to 26–27% of lake volume. Estimates of seepage to the lake from sodium, magnesium, chloride, and dissolved organic carbon did not agree with the values determined from flow net approach or oxygen 18. These results indicated the importance of using a combination of hydrogeological and chemical approaches to define volume of seepage to and from Williams Lake and identify uncertainties in chemical fluxes.

Mercury on the move during snowmelt in Vermont

Although mercury (Hg) emissions peaked in the United States over the last 20 to 40 years and are now declining, they remain well above natural background levels in soils and sediments. Only a small fraction of the Hg deposited from the atmosphere to the terrestrial landscape runs off in streamflow. However, some of this Hg is methylated in the environment and can potentially bioaccumulate to the top of food webs, posing a hazard to people who eat fish, especially children and pregnant women. What factors determine the amount of Hg that runs off in streams? During the 2000 snowmelt at Sleepers River in Vermont, strong correlations were found between dissolved and particulate mercury and the respective dissolved and particulate organic carbon fractions, even when data were pooled from 10 streams of diverse watershed size and land cover. Episodic export of particulate Hg during the highest flows appears to be the dominant mechanism of Hg movement.

Mercury export from the Yukon River Basin and potential response to a changing climate

We measured mercury (Hg) concentrations and calculated export and yield from the Yukon River Basin (YRB) to quantify Hg flux from a large, permafrost-dominated, high-latitude watershed. Exports of Hg averaged 4400 kg Hg yr(-1). The average annual yield for the YRB during the study period was 5.17 μg m(-2) yr(-1), which is 3-32 times more than Hg yields reported for 8 other major northern hemisphere river basins. The vast majority (90%) of Hg export is associated with particulates. Half of the annual export of Hg occurred during the spring with about 80% of 34 samples exceeding the U.S. EPA Hg standard for adverse chronic effects to biota. Dissolved and particulate organic carbon exports explained 81% and 50%, respectively, of the variance in Hg exports, and both were significantly (p < 0.001) correlated with water discharge. Recent measurements indicate that permafrost contains a substantial reservoir of Hg. Consequently, climate warming will likely accelerate the mobilization of Hg from thawing permafrost increasing the export of organic carbon associated Hg and thus potentially exacerbating the production of bioavailable methylmercury from permafrost-dominated northern river basins.

Influences of glacier melt and permafrost thaw on the age of dissolved organic carbon in the Yukon River basin

Responses of near-surface permafrost and glacial ice to climate change are of particular significance for understanding long-term effects on global carbon cycling and carbon export by high-latitude northern rivers. Here we report Δ14C-dissolved organic carbon (DOC) values and dissolved organic matter optical data for the Yukon River, 15 tributaries of the Yukon River, glacial meltwater, and groundwater and soil water end-member sources draining to the Yukon River, with the goal of assessing mobilization of aged DOC within the watershed. Ancient DOC was associated with glacial meltwater and groundwater sources. In contrast, DOC from watersheds dominated by peat soils and underlain by permafrost was typically enriched in Δ14C indicating that degradation of ancient carbon stores is currently not occurring at large enough scales to quantitatively influence bulk DOC exports from those landscapes. On an annual basis, DOC exported was predominantly modern during the spring period throughout the Yukon River basin and became older through summer-fall and winter periods, suggesting that contributions of older DOC from soils, glacial meltwaters, and groundwater are significant during these months. Our data indicate that rapidly receding glaciers and increasing groundwater inputs will likely result in greater contributions of older DOC in the Yukon River and its tributaries in coming decades.

Runoff sources and flow paths in a partially burned, upland boreal catchment underlain by permafrost

Boreal soils in permafrost regions contain vast quantities of frozen organic material that is released to terrestrial and aquatic environments via subsurface flow paths as permafrost thaws. Longer flow paths may allow chemical reduction of solutes, nutrients, and contaminants, with implications for greenhouse gas emissions and aqueous export. Predicting boreal catchment runoff is complicated by soil heterogeneities related to variability in active layer thickness, soil type, fire history, and preferential flow potential. By coupling measurements of permeability, infiltration potential, and water chemistry with a stream chemistry end-member mixing model, we tested the hypothesis that organic soils and burned slopes are the primary sources of runoff, and that runoff from burned soils is greater due to increased hydraulic connectivity. Organic soils were more permeable than mineral soils, and 25% of infiltration moved laterally upon reaching the organic-mineral soil boundary on unburned hillslopes. A large portion of the remaining water infiltrated into deeper, less permeable soils. In contrast, burned hillslopes displayed poorly defined soil horizons, allowing rapid, mineral-rich runoff through preferential pathways at various depths. On the catchment scale, mineral/organic runoff ratios averaged 1.6 and were as high as 5.2 for an individual storm. Our results suggest that burned soils are the dominant source of water and solutes reaching the stream in summer, whereas unburned soils may provide longer term storage and residence times necessary for production of anaerobic compounds. These results are relevant to predicting how boreal catchment drainage networks and stream export will evolve given continued warming and altered fire regimes.

