scholarly journals Scavenging ratio of polycyclic aromatic compounds in rain and snow at the Athabasca oil sands region

2014 ◽  
Vol 14 (13) ◽  
pp. 19395-19429
Author(s):  
L. Zhang ◽  
I. Cheng ◽  
D. Muir ◽  
J.-P. Charland
Keyword(s):  
Gas Phase ◽  
Aromatic Compounds ◽  
Oil Sands ◽  
Polycyclic Aromatic Compounds ◽  
Particulate Phase ◽  
Athabasca Oil Sands ◽  
Polycyclic Aromatic ◽  
Alkylated Pahs ◽  
Snow Samples ◽  
Air Concentrations

Abstract. Athabasca oil sands industry in northern Alberta, Canada is a possible source of polycyclic aromatic compounds (PACs). Monitored PACs, including polycyclic aromatic hydrocarbons (PAHs), alkylated PAHs, and dibenzothiophenes, in precipitation and in air at three near-source sites in the Fort MacKay and Fort McMurray area during May 2011 to August 2012 were analyzed to generate a database of scavenging (or washout) ratios (Wt) for PACs scavenged by both snow and rain. Median precipitation and air concentrations of parent PAHs over the May 2011 to August 2012 period ranged from 0.3–184.9 (chrysene) ng L−1 and 0.01–3.9 (naphthalene) ng m−3, respectively, which were comparable to literature values. Higher concentrations in precipitation and air were observed for alkylated PAHs and dibenzothiophenes. The median precipitation and air concentrations were 11.3–646.7 (C3-fluoranthene/pyrene) ng L−1 and 0.21–16.9 (C3-naphthalene) ng m−3, respectively, for alkylated PAHs, and 8.5–530.5 (C4-dibenzothiophene) ng L−1 and 0.13–6.6 (C2-dibenzothiophene) ng m−3 for dibenzothiophenes and their alkylated derivatives. Median Wt over the measurement period were 6100–1.1 × 106 from snow scavenging and 350–2.3 × 105 from rain scavenging depending on the PAC species. Median Wt for parent PAHs were within the range of those observed at other urban and suburban locations. But Wt for acenaphthylene in snow samples was 2–7 times higher. Some individual snow and rain samples exceeded literature values by a factor of 10. Wt for benzo(a)pyrene, dibenz(a,h)anthracene, and benzo(g,h,i)perylene in snow samples had reached 107, which is the maximum for PAH snow scavenging ratios reported in literature. From the analysis of data subsets, Wt for particulate-phase dominant PACs were 14–20 times greater than gas-phase dominant PACs in snow samples and 7–20 times greater than gas-phase dominant PACs in rain samples. Wt from snow scavenging was ∼9 times greater than rain scavenging for particulate-phase dominant PACs and 4–9.6 times greater than rain scavenging for gas-phase dominant PACs. Gas-particle fractions of each PAC, particle size distributions of particulate-phase dominant PACs, and Henry's Law constant of gas-phase dominant PACs explained, to a large extent, the different Wt values among the different PACs and precipitation types. This study verified findings from a previous study of Wang et al. (2014) which suggested that snow scavenging is more efficient than rain scavenging of particles for equivalent precipitation amount, and also provided new knowledge on the scavenging of gas-phase PACs by snow and rain.

scholarly journals Scavenging ratios of polycyclic aromatic compounds in rain and snow in the Athabasca oil sands region

2015 ◽  
Vol 15 (3) ◽  
pp. 1421-1434 ◽  
Author(s):  
L. Zhang ◽  
I. Cheng ◽  
D. Muir ◽  
J.-P. Charland
Keyword(s):  
Gas Phase ◽  
Aromatic Compounds ◽  
Oil Sands ◽  
Polycyclic Aromatic Compounds ◽  
Particulate Phase ◽  
Athabasca Oil Sands ◽  
Polycyclic Aromatic ◽  
Alkylated Pahs ◽  
Scavenging Ratios ◽  
Snow Samples

