The absence of well-executed environmental monitoring in the Athabasca oil sands (Alberta, Canada) has necessitated the use of indirect approaches to determine background conditions of freshwater ecosystems before development of one of the Earth’s largest energy deposits. Here, we use highly resolved lake sediment records to provide ecological context to ∼50 y of oil sands development and other environmental changes affecting lake ecosystems in the region. We show that polycyclic aromatic hydrocarbons (PAHs) within lake sediments, particularly C1-C4–alkylated PAHs, increased significantly after development of the bitumen resource began, followed by significant increases in dibenzothiophenes. Total PAH fluxes in the modern sediments of our six study lakes, including one site ∼90 km northwest of the major development area, are now ∼2.5–23 times greater than ∼1960 levels. PAH ratios indicate temporal shifts from primarily wood combustion to petrogenic sources that coincide with greater oil sands development. Canadian interim sediment quality guidelines for PAHs have been exceeded since the mid-1980s at the most impacted site. A paleoecological assessment of Daphnia shows that this sentinel zooplankter has not yet been negatively impacted by decades of high atmospheric PAH deposition. Rather, coincident with increases in PAHs, climate-induced shifts in aquatic primary production related to warmer and drier conditions are the primary environmental drivers producing marked daphniid shifts after ∼1960 to 1970. Because of the striking increase in PAHs, elevated primary production, and zooplankton changes, these oil sands lake ecosystems have entered new ecological states completely distinct from those of previous centuries.

Recent and historical deposition of mercury (Hg) was examined over a broad geographic area from southwestern Northwest Territories to Labrador and from the U.S. Northeast to northern Ellesmere Island using dated sediment cores from 50 lakes (18 in midlatitudes (41-50 degrees N), 14 subarctic (51-64 degrees N) and 18 in the Arctic (65-83 degrees N)). Distinct increases of Hg overtime were observed in 76% of Arctic, 86% of subarctic and 100% of midlatitude cores. Subsurface maxima in Hg depositional fluxes (microg m(-2) y(-1)) were observed in only 28% of midlatitude lakes and 18% of arctic lakes, indicating little recent reduction of inputs. Anthropogenic Hg fluxes adjusted for sediment focusing and changes in sedimentation rates (deltaF(adj,F)) ranged from -22.9 to 61 microg m(-2) y(-1) and were negatively correlated (r = -0.57, P < 0.001) with latitude. Hg flux ratios (FRs; post-1990)/pre-1850) ranged from 0.5 to 7.7. The latitudinal trend for Hg deltaF(adj,F) values showed excellent agreement with predictions of the global mercury model, GRAHM for the geographic location of each lake (r = 0.933, P < 0.001). The results are consistent with a scenario of slow atmospheric oxidation of mercury, and slow deposition of reactive mercury emissions, declining with increasing latitude away from emission sources in the midlatitudes, and support the view that there are significant anthropogenic Hg inputs in the Arctic.

Environmental context. Mercury, in its methylated form, is a neurotoxin that biomagnifies in marine and terrestrial foodwebs leading to elevated levels in fish and fish-eating mammals worldwide, including at numerous Arctic locations. Elevated mercury concentrations in Arctic country foods present a significant exposure risk to Arctic people. We present a detailed review of the fate of mercury in Arctic terrestrial and marine ecosystems, taking into account the extreme seasonality of Arctic ecosystems and the unique processes associated with sea ice and Arctic hydrology.Abstract. This review is the result of a series of multidisciplinary meetings organised by the Arctic Monitoring and Assessment Programme as part of their 2011 Assessment 'Mercury in the Arctic'. This paper presents the state-of-the-art knowledge on the environmental fate of mercury following its entry into the Arctic by oceanic, atmospheric and terrestrial pathways. Our focus is on the movement, transformation and bioaccumulation of Hg in aquatic (marine and fresh water) and terrestrial ecosystems. The processes most relevant to biological Hg uptake and the potential risk associated with Hg exposure in wildlife are emphasised. We present discussions of the chemical transformations of newly deposited or transported Hg in marine, fresh water and terrestrial environments and of the movement of Hg from air, soil and water environmental compartments into food webs. Methylation, a key process controlling the fate of Hg in most ecosystems, and the role of trophic processes in controlling Hg in higher order animals are also included. Case studies on Eastern Beaufort Sea beluga (Delphinapterus leucas) and landlocked Arctic char (Salvelinus alpinus) are presented as examples of the relationship between ecosystem trophic processes and biologic Hg levels. We examine whether atmospheric mercury depletion events (AMDEs) contribute to increased Hg levels in Arctic biota and provide information on the links between organic carbon and Hg speciation, dynamics and bioavailability. Long-term sequestration of Hg into non-biological archives is also addressed. The review concludes by identifying major knowledge gaps in our understanding, including:(1) the rates of Hg entry into marine and terrestrial ecosystems and the rates of inorganic and MeHg uptake by Arctic microbial and algal communities; (2) the bioavailable fraction of AMDE-related Hg and its rate of accumulation by biota and (3) the fresh water and marine MeHg cycle in the Arctic, especially the marine MeHg cycle.