Divergent Temporal Trends of Mercury in Arctic Char from Paired Lakes Influenced by Climate-Related Drivers.

Climate-driven changes including rising air temperatures, enhanced permafrost degradation, and altered precipitation patterns can have profound effects on contaminants, such as mercury (Hg), in High Arctic lakes. Two physically similar lakes, East Lake and West Lake at the Cape Bounty Arctic Watershed Observatory on Melville Island, Nunavut, Canada are being affected by climate change differently. Both lakes have experienced permafrost degradation in their catchments; however, West Lake has also undergone multiple underwater Mass Movement Events (MMEs; beginning in fall 2008), leading to a sustained 50-fold increase in turbidity. This provided the unique opportunity to understand the potential impacts of permafrost degradation and other climate-related effects on Hg concentrations and body condition of landlocked Arctic char (Salvelinus alpinus), an important sentinel species across the Circum-Arctic. Our objectives were to assess temporal trends in char Hg concentrations and to determine potential mechanisms driving the trends. There was a significant decrease in Hg concentrations in East Lake char, averaging 6.5%/year and 3.8%/year for length-adjusted and age-adjusted means, respectively, from 2008 to 2019. Conversely, in West Lake there was a significant increase, averaging 7.9%/year and 8.0%/year for length-adjusted and age-adjusted mean Hg concentrations, respectively, for 2009 to 2017 (the last year with sufficient sample size). The best predictors of length-adjusted Hg concentrations in West Lake were carbon and nitrogen stable isotope ratios, indicating a shift in diet including possible dietary starvation brought on by the profound increase in lake turbidity. Our study provides an example of how increasing lake turbidity, a likely consequence of climate warming in Arctic lakes, may influence fish condition and Hg concentrations. Environ Toxicol Chem 2023;42:2712-2725. © 2023 His Majesty the King in Right of Canada and The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC. Reproduced with the permission of the Minister of Environment and Climate Change Canada.

Snow Deposition and Melting as Drivers of Polychlorinated Biphenyls and Organochlorine Pesticides in Arctic Rivers, Lakes, and Ocean.

Concurrent sampling of freshwater (lakes and rivers), seawater, snow, air, and zooplankton for a range of legacy polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) was undertaken in the Canadian High Arctic during ice-covered, melting, and ice-free conditions. Overall, there was a general trend of higher fluvial PCB/OCP concentrations associated with the spring snow melt (early-mid June), while much lower concentrations were detected during the snow-free season (end of July). In contrast, PCB concentrations in two Arctic lakes (West and East Lakes, Melville Island) and in ocean waters, sharply increased in the ice-free period, likely because of inputs from the ice/snow layer melting and river runoff. The resulting air-water fugacity ratios and fluxes followed a remarkable shift during the sampling campaign. PCBs and OCPs shifted from equilibrium during ice/snow-covered conditions toward a clear net volatilization of PCBs and most of the OCPs during snow/ice-free conditions. Differences in the bioaccumulation factor for PCB/OCPs in zooplankton between West and East Lakes were observed, likely because of zooplankton being exposed to more contaminated food in West Lake due to higher turbidity related to in-lake disturbances.

Legacy and Emerging Persistent Organic Pollutants (POPs) in Terrestrial Compartments in the High Arctic: Sorption and Secondary Sources.

Legacy persistent organic pollutants (POPs) such as polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs), and emerging perfluoroalkyl substances (PFASs) were measured in vegetation and soil samples collected at remote lakes in the Canadian High Arctic. Field studies were carried out in 2015 and 2016 to assess concentrations of POPs, study the relevant sorbing phases, and determine whether Arctic soils were sinks or sources of legacy POPs to the atmosphere and to neighboring lakes. The patterns of legacy POPs in vegetation and soils were dominated by low molecular weight PCB congeners along with OCPs, confirming the importance of long-range atmospheric transport. Lipid and non-lipid organic matter was a key determinant of legacy POPs in Arctic vegetation. Soil organic matter was the main descriptor of hydrophobic PCBs and OCPs in soils, while soil inorganic carbon content, was an important driver of the sorption of PFASs in soils. While contaminant concentrations were low in soil and vegetation, higher PCBs and PFOS organic and inorganic carbon-normalized concentrations were found at Resolute Lake indicating the presence of local sources of contamination. Comparison of fugacities of PCBs in soil and air from Resolute Lake indicated soils as net sources of PCBs to the atmosphere.

The world's largest High Arctic lake responds rapidly to climate warming.

Using a whole-watershed approach and a combination of historical, contemporary, modeled and paleolimnological datasets, we show that the High Arctic's largest lake by volume (Lake Hazen) has succumbed to climate warming with only a ~1 °C relative increase in summer air temperatures. This warming deepened the soil active layer and triggered large mass losses from the watershed's glaciers, resulting in a ~10 times increase in delivery of glacial meltwaters, sediment, organic carbon and legacy contaminants to Lake Hazen, a >70% decrease in lake water residence time, and near certainty of summer ice-free conditions. Concomitantly, the community assemblage of diatom primary producers in the lake shifted dramatically with declining ice cover, from shoreline benthic to open-water planktonic species, and the physiological condition of the only fish species in the lake, Arctic Char, declined significantly. Collectively, these changes place Lake Hazen in a biogeochemical, limnological and ecological regime unprecedented within the past ~300 years.

