title: Isotopic Evidence for Oil Sands Petroleum Coke in the Peace-Athabasca Delta.
abstract: The continued growth of mining and upgrading activities in Canada's Athabasca oil sands (AOS) region has led to concerns about emissions of contaminants such as polycyclic aromatic hydrocarbons (PAHs). Whereas a recent increase in PAH emissions has been demonstrated within around 50 km of the main center of surface mining and upgrading operations, the exact nature of the predominant source(s) and the geographical extent of the deposition are still under debate. Here, we report a century-long source apportionment of PAHs using dual (δ(2)H, δ(13)C) compound-specific isotope analysis on phenanthrene deposited in a lake from the Athabasca sector of the Peace-Athabasca Delta situated ∼150 km downstream (north) of the main center of mining operations. The isotopic signatures in the core were compared to those of the main potential sources in this region (i.e., unprocessed AOS bitumen, upgrader residual coke, forest fires, coal, gasoline and diesel soot). A significant concurrent increase (∼55.0‰) in δ(2)H and decrease (∼1.5‰) in δ(13)C of phenanthrene over the last three decades pointed to an increasingly greater component of petcoke-derived PAHs. This study is the first to quantify long-range (i.e., >100 km) transport of a previously under-considered anthropogenic PAH source in the AOS region.
authors.affiliation: INRS Eau Terre Environnement , Québec, Québec G1K 9A9, Canada.
authors.forename: Josué J
authors.initials: JJ
authors.lastname: Jautzy
authors.affiliation: Geological Survey of Canada, Natural Resources Canada , Québec, Québec G1K 9A9, Canada.
authors.forename: Jason M E
authors.initials: JM
authors.lastname: Ahad
authors.affiliation: INRS Eau Terre Environnement , Québec, Québec G1K 9A9, Canada.
authors.forename: Charles
authors.initials: C
authors.lastname: Gobeil
authors.affiliation: Geological Survey of Canada, Natural Resources Canada , Québec, Québec G1K 9A9, Canada.
authors.forename: Anna
authors.initials: A
authors.lastname: Smirnoff
authors.affiliation: INRS Eau Terre Environnement , Québec, Québec G1K 9A9, Canada.
authors.forename: Benjamin D
authors.initials: BD
authors.lastname: Barst
authors.affiliation: Geological Survey of Canada, Natural Resources Canada , Québec, Québec G1K 9A9, Canada.
authors.forename: Martine M
authors.initials: MM
authors.lastname: Savard
mesh_terms: D000416:Alberta; D002247:Carbon Isotopes / Q000032:analysis; D003031:Coal; D004784:Environmental Monitoring / Q000379:methods*; D006838:Hydrocarbons; D060106:Lakes / Q000032:analysis*; D061329:Oil and Gas Fields; D010578:Petroleum / Q000032:analysis; D010616:Phenanthrenes / Q000032:analysis; D011084:Polycyclic Aromatic Hydrocarbons / Q000032:analysis*; D014874:Water Pollutants, Chemical / Q000032:analysis
chemical_list: D002247:Carbon Isotopes; D003031:Coal; D006838:Hydrocarbons; D010578:Petroleum; D010616:Phenanthrenes; D011084:Polycyclic Aromatic Hydrocarbons; D014874:Water Pollutants, Chemical; C031181:phenanthrene; C006647:asphalt