Abstract. The Athabasca oil sands industry in northern Alberta, Canada, is a possible source of polycyclic aromatic compounds (PACs). Monitored PACs, including polycyclic aromatic hydrocarbons (PAHs), alkylated PAHs, and dibenzothiophenes (DBTs), in precipitation and in air at three near-source sites in the Fort MacKay and Fort McMurray area during January 2011 to May 2012, were used to generate a database of scavenging ratios (Wt) for PACs scavenged by both snow and rain. Higher concentrations in precipitation and air were observed for alkylated PAHs and DBTs compared to the other PACs. The sums of the median precipitation concentrations over the period of data analyzed were 0.48 μ g L−1 for the 18 PAHs, 3.38 μ g L−1 for the 20 alkylated PAHs, and 0.94 μ g L−1 for the 5 DBTs. The sums of the median air concentrations for parent PAHs, alkylated PAHs, and DBTs were 8.37, 67.26, and 11.83 ng m−3, respectively. Median Wt over the measurement period were 6100 – 1.1 × 106 from snow scavenging and 350 – 2.3 × 105 from rain scavenging depending on the PAC species. Median Wt for parent PAHs were within the range of those observed at other urban and suburban locations, but Wt for acenaphthylene in snow samples were 2–7 times higher compared to other urban and suburban locations. Wt for some individual snow and rain samples exceeded literature values by a factor of 10. Wt for benzo(a)pyrene, dibenz(a,h)anthracene, and benzo(g,h,i)perylene in snow samples had reached 107, which is the maximum for PAH snow scavenging ratios reported in the literature. From the analysis of data subsets, Wt for particulate-phase dominant PACs were 14–20 times greater than gas-phase dominant PACs in snow samples and 7–20 times greater than gas-phase dominant PACs in rain samples. Wt from snow scavenging were ~ 9 times greater than from rain scavenging for particulate-phase dominant PACs and 4–9.6 times greater than from rain scavenging for gas-phase dominant PACs. Gas-particle fractions of each PAC, particle size distributions of particulate-phase dominant PACs, and the Henry's law constant of gas-phase dominant PACs explained, to a large extent, the different Wt values among the different PACs and precipitation types. The trend in Wt with increasing alkyl substitutions may be attributed to their physico-chemical properties, such as octanol–air and particle partition coefficients and subcooled vapor pressure, which increases gas-particle partitioning and, subsequently, the particulate mass fraction. This study verified findings from a previous study of Wang et al. (2014) that suggested that snow scavenging is more efficient than rain scavenging of particles for equivalent precipitation amounts, and also provided new knowledge of the scavenging of gas-phase PACs and alkylated PACs by snow and rain.

scholarly journals Comparison of polycyclic aromatic compounds in air measured by conventional passive air samplers and passive dry deposition samplers and contributions from petcoke and oil sands ore

2018 ◽  
Vol 18 (12) ◽  
pp. 9161-9171 ◽  
Author(s):  
Narumol Jariyasopit ◽  
Yifeng Zhang ◽  
Jonathan W. Martin ◽  
Tom Harner
Keyword(s):  
Gas Phase ◽  
Dry Deposition ◽  
Aromatic Compounds ◽  
Oil Sands ◽  
Sampling Site ◽  
Polycyclic Aromatic Compounds ◽  
Open Pit ◽  
Open Pit Mining ◽  
Air Samples ◽  
Polycyclic Aromatic

Abstract. Conventional passive air samplers (PAS) and passive dry deposition samplers (PAS-DD) were deployed along a 90 km south–north transect at five sites in the Athabasca oil sands region (AOSR) during October to November 2015. The purpose was to compare and characterize the performance of the two passive sampling methods for targeted compounds across a range of site types. Samples were analyzed for polycyclic aromatic compounds (PACs), nitrated polycyclic aromatic hydrocarbons (NPAHs), and oxygenated PAHs (OPAHs). ΣPAC and ΣNPAH concentrations were highest in PAS and PAS-DD samplers at site AMS5, which is the closest sampling site to surface mining and upgrading facilities. The OPAHs were elevated at site AMS6, which is located in the town of Fort McMurray, approximately 30 km south of the main mining area. PAS-DD was enriched relative to PAS in particle-associated target chemicals, which is consistent with the relatively more open design of PAS-DD intended to capture particle-phase (and gas-phase) deposition. Petroleum coke (petcoke) (i.e., the carbonaceous byproduct of bitumen upgrading) and oil sands ore (i.e., the material mined in open-pit mines from which bitumen is extracted) were assessed for their potential to be a source of PACs to air in the oil sands region. The ore samples contained ∼ 8 times and ∼ 40 times higher ΣPACs concentrations (dry weight basis) than delayed and fluid petcoke, respectively. The residue analysis of ore and petcoke samples also revealed that the chemical 4-nitrobiphenyl (4-NBP) can be used to track gas-phase emissions to air. A comparison of chemical residues in ore, petcoke, and air samples revealed that the ore is likely a major contributor to volatile PACs present in air and that both ore and petcoke are contributing to the particle-associated PACs in air near open-pit mining areas. The contribution of petcoke particles in passive air samples was also confirmed qualitatively using scanning electron microscopy coupled with energy dispersive X-ray spectroscopy (SEM-EDS).

scholarly journals Emissions databases for polycyclic aromatic compounds in the Canadian Athabasca Oil Sands Region – development using current knowledge and evaluation with passive sampling and air dispersion modelling data

