Abstract
We examined polycyclic aromatic compounds (PACs) and petroleum biomarkers (steranes, hopanes, and terpanes) in radiometrically-dated lake sediment cores from the Athabasca oil sands region (AOSR) and the Peace-Athabasca Delta (PAD) region in Alberta (Canada) to determine whether contributions from petroleum hydrocarbons have changed over time. Two floodplain lakes in the PAD (PAD 30, PAD 31) recorded increased flux of alkylated PACs and increased petrogenic (petroleum-derived) hydrocarbons after ∼1980, coincident with a decline of sediment organic carbon content and a rise of bulk sedimentation rate, likely due to increased Athabasca River flow. A large expansion of upstream oilsands mining, upgrading, and refining may also have contributed to the observed shift to more petrogenic hydrocarbons to sediments since the 1980s. Alkylated PAC flux increased in the floodplain lake analyzed within the AOSR (Saline Lake) since the 1970s–1980s, coincident with a sharp rise in sediment organic carbon content and increased contributions of petrogenic hydrocarbons. These changes identify increased supply of petrogenic PACs occurred as Athabasca River floodwaters waned, and may implicate aerial contributions of petrogenic hydrocarbons from oilsands activity. PACs and petroleum biomarkers (steranes, hopanes, and terpanes) in sediment cores from Saline Lake, PAD 30 and PAD 31 revealed a predominance of petrogenic hydrocarbons in these lakes. In contrast, we recorded minimal petrogenic hydrocarbons in the reference lakes outside the surface minable area of the AOSR and PAD (Mariana Lake and BM11), though we noted slight increases in petrogenic contributions to modern (2010–2016) sediments. We show how a combined analysis of PACs and petroleum biomarkers in sediments is useful to quantify petrogenic contributions to lakes with added confidence and highlight the potential for petroleum biomarkers in lake sediment cores as a novel and effective method to track petroleum hydrocarbons in lake sediment.