Search

Determining the controls on dissolved mercury (HgD) transport is necessary to improve estimations of export from unmonitored watersheds and to forecast responses to changes in deposition and other environmental forcings. Stream water HgD and dissolved organic carbon (DOC) were evaluated over a range of discharge conditions in three streams within Shenandoah National Park, VA. Watersheds are distinguished by stream water pH (ranging from neutral to acidic) and soil size fractioning (ranging from clays to sands). At all sites, discharge was a significant but poor predictor of HgD concentrations (r2 from 0.13-0.52). HgD was strongly coupled with DOC at all sites (r2 from 0.74-0.89). UV absorbance at 254 nm (UV254), a proxy for DOC quantity and quality, slightly improved the predictions of HgD. Mean DOC quality differed between streams, with less aromatic DOC mobilized from the more acidic watershed. The site with less aromatic DOC and sandy soils mobilized more Hg to the stream for the same quantity and quality of DOC, likely due to the reduced capacity of the larger-grained soils to retain Hg, leaving a greater fraction associated with the organic matter. A similar amount of 0.54 ng HgD/mg DOC is transported at all sites, suggesting the less aromatic DOC transports less Hg per unit DOC, offsetting the effects of soil type. This research demonstrates that soil composition and DOC quality influence HgD export. We also provide evidence that soil organic carbon is a primary control on Hg-DOC ratios (0.12-1.4 ng mg-1) observed across the U.S. and Sweden. [ABSTRACT FROM AUTHOR]

Reductions in acidic deposition following the 1990 Amendments to the Clean Air Act have led to improvements in the acid/base status of many freshwater bodies in the eastern United States, but such recovery has not been as widespread in Virginia mountain streams. In the current analysis, water chemistry trends are determined for 63 streams within Shenandoah National Park, Virginia, and surrounding national forests, where water samples have been collected on a quarterly basis from 1987 to 2019. Over this timeframe, a majority of the most acid-sensitive streams – those with watersheds underlain by siliciclastic bedrock – have experienced reductions in acid neutralizing capacity (ANC). This outcome, which differs from the modest recovery predicted by earlier modeling studies, is likely due to further depletion of soil base cations and perhaps increases in organic acids. Meanwhile, stream water pH has increased for all watershed bedrock types, averaging between 0.05 and 0.10 pH units per decade. High-flow sampling was conducted at three sites from 1992 to 2019, revealing an assessment of episodic acidification that is more encouraging than that of chronic acidification. For two of these sites, pH during high-flow conditions increased much more rapidly than pH during low-flow conditions. Steep reductions in sulfur deposition over the three decades since the 1990 Amendments have led to a "flushing" of sulfate from shallow soils, which has contributed to the improved acid/base status during episodes of high flow. The findings suggest that continued low acidic deposition rates will lead to further improvements in stream water quality, with the timescales of recovery dependent upon bedrock geology of the watersheds. • Declines in acidic deposition led to limited recovery of Virginia mountain streams. • Acid neutralizing capacity has continued to decrease in many acid-sensitive streams. • Depletion of soil base cations has hindered recovery. • Greater improvements to the acid/based status are found during high-flow conditions. [ABSTRACT FROM AUTHOR]