Mercury (Hg) contamination of aquatic ecosystems and subsequent methylmercury bioaccumulation are significant environmental problems of global extent. At regional to global scales, the primary mechanism of Hg contamination is atmospheric Hg transport. Thus, a better understanding of the long-term history of atmospheric Hg cycling and quantification of the sources is critical for assessing the regional and global impact of anthropogenic Hg emissions. Ice cores collected from the Upper Fremont Glacier (UFG), Wyoming, contain a high-resolution record of total atmospheric Hg deposition (ca. 1720-1993). Total Hg in 97 ice-core samples was determined with trace-metal clean handling methods and low-level analytical procedures to reconstruct the first and most comprehensive atmospheric Hg deposition record of its kind yet available from North America. The record indicates major atmospheric releases of both natural and anthropogenic Hg from regional and global sources. Integrated over the past 270-year ice-core history, anthropogenic inputs contributed 52%, volcanic events 6%, and background sources 42%. More significantly, during the last 100 years, anthropogenic sources contributed 70% of the total Hg input. Unlike the 2-7-fold increase observed from preindustrial times (before 1840) to the mid-1980s in sediment-core records, the UFG record indicates a 20-fold increase for the same period. The sediment-core records, however, are in agreement with the last 10 years of this ice-core record, indicating declines in atmospheric Hg deposition.

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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 sediment total mercury (STHg), soil organic carbon (SOC), and the Hg to carbon ratio (RHgC) combined with maps of soil carbon. We measured a median STHg of 43 ± 30 ng Hg g soil−1 and a median RHgC of 1.6 ± 0.9 μg Hg g C−1, consistent with published results of STHg for tundra soils and 11,000 measurements from 4,926 temperate, nonpermafrost sites in North America and Eurasia. We estimate that the Northern Hemisphere permafrost regions contain 1,656 ± 962 Gg Hg, of which 793 ± 461 Gg Hg is frozen in permafrost. Permafrost soils store nearly twice as much Hg as all other soils, the ocean, and the atmosphere combined, and this Hg is vulnerable to release as permafrost thaws over the next century. Existing estimates greatly underestimate Hg in permafrost soils, indicating a need to reevaluate the role of the Arctic regions in the global Hg cycle.

[1] A detailed study of the climatic significance of d 18O in precipitation was completed on a 1500 km southwest-northeast transect of the Tibetan Plateau in central Asia. Precipitation samples were collected at four meteorological stations for up to 9 years. This study shows that the gradual impact of monsoon precipitation affects the spatial variation of d 18 O-T relationship along the transect. Strong monsoon activity in the southern Tibetan Plateau results in high precipitation rates and more depleted heavy isotopes. This depletion mechanism is described as a precipitation ''amount effect'' and results in a poor d18 O-T relationship at both seasonal and annual scales. In the middle of the Tibetan Plateau, the effects of the monsoon are diminished but continue to cause a reduced correlation of d 18 O and temperature at the annual scale. At the monthly scale, however, a significant d 18 O-T relationship does exist. To the north of the Tibetan Plateau beyond the extent of the effects of monsoon precipitation, d18 O in precipitation shows a strong temperature dependence. d18 O records from two shallow ice cores and historic air temperature data were compared to verify the modern d O in the ice core record in the monsoon regions of the southern Tibetan Plateau suggest past monsoon seasons were probably more expansive. It is still unclear, however, how changes in large-scale atmosphere circulation might influence summer monsoon precipitation on the Tibetan Plateau.

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.

Martin M., "Comparison of total mercury and methylmercury cycling at five sites using the small watershed approach" (2008 High-flow sampling reveals strong contrasts in total mercury and methylmercury cycling in five diverse USA watersheds. AbstractThe 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 1 ng L À1 and MeHg was less than 0.2 ng L À1. 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 À1 at Sleepers River, Vermont; 112 (0.75) ng L À1 at Rio Icacos, Puerto Rico; and 55 (0.80) ng L À1at Panola Mt., Georgia. Filtered (<0.7 mm) THg increased more modestly with flow in association with the hydrophobic acid fraction (HPOA) of DOC, with maximum filtered THg concentrations near 5 ng L À1 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.

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.

Mercury and organic carbon concentrations vary dynamically in streamwater at the Sleepers River Research Watershed in Vermont, USA. Total mercury (THg) concentrations ranged from 0.53 to 93.8 ng/L during a 3-year period of study. The highest mercury (Hg) concentrations occurred slightly before peak flows and were associated with the highest organic carbon (OC) concentrations. Dissolved Hg (DHg) was the dominant form in the upland catchments; particulate Hg (PHg) dominated in the lowland catchments. The concentration of hydrophobic acid (HPOA), the major component of dissolved organic carbon (DOC), explained 41-98% of the variability of DHg concentration while DOC flux explained 68-85% of the variability in DHg flux, indicating both quality and quantity of the DOC substantially influenced the transport and fate of DHg. Particulate organic carbon (POC) concentrations explained 50% of the PHg variability, indicating that POC is an important transport mechanism for PHg. Despite available sources of DHg and wetlands in the upland catchments, dissolved methylmercury (DmeHg) concentrations in streamwaters were below detection limit (0.04 ng/L). PHg and particulate methylmercury (PmeHg) had a strong positive correlation (r 2 =0.84, p<0.0001), suggesting a common source; likely instream or near-stream POC eroded or re-suspended during spring snowmelt and summer storms. Ratios of PmeHg to THg were low and fairly constant despite an apparent higher methylmercury (meHg) production potential in the summer. Methylmercury production in soils and stream sediments was below detection during snowmelt in April and highest in stream sediments (compared to forest and wetland soils) sampled in July. Using the watershed approach, the correlation of the percent of wetland cover to TmeHg concentrations in streamwater indicates that poorly drained wetland soils are a source of meHg and the relatively high concentrations found in stream surface sediments in July indicate these zones are a meHg sink.