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[en] From 2000 to 2004, we sampled for total mercury (THg) and methylmercury (MeHg) in inlet streams to Lake Champlain, targeting high flow periods to capture increases in THg and MeHg concentrations with increasing flow. We used these data to model stream THg and MeHg fluxes for Water Years 2001 through 2009. In this mountainous forested basin with a high watershed-to-lake area ratio of 18, fluvial export from the terrestrial watershed was the dominant source of Hg to the lake. Unfiltered THg and MeHg fluxes were dominated by the particulate fraction; about 40% of stream THg was in the filtered (<0.4 μm) phase. THg flux from the watershed to the lake averaged 2.37 μg m−2 yr−1, or about 13% of atmospheric Hg wet and dry deposition to the basin. THg export from the lake represented only about 3% of atmospheric Hg input to the basin. - Highlights: ► We monitored total mercury and methylmercury in major tributaries to Lake Champlain. ► Mercury and methylmercury export was primarily as particulates during high flow. ► Only 13% of atmospheric total mercury input reached the lake via streams. ► Only 3% of atmospheric total mercury input reached the lake outlet. - Eighty-seven percent of total mercury deposition to the Lake Champlain basin is retained in the terrestrial basin; stream export of total and methylmercury to the lake is primarily in the particulate phase.
[en] Hydrochemical changes between 1991 and 2001 were assessed based on two synoptic stream surveys from the 820-km2 region of the Slavkov Forest and surrounding area, western Czech Republic. Marked declines of sulfate, nitrate, chloride, calcium and magnesium in surface waters were compared with other areas of Europe and North America recovering from acidification. Declines of sulfate concentration in the Slavkov Forest (-30 μeq L-1 yr-1) were more dramatic than declines reported from other sites. However, these dramatic declines of strong acid anions did not generate a widespread increase of stream water pH in the Slavkov Forest. Only the most acidic streams experienced a slight increase of pH by 0.5 unit. An unexpected decline of stream water pH occurred in slightly alkaline streams. - Acidified streams experienced unprecedented recovery from sulfate and nitrate pollution but pH and ANC decreased in alkaline streams
[en] Stable sulfur (S) isotope ratios can be used to identify the sources of sulfate contributing to streamwater. We collected weekly and high-flow stream samples for S isotopic analysis of sulfate through the entire water year 2003 plus the snowmelt period of 2004. The study area was the 41-ha forested W-9 catchment at Sleepers River Research Watershed, Vermont, a site known to produce sulfate from weathering of sulfide minerals in the bedrock. The δ34S values of streamwater sulfate followed an annual sinusoidal pattern ranging from about 6.5 per millein early spring to about 10 per millein early fall. During high-flow events, δ34S values typically decreased by 1 to 3 per millefrom the prevailing seasonal value. The isotopic evidence suggests that stream sulfate concentrations are controlled by: (1) an overall dominance of bedrock-derived sulfate (δ34S ∼ 6-14 per mille); (2) contributions of pedogenic sulfate (δ34S ∼ 5-6 per mille) during snowmelt and storms with progressively diminishing contributions during base flow recession; and (3) minor effects of dissimilatory bacterial sulfate reduction and subsequent reoxidation of sulfides. Bedrock should not be overlooked as a source of S in catchment sulfate budgets
[en] Stream water samples were collected over a range of hydrologic and seasonal conditions at three forested watersheds in the northeastern USA. Samples were analyzed for dissolved total mercury (THgd), DOC concentration and DOC composition, and UV254 absorbance across the three sites over different seasons and flow conditions. Pooling data from all sites, we found a strong positive correlation of THgd to DOC (r2 = 0.87), but progressively stronger correlations of THgd with the hydrophobic acid fraction (HPOA) of DOC (r2 = 0.91) and with UV254 absorbance (r2 = 0.92). The strength of the UV254 absorbance-THgd relationship suggests that optical properties associated with dissolved organic matter may be excellent proxies for THgd concentration in these streams. Ease of sample collection and analysis, the potential application of in-situ optical sensors, and the possibility for intensive monitoring over the hydrograph make this an effective, inexpensive approach to estimate THgd flux in drainage waters. - Ultraviolet absorbance measurements are a cost-effective proxy to estimate dissolved mercury concentration in stream water.
[en] The prospect of changing climate has led to uncertainty about the resilience of forested mountain watersheds in the tropics. In watersheds where frequent, high rainfall provides ample runoff, we often lack understanding of how the system will respond under conditions of decreased rainfall or drought. Factors that govern water supply, such as recharge rates and groundwater storage capacity, may be poorly quantified. This paper describes 8-year data sets of water stable isotope composition (δ"2H and δ"1"8O) of precipitation (4 sites) and a stream (1 site), and four contemporaneous stream sample sets of solute chemistry and isotopes, used to investigate watershed response to precipitation inputs in the 1780-ha Río Mameyes basin in the Luquillo Mountains of northeastern Puerto Rico. Extreme δ"2H and δ"1"8O values from low-pressure storm systems and the deuterium excess (d-excess) were useful tracers of watershed response in this tropical system. A hydrograph separation experiment performed in June 2011 yielded different but complementary information from stable isotope and solute chemistry data. The hydrograph separation results indicated that 36% of the storm rain that reached the soil surface left the watershed in a very short time as runoff. Weathering-derived solutes indicated near-stream groundwater was displaced into the stream at the beginning of the event, followed by significant dilution. The more biologically active solutes exhibited a net flushing behavior. The d-excess analysis suggested that streamflow typically has a recent rainfall component (∼25%) with transit time less than the sampling resolution of 7 days, and a more well-mixed groundwater component (∼75%). The contemporaneous stream sample sets showed an overall increase in dissolved solute concentrations with decreasing elevation that may be related to groundwater inputs, different geology, and slope position. A considerable amount of water from rain events runs off as quickflow and bypasses subsurface watershed flowpaths, and better understanding of shallow hillslope and deeper groundwater processes in the watershed will require sub-weekly data and detailed transit time modeling. A combined isotopic and solute chemistry approach can guide further studies to a more comprehensive model of the hydrology, and inform decisions for managing water supply with future changes in climate and land use. - Highlights: • Stream dissolved solutes increased with decreasing elevation in watershed. • Hydrograph separation showed brief groundwater input then dilution of solutes. • Stable isotopes indicated quickflow was 36% of the storm hydrograph. • Deuterium excess is a good tracer of seasonal watershed response and transit time. • Streamflow typically comprises ∼25% quickflow, ∼75% groundwater baseflow.
[en] 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 1 ng L-1 and MeHg was less than 0.2 ng 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 (<0.7 μm) 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-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. - High-flow sampling reveals strong contrasts in total mercury and methylmercury cycling in five diverse USA watersheds