Abundant reserves of metals and oil have spurred large-scale mining developments across northwestern Canada during the past 80 years. Historically, the associated emissions footprint of hazardous metal(loid)s has been difficult to identify, in part, because monitoring records are too short and sparse to have characterized their natural concentrations before mining began. Stratigraphic analysis of lake sediment cores has been employed where concerns of pollution exist to determine pre-disturbance metal(loid) concentrations and quantify the degree of enrichment since mining began. Here, we synthesize the current state of knowledge via systematic re-analysis of temporal variation in sediment metal(loid) concentrations from 51 lakes across four key regions spanning 670 km from bitumen mining in the Alberta Oil Sands Region (AOSR) to gold mining (Giant and Con mines) at Yellowknife in central Northwest Territories. Our compilation includes upland and floodplain lakes at varying distances from the mines to evaluate dispersal of pollution-indicator metal(loid)s from bitumen (vanadium and nickel) and gold mining (arsenic and antimony) via atmospheric and fluvial pathways. Results demonstrate ‘severe’ enrichment of vanadium and nickel at near-field sites (≤20 km) within the AOSR and ‘severe’ (near-field; ≤ 40 km) to ‘considerable’ (far-field; 40–80 km) enrichment of arsenic and antimony due to gold mining at Yellowknife via atmospheric pathways, but no evidence of enrichment of vanadium or nickel via atmospheric or fluvial pathways at the Peace-Athabasca Delta and Slave River Delta. Findings can be used by decision makers to evaluate risks associated with contaminant dispersal by the large-scale mining activities. In addition, we reflect upon methodological approaches to be considered when evaluating paleolimnological data for evidence of anthropogenic contributions to metal(loid) deposition and advocate for proactive inclusion of paleolimnology in the early design stage of environmental contaminant monitoring programs.

Exploitation of bitumen-rich deposits in the Alberta Oil Sands Region (AOSR) by large-scale mining and processing activities has generated widespread concern about the potential for dispersal of harmful contaminants to aquatic ecosystems via fluvial and atmospheric pathways. The release of mercury has received attention because it is a potent neurotoxin for wildlife and humans. However, knowledge of baseline mercury concentration prior to disturbance is required to evaluate the extent to which oil sands development has contributed mercury to aquatic ecosystems. Here, we use stratigraphic analysis of total mercury concentration ([THg]) in radiometrically dated sediment cores from nine floodplain lakes in the AOSR and downstream Peace-Athabasca Delta (PAD) and two upland lakes in the PAD region to establish pre-1900 baseline [THg] and evaluate if [THg] has become enriched via fluvial and atmospheric pathways since oil sands mining and processing began in 1967. Concentrations of THg in sediment cores from the study lakes range from 0.022–0.096 mg/kg (dry wt.) and are below the Canadian interim sediment quality guidelines for freshwater (0.17 mg/kg). Results demonstrate no enrichment of [THg] above pre-1900 baseline via fluvial pathways at floodplain lakes in the AOSR or PAD. Enrichment of [THg] was detected via atmospheric pathways at upland lakes in the PAD region, but this occurred prior to oil sands development and aligns with long-range transport of emissions from coal combustion and other anthropogenic sources across the northern hemisphere recognized in many other lake sediment records. The inventory of anthropogenic [THg] in the upland lakes in the AOSR is less than at the Experimental Lakes Area of northwestern Ontario (Canada), widely regarded as a “pristine” area. The absence of enrichment of [THg] in lake sediment via fluvial pathways is a critical finding for stakeholders, and we recommend that monitoring at the floodplain lakes be used to inform stewardship as oil sands operators prepare to discharge treated oil sands process waters directly into the Athabasca River upstream of the PAD.

• Lack of pre-industrial baseline data hampers assessment of oil sands river pollution. • We analyzed metals concentrations in cores of Athabasca Delta floodplain lakes. • No enrichment was detected for metals associated with oil sands development. • Results inform decision on World Heritage status of Wood Buffalo National Park. • A framework has been established for ongoing aquatic ecosystem monitoring. Sediment quality monitoring is widely used to quantify extent of river pollution, but requires knowledge of pre-disturbance conditions in the potentially altered landscape. This has long been identified as a critical aspect to develop for addressing concerns of river pollution in the Alberta Oil Sands Region. Here, we use analyses of sediment cores from eight floodplain lakes spanning a 67 river-km transect across the Athabasca Delta to define pre-1920 (pre-industrial) baseline concentrations for vanadium and five primary pollutants. We then evaluate if sediment metals concentrations have become enriched above baseline since onset of oil sands development and other industrial activities. Results demonstrate no enrichment of metals concentrations (except zinc at one lake) and absence of consistent temporal increases above pre-industrial baselines. Thus, natural processes continue to dominate metal deposition in floodplain lakes of the Athabasca Delta -- an important finding to inform stewardship decisions. The pre-1920 metals concentrations baselines offer a useful tool for ongoing sediment monitoring in aquatic ecosystems of the Athabasca Delta.

Climate‐driven decline in freshwater supplied by rivers draining the hydrographic apex of western North America has ramifications for downstream ecosystems and society. For the Peace‐Athabasca Delta (PAD), floods from the Peace and Athabasca rivers are critical for sustaining abundant shallow water habitat, but their frequency has been in decline for decades over much of its area. Here, we assess current hydrological and limnological status in the PAD by integrating spatial and temporal data. Analysis of water isotope compositions and water chemistry measured at numerous lakes across the delta shows that hydro‐limnological effects of the large‐scale ice‐jam flood event of 2014 failed to persist beyond the early ice‐free season of 2015. Isotope‐inferred paleohydrological records from five hydrologically representative lakes in the PAD indicate that periodic desiccation during the Little Ice Age occurred at the most elevated basin in response to locally arid climatic conditions, yet other lower elevation sites were influenced by high water level on Lake Athabasca owing to increased snowmelt‐ and glacier‐derived river discharge. In contrast, water isotope data during the past 15 yr at all five lakes consistently document the strong role of evaporation, a trend which began in the early to mid‐20th century according to sediment records and is indicative of widespread aridity unprecedented during the past 400 yr. We suggest that integration of hydrological and limnological approaches over space and time is needed to inform assessment of contemporary lake conditions in large, complex floodplain landscapes.