Differences in Riverine and Pond Water Dissolved Organic Matter Composition and Sources in Canadian High Arctic Watersheds Affected by Active Layer Detachments.

Regional warming has caused permafrost thermokarst and disturbances, such as active layer detachments (ALDs), which may alter carbon feedback in Arctic ecosystems. However, it is currently unclear how these disturbances alter DOM biogeochemistry in rivers and ponds in Arctic ecosystems. Water samples from the main river channel, ALD-disturbed/undisturbed tributaries, and disturbed/undisturbed ponds within a catchment in the Canadian High Arctic were collected and analyzed using carbon isotopes and spectroscopic methods. Both river and pond samples had large variations in dissolved organic carbon (DOC) concentrations. Ponds, particularly ALD-disturbed ponds, had much older 14C DOC ages than rivers. Results from δ13C and absorption and fluorescence analyses indicate higher autochthonous contributions in ponds than rivers and increasing autochthonous contributions from upper to lower reaches of the main channel. The disturbed samples had less carbohydrates but more carboxyl-rich alicyclic molecules in 1H nuclear magnetic resonance spectra than undisturbed samples. These ALD-impacted samples also contained less terrestrial-humic-like but more oxidized-quinone-like components in the fluorescence spectra. Interestingly, the disturbed pond DOM displayed the greatest DOM oxidation with ALDs compared to undisturbed areas. Compared to Arctic rivers, small Arctic ponds have DOM predominantly from permafrost and microbial sources and may have a disproportionally stronger positive feedback on climate warming.

Climate change and mercury accumulation in Canadian high and subarctic lakes.

Mercury (Hg) profiles were compared to profiles of climate indicators including microfossil remains and algal-derived or S2 carbon (C) in dated sediment cores from 14 lakes spanning latitudinal and longitudinal gradients across the Canadian high and subarctic. Hg fluxes increased postindustrialization (post-∼1850) in 11 of these lakes (postindustrialization Hg fluxes (ΔHgF(F)) = 2-24 µg m(-2) y(-1)). Correction of HgF(F) for catchment contributions demonstrated that Hg deposition originating from catchment-independent factors, such as atmospheric deposition, increased since industrialization in all 14 lakes. Several of these lakes also showed postindustrial shifts in algal assemblages consistent with climate-induced changes. Eleven lakes showed post-1850s increases in S2F(F), suggesting that lake primary productivity has recently increased in the majority of our sites (ΔS2F(F) = 0.1-4 g m(-2) y(-1)). Other studies have interpreted significant relationships between Hg:S2 concentrations in Arctic sediment as support for the algal scavenging hypothesis, which postulates that Hg fluxes to Arctic sediments are largely driven by S2. However, in six of our lakes we observed no Hg:S2 relationship, and in one lake a significant negative Hg:S2 relationship was observed due to increased Hg and decreased S2 C deposition during the postindustrialization period. In six of the seven lakes where a significant positive Hg:S2 relationship was observed, algal assemblages either did not change through time or the timing of the shifts did not correspond to changes in Hg deposition. Our results demonstrate that, although Arctic lakes are experiencing a myriad of changes, including increased Hg and S2 deposition or changing algal assemblages, increased lake primary productivity does not appear to be driving changes in Hg fluxes to sediments.

Arctic permafrost active layer detachments stimulate microbial activity and degradation of soil organic matter.

Large quantities of soil organic carbon in Arctic permafrost zones are becoming increasingly unstable due to a warming climate. High temperatures and substantial rainfall in July 2007 in the Canadian High Arctic resulted in permafrost active layer detachments (ALDs) that redistributed soils throughout a small watershed in Nunavut, Canada. Molecular biomarkers and NMR spectroscopy were used to measure how ALDs may lead to microbial activity and decomposition of previously unavailable soil organic matter (SOM). Increased concentrations of extracted bacterial phospholipid fatty acids (PLFAs) and large contributions from bacterial protein/peptides in the NMR spectra at recent ALDs suggest increased microbial activity. PLFAs were appreciably depleted in a soil sample where ALDs occurred prior to 2003. However an enrichment of bacterial derived peptidoglycan was observed by (1)H-(13)C heteronuclear multiple quantum coherence (HMQC) and (1)H diffusion edited (DE) NMR and enhanced SOM degradation was observed by (13)C solid-state NMR. These data suggest that a previous rise in microbial activity, as is currently underway at the recent ALD site, led to degradation and depletion of labile SOM components. Therefore, this study indicates that ALDs may amplify climate change due to the release of labile SOM substrates from thawing High Arctic permafrost.