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.

Gold mining operations near Yellowknife (Northwest Territories, Canada) released vast quantities of arsenic trioxide during the 1950s, which dispersed across the landscape. Contemporary measurements of arsenic concentrations in lake water and surficial sediment identify enrichment within a 30 km radius. However, paleolimnological studies have identified possible evidence of mining influence during the 1950s at a lake beyond this distance, suggesting a more expansive legacy footprint may exist. Here, we analyze spatiotemporal patterns of arsenic, antimony, and lead deposition from sediment cores at lakes located 10–40 km (near-field) and 50–80 km (far-field) from the mines along the prevailing northwesterly wind direction (NW) and 20–40 km to the northeast (NE) of the mines to improve characterization of the legacy footprint of emissions. We build upon previous findings to determine if: 1) there is evidence of mine-related pollutants beyond the well-established 30 km radius and 2) enrichment is greatest in the prevailing wind direction, as expected for aerial dispersion from a point source of emissions. Results demonstrate enrichment since the 1950s for arsenic and antimony at least as far as 80 km to the NW and 40 km to the NE, thus legacy deposition extended beyond the currently defined 30 km radius ‘zone of immediate influence’. Concentrations, enrichment factors, and total excess inventories of arsenic and antimony decline with distance from the mines and are greater along the prevailing (NW) than orthogonal (NE) wind direction. Peak concentrations in uppermost sediment strata at near-field lakes in the prevailing wind direction suggest supply of arsenic and antimony remains high from legacy stores in the catchment and lake sediment profiles >60 years after emissions were released. Such lasting influence of legacy emissions likely is not limited to mines in the Yellowknife region, and paleolimnological approaches can effectively delineate zones of past and ongoing pollution from legacy sources elsewhere. • We analyze metals in sediment cores to track dispersal of legacy mine emissions. • Enrichment of As and Sb evident beyond known 30-km radius pollution zone. • Distance from source and wind direction influenced contaminant dispersal. • Enriched surface sediments within 30 km suggest ongoing delivery of legacy metals.

• 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.

Abstract Well-designed monitoring approaches are needed to assess effects of industrial development on downstream aquatic environments and guide environmental stewardship. Here, we develop and apply a monitoring approach to detect potential enrichment of metals concentrations in surficial lake sediments of the Peace-Athabasca Delta (PAD), northern Alberta, Canada. Since the ecological integrity of the PAD is strongly tied to river floodwaters that replenish lakes in the delta, and the PAD is located downstream of the Alberta oil sands, concerns have been raised over the potential transport of industry-supplied metals to the PAD via the Athabasca River. Surface sediment samples were collected in September 2017 from 61 lakes across the delta, and again in July 2018 from 20 of the same lakes that had received river floodwaters 2 months earlier, to provide snapshots of metals concentrations (Be, Cd, Cr, Cu, Ni, Pb, V, and Zn) that have recently accumulated in these lakes. To assess for anthropogenic enrichment, surficial sediment metals concentrations were normalized to aluminum and compared to pre-industrial baseline (i.e., reference) metal-aluminum linear relations for the Athabasca and Peace sectors of the PAD developed from pre-1920 measurements in lake sediment cores. Numerical analysis demonstrates no marked enrichment of these metals concentrations above pre-1920 baselines despite strong ability (> 99% power) to detect enrichment of 10%. Measurements of river sediment collected by the Regional Aquatics- and Oil Sands-Monitoring Programs (RAMP/OSM) also did not exceed pre-1920 concentrations. Thus, results presented here show no evidence of substantial oil sands-derived metals enrichment of sediment supplied by the Athabasca River to lakes in the PAD and demonstrate the usefulness of these methods as a monitoring framework.

Opposing interpretations of Lower Peace River ice-jam flood frequency data sets are at the centre of identifying causes of reduced freshwater availability in the Peace-Athabasca Delta (northern Alberta), a Ramsar Wetland of International Importance and a major contributor to Wood Buffalo National Park’s listing as a UNESCO World Heritage Site. Recently, conclusions drawn from statistical inference of traditional knowledge and historical observation sources suggested that flood frequency was accelerating during 1880–1967 and then declined coincident with hydroelectric regulation of Peace River flow since 1968 that altered the river’s hydrograph. In contrast, prior paleolimnological measurements of laminated sediments from oxbow lakes proximal to the Peace River have, along with alternate presentation of the traditional knowledge and historical observation sources, identified flood frequency was in decline for decades preceding river regulation due to climate change since the Little Ice Age. Here we revisit these data sets and, specifically, review their inherent uncertainties to assess their value and limitations. The notion of increasing versus decreasing flood frequency in the decades preceding river regulation (1880–1967) is tested using previously published paleohydrological records from perched lakes in the delta. Those records from lakes most proximal and sensitive to changes in the flow regime of the Peace River show increasing influence of lake evaporation during 1880–1967, consistent with long-term decline in flood frequency. Reconciling uncertainties of multiple lines-of-evidence and their findings should inform decisions by UNESCO on the World Heritage status of Wood Buffalo National Park and execution of the park’s federally funded Action Plan. New paleolimnological studies that have recently been launched will continue to probe the hydrological history of the Peace-Athabasca Delta to serve as a foundation for effective stewardship.

