Impact of Athabasca oil sands operations on mercury levels in air and deposition

Oil sands upgrading facilities in the Athabasca oil sands region (AOSR) in Alberta, Canada, have been reporting mercury (Hg) emissions to public government databases (National Pollutant Release Inventory (NPRI)) since the year 2000, yet the relative contribution of these emissions to ambient Hg deposition remains unknown. The impact of oil sands emissions (OSE) on Hg levels in and around the AOSR, relative to contributions from global (anthropogenic, geogenic and legacy) emissions and regional biomass burning emissions (BBE), was assessed using a global 3D-process-based Hg model, GEM-MACH-Hg, from 2012 to 2015. In addition, the relative importance of year-to-year changes in Hg emissions from the above sources and meteorological conditions to inter-annual variations in Hg deposition was examined. Surface air concentrations of Hg species and annual snowpack Hg loadings simulated by the model were found comparable to measured levels in the AOSR, suggesting consistency between reported Hg emissions from oil sands activities and Hg levels in the region. As a result of global-scale transport and the long lifetime of gaseous elemental Hg (Hg(0)), surface air concentrations of Hg(0) in the AOSR reflected the background Hg(0) levels in Canada. By comparison, average air concentrations of total oxidized Hg (efficiently deposited Hg species) in the AOSR were elevated up to 60 % within 50 km of the oil sands Hg emission sources. Hg emissions from wildfire events led to episodes of high ambient Hg(0) concentrations and deposition enrichments in northern Alberta, including the AOSR, during the burning season. Hg deposition fluxes in the AOSR were within the range of the deposition fluxes measured for the entire province of Alberta. On a broad spatial scale, contribution from imported Hg from global sources dominated the annual background Hg deposition in the AOSR, with present-day global anthropogenic emissions contributing to 40 % (< 1 % from Canada excluding OSE) and geogenic and legacy emissions contributing to 60 % of the background Hg deposition. In contrast, oil sands Hg emissions were responsible for significant enhancements in Hg deposition in the immediate vicinity of oil sands Hg emission sources, which were ∼ 10 times larger in winter than summer (250 %–350 % in winter and ∼ 35 % in summer within 10 km of OSE, 2012–2013). The spatial extent of the influence of oil sands emissions on Hg deposition was also greater in winter relative to summer (∼ 100 km vs. 30 km from Hg-emitting facilities). In addition, inter-annual changes in meteorological conditions and oil sands emissions also led to significantly higher inter-annual variations in wintertime Hg deposition compared to summer. In 2015, within 10 km of major oil sands sources, relative to 2012, Hg deposition declined by 46 % in winter but 22 % annually, due to a larger OSE-led reduction in wintertime deposition. Inter-annual variations in meteorological conditions were found to both exacerbate and diminish the impacts of OSE on Hg deposition in the AOSR, which can confound the interpretation of trends in short-term environmental Hg monitoring data. Hg runoff in spring flood, comprising the majority of annual Hg runoff, is mainly derived from seasonal snowpack Hg loadings and mobilization of Hg deposited in surface soils, both of which are sensitive to Hg emissions from oil sands developments in the proximity of sources. Model results suggest that sustained efforts to reduce anthropogenic Hg emissions from both global and oil sands sources are required to reduce Hg deposition in the AOSR.

Hydrogeochemistry Studies in the Oil Sands Region to Investigate the Role of Terrain Connectivity in Nitrogen Critical Loads

Hydrology and geochemistry studies were conducted in the Athabasca Oil Sands region to better understand the water and nitrogen cycles at two selected sites in order to assess the potential for nitrogen transport between adjacent terrain units. A bog—poor fen—upland system was instrumented near Mariana Lakes (ML) (55.899° N, 112.090° W) and a rich fen—upland system was instrumented at JPH (57.122° N, 111.444° W), 100 km south and 45 km north of Fort McMurray, Alberta respectively. LiDAR surveys were initially conducted to delineate the watershed boundaries and topography and to select a range of specific locations for the installation of water table wells and groundwater piezometers. Field work, which included a range of physical measurements as well as water sampling for geochemical and isotopic characterization, was carried out mainly during the thaw seasons of 2011 to 2015. From analysis of the runoff response and nitrogen species abundances we estimate that nitrogen exchange between the wetlands and adjacent terrain units ranged between 2.2 and −3.1 kg/ha/year for rich fens, 0.6 to −1.1 kg/ha/year for poor fens, and between 0.6 and −2.5 kg/ha/year for bogs, predominantly via surface pathways and in the form of dissolved nitrate. A significant storage of dissolved ammonium (and also dissolved organic nitrogen) was found within the pore water of the bog-fen complex at Mariana Lakes, which we attribute to decomposition, although it is likely immobile under current hydrologic conditions, as suggested by tritium distributions. In comparison with the experimental loads of between 5 and 25 kg/ha/year, the potential nitrogen exchange with adjacent terrain units is expected to have only a minor or negligible influence, and is therefore of secondary importance for defining critical loads across the regional landscape. Climate change and development impacts may lead to significant mobilization of nitrogen storages, although more research is required to quantify the potential effects on local ecosystems.

Using carbon-14 and carbon-13 measurements for source attribution of atmospheric methane in the Athabasca Oil Sands Region

The rapidly expanding and energy intensive production from the Canadian oil sands, one of the largest oil reserves globally, accounts for almost 12 % of Canada’s greenhouse gas emissions according to inventories. Developing approaches for evaluating reported methane (CH4) emission is crucial for developing effective mitigation policies, but only one study has characterized CH4 sources in the Athabasca Oil Sands Region (AOSR). We tested the use of 14C and 13C carbon isotope measurements in ambient CH4 from the AOSR to estimate source contributions from key regional CH4 sources: (1) tailings ponds, (2) surface mines and processing facilities, and (3) wetlands. The isotopic signatures of ambient CH4 indicate that the CH4 enrichments measured at the site were mainly influenced by fossil CH4 emissions from surface mining and processing facilities (53 ± 18 %), followed by fossil CH4 emissions from tailings ponds (36 ± 18 %), and to a lesser extent by modern CH4 emissions from wetlands (10 < 1 %). Our results confirm the importance of tailings ponds in regional CH4 emissions and show that this method can successfully separate wetland CH4 emissions. In the future, the isotopic characterization of CH4 sources, and measurements from different seasons and wind directions are needed to provide a better source attribution in the AOSR.