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.

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.

Peace-Athabasca Delta (PAD), northeastern Alberta. Potential for downstream delivery of contaminants via Athabasca River floodwaters to lakes of the PAD has raised local to international concern. Here, we quantify enrichment of eight metals (Be, Cd, Cr, Cu, Ni, Pb, V, Zn) in aquatic biota, relative to sediment-based pre-industrial baselines, via analysis of biofilm-sediment mixtures accrued on artificial substrate samplers deployed during summers of 2017 and 2018 in > 40 lakes. Widespread flooding in the southern portion of the delta in spring 2018 allows for assessment of metal enrichment by Athabasca River floodwaters. River floodwaters are not implicated as a pathway of metal enrichment to biofilm-sediment mixtures in PAD lakes from upstream sources. MANOVA tests revealed no significant difference in residual concentrations of all eight metals in lakes that did not flood versus lakes that flooded during one or both study years. Also, no enrichment was detected for concentrations of biologically inert metals (Be, Cr, Pb) and those related to oil-sands development (Ni, V). Enrichment of Cd, Cu, and Zn at non-flooded lakes, however, suggests uptake of biologically active metals complicates comparisons of organic-rich biofilm-sediment mixtures to sediment-derived baselines for these metals. Results demonstrate that this novel approach could be adopted for lake monitoring within the federal Action Plan. • Oil sands monitoring of lakes in the Peace-Athabasca Delta needs pre-disturbance data. • Study compares [metals] in biofilm-sediment to [metals] in pre-1920 lake sediment. • Athabasca River floodwaters not implicated as pathway for metal enrichment. • Monitoring framework contributes to Wood Buffalo National Park Action Plan.

Peace-Athabasca Delta (PAD), northeastern Alberta. Potential for downstream delivery of contaminants via Athabasca River floodwaters to lakes of the PAD has raised local to international concern. Here, we quantify enrichment of eight metals (Be, Cd, Cr, Cu, Ni, Pb, V, Zn) in aquatic biota, relative to sediment-based pre-industrial baselines, via analysis of biofilm-sediment mixtures accrued on artificial substrate samplers deployed during summers of 2017 and 2018 in > 40 lakes. Widespread flooding in the southern portion of the delta in spring 2018 allows for assessment of metal enrichment by Athabasca River floodwaters. River floodwaters are not implicated as a pathway of metal enrichment to biofilm-sediment mixtures in PAD lakes from upstream sources. MANOVA tests revealed no significant difference in residual concentrations of all eight metals in lakes that did not flood versus lakes that flooded during one or both study years. Also, no enrichment was detected for concentrations of biologically inert metals (Be, Cr, Pb) and those related to oil-sands development (Ni, V). Enrichment of Cd, Cu, and Zn at non-flooded lakes, however, suggests uptake of biologically active metals complicates comparisons of organic-rich biofilm-sediment mixtures to sediment-derived baselines for these metals. Results demonstrate that this novel approach could be adopted for lake monitoring within the federal Action Plan. • Oil sands monitoring of lakes in the Peace-Athabasca Delta needs pre-disturbance data. • Study compares [metals] in biofilm-sediment to [metals] in pre-1920 lake sediment. • Athabasca River floodwaters not implicated as pathway for metal enrichment. • Monitoring framework contributes to Wood Buffalo National Park Action Plan.