The late John Glew contributed valuable equipment to the paleolimnology community for successful collection and processing of cores of sediment from aquatic ecosystems. Unfortunately, tubes that fit his hammer-gravity corer design are no longer conveniently available for purchase and, with his sudden passing, Glew gravity and coring equipment is difficult or impossible to access. In some field-sampling situations, other commercially available equipment present limitations. Here, we provide an updated design of the Glew gravity corer which accommodates a hammer-percussion instrument and overcomes limitations we have encountered when coring lakes in remote locations from floats of a helicopter or small, inflatable watercraft. Our approach integrates the ‘best of both worlds’ provided by the Glew and commercially available Uwitec designs, using readily available components. We updated the Glew corer tube collar to be compatible with standard, commercially available 90-mm external diameter (86-mm internal diameter) PVC tubing that fits Uwitec components (e.g., Uwitec rubber ‘piston’ and ‘stoppers’; using terminology of the Uwitec catalogue), and designed a spring-loaded gasket-style plunger that achieves greater suction than the standard Glew designs. We also updated the Glew vertical sectioner to be compatible with 90-mm-diameter core tubes typically ranging from 60–120 cm long. An outcome is consolidation of the Uwitec and Glew gravity coring systems, which has allowed for interchangeability and choice among use of original and hammer-driven Glew, Uwitec, and the new hybrid ‘Uwi-Glew-ee’ gravity corer and sectioner configurations, depending on logistical constraints of fieldwork and anticipated lake sediment composition. The parts and systems are available from University of Waterloo’s Science Technical Services (https://uwaterloo.ca/science-technical-services/).

Lake 227 of the Experimental Lakes Area (ELA) in Ontario, Canada, has been fertilized with phosphorus (P) since 1969, which resulted in a rapid transition from oligotrophic to eutrophic conditions. Sediment cores collected from the oxygenated epilimnion, and the mostly anoxic hypolimnion of this unique lake contain a historical record of the changes in sediment P speciation and burial rates across the trophic transition. To elucidate these changes, results of chemical extractions were combined with 210Pb sediment dating, and with 31P NMR, Mossbauer, and XANES spectroscopies. Prior to 1969, organic P (POrg) was the major sedimentary P sink in Lake 227. Eutrophication of the lake coincided with marked increases in the burial rate of total P (TP), as well as in the relative contribution of the NaHCO3-extractable P pool (humic-bound P, PHum). Together, PHum and POrg account for ≥70% of total P burial in the sediments deposited since artificial fertilization started. The PHum fraction likely comprises phosphate complexes with humic substances. The strong linear correlation between P and iron (Fe) extracted by NaHCO3 implies a close association of the two elements in the humic fraction. Mossbauer and XANES spectra further indicate that most Fe in the post-1969 sediments remained in the Fe (III) oxidation state, which is attributed to the stabilization of reducible Fe by organic matter, in part via the formation of phosphate-Fe (III)-humic complexes. Importantly, our results show that the eutrophication experimentation of Lake 227 caused the accumulation of a large reservoir of reactive sediment P, which may continue to fuel internal P loading to the water column once artificial fertilization is terminated.

Hydrological monitoring in complex, dynamic northern floodplain landscapes is challenging, but increasingly important as a consequence of multiple stressors. The Peace‐Athabasca Delta in northern Alberta, Canada, is a Ramsar Wetland of International Importance reliant on episodic river ice‐jam flood events to recharge abundant perched lakes and wetlands. Improved and systematic monitoring of landscape‐scale hydrological connectivity among freshwater ecosystems (rivers, channels, wetlands, and lakes) is needed to guide stewardship decisions in the face of climate change and upstream industrial development. Here, we use water isotope compositions, supplemented by measurements of specific conductivity and field observations, from 68 lakes and 9 river sites in May 2018 to delineate the extent and magnitude of spring ice‐jam induced flooding along the Peace and Athabasca rivers. Lake‐specific estimates of input water isotope composition (δI) were modelled after accounting for influence of evaporative isotopic enrichment. Then, using the distinct isotopic signature of input water sources, we develop a set of binary mixing models and estimate the proportion of input to flooded lakes attributable to river floodwater and precipitation (snow or rain). This approach allowed identification of areas and magnitude of flooding that were not captured by other methods, including direct observations from flyovers, and to demarcate flow pathways in the delta. We demonstrate water isotope tracers as an efficient and effective monitoring tool for delineating spatial extent and magnitude of an important hydrological process and elucidating connectivity in the Peace‐Athabasca Delta, an approach that can be readily adopted at other floodplain landscapes.

[1] Previous studies of river hydrometric records and Indigenous Knowledge holders claim that flood-induced recharge of ecologically important perched basins decreased across the Peace-Athabasca Delta after 1968 due mainly to hydroelectric regulation of Peace River flow. Natural deltaic processes and climate are acknowledged as additional, lesser contributors, but are challenging to evaluate. We use sediment records spanning ∼115 years from nine perched basins across the Athabasca Delta to test if unidirectional drying coincides with river regulation. Results show bi-directional hydrological changes since the early 1980s, not 1968, to reduced flooding in areas east of the Embarras River confluence with Cree/Mamawi creeks and increased flooding northward along the Cree/Mamawi distributary. The timing and pattern pinpoint the 1982 Embarras Breakthrough, a natural avulsion that diverted flow northward and away from the Athabasca Delta terminus, as the principal cause. The results demonstrate the need to factor natural deltaic processes into impending decisions on the delta’s UNESCO World Heritage status and implementation of a federal Action Plan to mitigate widespread drying.