2017 ◽  
Author(s):  
Xin Qiu ◽  
Irene Cheng ◽  
Fuquan Yang ◽  
Erin Horb ◽  
Leiming Zhang ◽  
...  
Keyword(s):  
Aromatic Compounds ◽  
Oil Sands ◽  
Current Knowledge ◽  
Monitoring Network ◽  
Polycyclic Aromatic Compounds ◽  
Athabasca Oil Sands ◽  
Voc Emissions ◽  
Fire Emissions ◽  
Athabasca Oil Sands Region ◽  
Polycyclic Aromatic

Abstract. Two speciated and spatially-resolved emissions databases for polycyclic aromatic compounds (PAC) in the Athabasca oil sands region (AOSR) were developed. The first database was derived from volatile organic compound (VOC) emissions data provided by the Cumulative Environmental Management Association (CEMA) and the second database was derived from additional data collected within the Joint Canada-Alberta Oil Sands Monitoring (JOSM) program. CALPUFF modelling results for atmospheric polycyclic aromatic hydrocarbons (PAH), alkylated PAH, and dibenzothiophenes (DBT), obtained using each of the emissions databases, are presented and compared with measurements from a passive air monitoring network. The JOSM-derived emissions resulted in better model-measurement agreement in the total PAH concentrations and for most PAH species concentrations, compared to results using CEMA-derived emissions. At local sites near oil sands mines, the percent error of the model compared to observations decreased from 30 % using the CEMA-derived emissions to 17 % using the JOSM-derived emissions. The improvement at local sites was likely attributed to the inclusion of updated tailings pond emissions estimated from JOSM activities. In either the CEMA-derived or JOSM-derived emissions scenario, the model underestimated PAH concentrations by a factor of 3 at remote locations. Potential reasons for the disagreement include forest fire emissions, re-emissions of previously deposited PAHs, and long-range transport not considered in the model. Alkylated PAH and DBT concentrations were also significantly underestimated. The CALPUFF model is expected to predict higher concentrations because of the limited chemistry and deposition modelling. Thus the model underestimation of PACs is likely due to gaps in the emissions database for these compounds and uncertainties in the methodology for estimating the emissions. Future work is required that focuses on improving the PAC emission estimation and speciation methodologies and reducing the uncertainties in VOC emissions which are subsequently used in PAC emissions estimation.

scholarly journals Emissions databases for polycyclic aromatic compounds in the Canadian Athabasca oil sands region – development using current knowledge and evaluation with passive sampling and air dispersion modelling data

2018 ◽  
Vol 18 (5) ◽  
pp. 3457-3467 ◽  
Author(s):  
Xin Qiu ◽  
Irene Cheng ◽  
Fuquan Yang ◽  
Erin Horb ◽  
Leiming Zhang ◽  
...  
Keyword(s):  
Aromatic Compounds ◽  
Oil Sands ◽  
Current Knowledge ◽  
Monitoring Network ◽  
Polycyclic Aromatic Compounds ◽  
Athabasca Oil Sands ◽  
Voc Emissions ◽  
Fire Emissions ◽  
Athabasca Oil Sands Region ◽  
Polycyclic Aromatic

Abstract. Two speciated and spatially resolved emissions databases for polycyclic aromatic compounds (PACs) in the Athabasca oil sands region (AOSR) were developed. The first database was derived from volatile organic compound (VOC) emissions data provided by the Cumulative Environmental Management Association (CEMA) and the second database was derived from additional data collected within the Joint Canada–Alberta Oil Sands Monitoring (JOSM) program. CALPUFF modelling results for atmospheric polycyclic aromatic hydrocarbons (PAHs), alkylated PAHs, and dibenzothiophenes (DBTs), obtained using each of the emissions databases, are presented and compared with measurements from a passive air monitoring network. The JOSM-derived emissions resulted in better model–measurement agreement in the total PAH concentrations and for most PAH species concentrations compared to results using CEMA-derived emissions. At local sites near oil sands mines, the percent error of the model compared to observations decreased from 30 % using the CEMA-derived emissions to 17 % using the JOSM-derived emissions. The improvement at local sites was likely attributed to the inclusion of updated tailings pond emissions estimated from JOSM activities. In either the CEMA-derived or JOSM-derived emissions scenario, the model underestimated PAH concentrations by a factor of 3 at remote locations. Potential reasons for the disagreement include forest fire emissions, re-emissions of previously deposited PAHs, and long-range transport not considered in the model. Alkylated PAH and DBT concentrations were also significantly underestimated. The CALPUFF model is expected to predict higher concentrations because of the limited chemistry and deposition modelling. Thus the model underestimation of PACs is likely due to gaps in the emissions database for these compounds and uncertainties in the methodology for estimating the emissions. Future work is required that focuses on improving the PAC emissions estimation and speciation methodologies and reducing the uncertainties in VOC emissions which are subsequently used in PAC emissions estimation.

Sign in / Sign up

Export Citation Format

Share Document