Multidecadal increases in the Yukon River Basin of chemical fluxes as indicators of changing flowpaths, groundwater, and permafrost

The Yukon River Basin, underlain by discontinuous permafrost, has experienced a warming climate over the last century that has altered air temperature, precipitation, and permafrost. We investigated a water chemistry database from 1982 to 2014 for the Yukon River and its major tributary, the Tanana River. Significant increases of Ca, Mg, and Na annual flux were found in both rivers. Additionally, SO4 and P annual flux increased in the Yukon River. No annual trends were observed for dissolved organic carbon (DOC) from 2001 to 2014. In the Yukon River, Mg and SO4 flux increased throughout the year, while some of the most positive trends for Ca, Mg, Na, SO4, and P flux occurred during the fall and winter months. Both rivers exhibited positive monthly DOC flux trends for summer (Yukon River) and winter (Tanana River). These trends suggest increased active layer expansion, weathering, and sulfide oxidation due to permafrost degradation throughout the Yukon River Basin.

Permafrost Stores a Globally Significant Amount of Mercury

Changing climate in northern regions is causing permafrost to thaw with major implications for the global mercury (Hg) cycle. We estimated Hg in permafrost regions based on in situ measurements of ...

A 50-year record of NOx and SO2 sources in precipitation in the Northern Rocky Mountains, USA

Ice-core samples from Upper Fremont Glacier (UFG), Wyoming, were used as proxy records for the chemical composition of atmospheric deposition. Results of analysis of the ice-core samples for stable isotopes of nitrogen (δ15N, ) and sulfur (δ34S, ), as well as and deposition rates from the late-1940s thru the early-1990s, were used to enhance and extend existing National Atmospheric Deposition Program/National Trends Network (NADP/NTN) data in western Wyoming. The most enriched δ34S value in the UFG ice-core samples coincided with snow deposited during the 1980 eruption of Mt. St. Helens, Washington. The remaining δ34S values were similar to the isotopic composition of coal from southern Wyoming. The δ15N values in ice-core samples representing a similar period of snow deposition were negative, ranging from -5.9 to -3.2 ‰ and all fall within the δ15N values expected from vehicle emissions. Ice-core nitrate and sulfate deposition data reflect the sharply increasing U.S. emissions data from 1950 to the mid-1970s.

Changing times, changing stories: generational differences in climate change perspectives from four remote indigenous communities in Subarctic Alaska

Indigenous Arctic and Subarctic communities currently are facing a myriad of social and environmental changes. In response to these changes, studies concerning indigenous knowledge (IK) and climate change vulnerability, resiliency, and adaptation have increased dramatically in recent years. Risks to lives and livelihoods are often the focus of adaptation research; however, the cultural dimensions of climate change are equally important because cultural dimensions inform perceptions of risk. Furthermore, many Arctic and Subarctic IK climate change studies document observations of change and knowledge of the elders and older generations in a community, but few include the perspectives of the younger population. These observations by elders and older generations form a historical baseline record of weather and climate observations in these regions. However, many indigenous Arctic and Subarctic communities are composed of primarily younger residents. We focused on the differences in the cultural dimensions of climate change found between young adults and elders. We outlined the findings from interviews conducted in four indigenous communities in Subarctic Alaska. The findings revealed that (1) intergenerational observations of change were common among interview participants in all four communities, (2) older generations observed more overall change than younger generations interviewed by us, and (3) how change was perceived varied between generations. We defined “observations” as the specific examples of environmental and weather change that were described, whereas “perceptions” referred to the manner in which these observations of change were understood and contextualized by the interview participants. Understanding the differences in generational observations and perceptions of change are key issues in the development of climate change adaptation strategies.