Multidecadal declines in particulate mercury and sediment export from Russian rivers in the pan-Arctic basin.

SignificanceRussian rivers are the predominant source of riverine mercury to the Arctic Ocean, where methylmercury biomagnifies to high levels in food webs. Pollution controls are thought to have decreased late-20th-century mercury loading to Arctic watersheds, but there are no published long-term observations on mercury in Russian rivers. Here, we present a unique hydrochemistry dataset to determine trends in Russian river particulate mercury concentrations and fluxes in recent decades. Using hydrologic and mercury deposition modeling together with multivariate time series analysis, we determine that 70 to 90% declines in particulate mercury fluxes were driven by pollution reductions and sedimentation in reservoirs. Results suggest that Russian rivers likely dominated over all other sources of mercury to the Arctic Ocean until recently.

Stream Dissolved Organic Matter in Permafrost Regions Shows Surprising Compositional Similarities but Negative Priming and Nutrient Effects.

Permafrost degradation is delivering bioavailable dissolved organic matter (DOM) and inorganic nutrients to surface water networks. While these permafrost subsidies represent a small portion of total fluvial DOM and nutrient fluxes, they could influence food webs and net ecosystem carbon balance via priming or nutrient effects that destabilize background DOM. We investigated how addition of biolabile carbon (acetate) and inorganic nutrients (nitrogen and phosphorus) affected DOM decomposition with 28-day incubations. We incubated late-summer stream water from 23 locations nested in seven northern or high-altitude regions in Asia, Europe, and North America. DOM loss ranged from 3% to 52%, showing a variety of longitudinal patterns within stream networks. DOM optical properties varied widely, but DOM showed compositional similarity based on Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis. Addition of acetate and nutrients decreased bulk DOM mineralization (i.e., negative priming), with more negative effects on biodegradable DOM but neutral or positive effects on stable DOM. Unexpectedly, acetate and nutrients triggered breakdown of colored DOM (CDOM), with median decreases of 1.6% in the control and 22% in the amended treatment. Additionally, the uptake of added acetate was strongly limited by nutrient availability across sites. These findings suggest that biolabile DOM and nutrients released from degrading permafrost may decrease background DOM mineralization but alter stoichiometry and light conditions in receiving waterbodies. We conclude that priming and nutrient effects are coupled in northern aquatic ecosystems and that quantifying two-way interactions between DOM properties and environmental conditions could resolve conflicting observations about the drivers of DOM in permafrost zone waterways.

Mercury Export from Arctic Great Rivers.

Land-ocean linkages are strong across the circumpolar north, where the Arctic Ocean accounts for 1% of the global ocean volume and receives more than 10% of the global river discharge. Yet estimates of Arctic riverine mercury (Hg) export constrained from direct Hg measurements remain sparse. Here, we report results from a coordinated, year-round sampling program that focused on the six major Arctic rivers to establish a contemporary (2012-2017) benchmark of riverine Hg export. We determine that the six major Arctic rivers exported an average of 20 000 kg y-1 of total Hg (THg, all forms of Hg). Upscaled to the pan-Arctic, we estimate THg flux of 37 000 kg y-1. More than 90% of THg flux occurred during peak river discharge in spring and summer. Normalizing fluxes to watershed area (yield) reveals higher THg yields in regions where greater denudation likely enhances Hg mobilization. River discharge, suspended sediment, and dissolved organic carbon predicted THg concentration with moderate fidelity, while suspended sediment and water yields predicted THg yield with high fidelity. These findings establish a benchmark in the face of rapid Arctic warming and an intensifying hydrologic cycle, which will likely accelerate Hg cycling in tandem with changing inputs from thawing permafrost and industrial activity.

Unprecedented Increases in Total and Methyl Mercury Concentrations Downstream of Retrogressive Thaw Slumps in the Western Canadian Arctic.

Retrogressive thaw slumps (RTSs) are thermokarst features created by the rapid thaw of ice-rich permafrost, and can mobilize vast quantities of sediments and solutes downstream. However, the effect of slumping on downstream concentrations and yields of total mercury (THg) and methylmercury (MeHg) is unknown. Fluvial concentrations of THg and MeHg downstream of RTSs on the Peel Plateau (Northwest Territories, Canada) were up to 2 orders of magnitude higher than upstream, reaching concentrations of 1,270 ng L-1 and 7 ng L-1, respectively, the highest ever measured in uncontaminated sites in Canada. MeHg concentrations were particularly elevated at sites downstream of RTSs where debris tongues dammed streams to form reservoirs where microbial Hg methylation was likely enhanced. However, > 95% of the Hg downstream was typically particle-bound and potentially not readily bioavailable. Mean open-water season yields of THg (610 mg km-2 d-1) and MeHg (2.61 mg km-2 d-1) downstream of RTSs were up to an order of magnitude higher than those for the nearby large Yukon, Mackenzie and Peel rivers. We estimate that ∼5% of the Hg stored for centuries or millennia in northern permafrost soils (88 Gg) is susceptible to release into modern-day Hg biogeochemical cycling from further climate changes and thermokarst formation.