Particulate matter emissions over the oil sands regions in Alberta, Canada

2017 ◽  
Vol 25 (4) ◽  
pp. 432-443 ◽  
Author(s):  
Zhenyu Xing ◽  
Ke Du
Keyword(s):  
Particulate Matter ◽  
Oil Sands ◽  
Secondary Organic Aerosol ◽  
Ambient Air ◽  
Organic Aerosol ◽  
Open Pit ◽  
Open Pit Mining ◽  
Formation Mechanisms ◽  
Aerosol Formation ◽  
Secondary Aerosol

Particulate matter (PM) emissions from the expanded oil sands development in Alberta are becoming a focus among the aerosol science community because of its significant negative impact on the regional air quality and climate change. Open-pit mining, petroleum coke (petcoke) dust, and the transportation of oil sands and waste materials by heavy-duty trucks on unpaved roads could release PM into the air. Incomplete combustion of fossil fuels by engines and stationary boilers leads to the formation of carbonaceous aerosols. In addition, wildfire and biogenic emissions surrounding the oil sands regions also have the potential to contribute primary PM to the ambient air. Secondary organic aerosol formation has been revealed as an important source of PM over nearby and distant areas from the oil sands regions. This review summarizes the primary PM sources and some secondary aerosol formation mechanisms that are linked to oil sands development. It also reviews the approaches that can be applied in aerosol source apportionment. Meteorological condition is an important factor that may influence the primary PM emission and secondary aerosol formation in Alberta’s oil sands regions. Current concern should not be limited to the primary emission of atmospheric PM. Secondary formation of aerosols, especially secondary organic aerosol originating from photochemical reaction, should also be taken into consideration. To obtain a more comprehensive understanding of the sources and amount of PM emissions based on the bottom-up emission inventory approach, investigations on how to reduce the uncertainty in determination of real-world PM emission factors for the variable sources are needed. Long-range transport trajectories of fine PM from Alberta’s oil sands regions remain unknown.

scholarly journals Secondary organic aerosol formation from α-pinene, alkanes and oil sands related precursors in a new oxidation flow reactor

2019 ◽  
Author(s):  
Kun Li ◽  
John Liggio ◽  
Patrick Lee ◽  
Chong Han ◽  
Qifan Liu ◽  
...  
Keyword(s):  
Oil Sands ◽  
Flow Reactor ◽  
Secondary Organic Aerosol ◽  
Pond Water ◽  
Organic Aerosol ◽  
Open Pit ◽  
Aerosol Formation ◽  
Mining Operations ◽  
Solvent Use ◽  
The Impact

Abstract. Oil sands (OS) operations in Alberta, Canada are a large source of secondary organic aerosol (SOA). However, the SOA formation process from OS-related precursors remains poorly understood. In this work, a newly developed oxidation flow reactor (OFR), the Environment and Climate Change Canada OFR (ECCC-OFR), was characterized and used to study the yields and composition of SOA formed from OH oxidation of α-pinene, selected alkanes, and the vapors evolved from five OS-related samples (OS ore, naphtha, tailings pond water, bitumen, and dilbit). The derived SOA yields from α-pinene and selected alkanes using the ECCC-OFR were in good agreement with those of traditional smog chamber experiments, but significantly higher than those of other OFR studies under similar conditions. The results also suggest that gas-phase reactions leading to fragmentation (i.e., C-C bond cleavage) have a relatively small impact on the SOA yields in the ECCC-OFR at high photochemical ages, in contrast to other previously reported OFR results. Translating the impact of fragmentation reactions in the ECCC-OFR to ambient atmospheric conditions reduces its impact on SOA formation even further. These results highlight the importance of careful evaluation of OFR data, particularly when using such data to provide empirical factors for the fragmentation process in models. Application of the ECCC-OFR to OS-related precursor mixtures, demonstrated that the SOA yields from OS ore and bitumen vapors (maximum of ~ 0.6–0.7) are significantly higher than those from the vapors from solvent use (naphtha), effluent from OS processing (tailing pond water) and from the solvent diluted bitumen (dilbit) (maximum of ~ 0.2–0.3), likely due to the volatility of each precursor mixture. A comparison of the yields and elemental ratios (H / C and O / C) of the SOA from the OS-related precursors to those of linear and cyclic alkane precursors of similar carbon numbers suggests that cyclic alkanes play an important role in the SOA formation in the OS. The analysis further indicates that the majority of the SOA formed downwind of OS facilities is derived from open-pit mining operations (i.e., OS ore evaporative emissions), rather than from higher volatility precursors from solvent use during processing and/or tailing management. The current results have implications for improving the regional modeling of SOA from OS sources, for the potential mitigation of OS precursor emissions responsible for observed SOA downwind of OS operations, and for the understanding of petrochemical and alkane derived SOA in general.

scholarly journals In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

2015 ◽  
Vol 15 (21) ◽  
pp. 30409-30471 ◽  
Author(s):  
B. B. Palm ◽  
P. Campuzano-Jost ◽  
A. M. Ortega ◽  
D. A. Day ◽  
L. Kaser ◽  
...  
Keyword(s):  
Organic Compounds ◽  
Flow Reactor ◽  
Secondary Organic Aerosol ◽  
Ambient Air ◽  
Organic Aerosol ◽  
Pine Forest ◽  
Oxidation Products ◽  
Oh Radicals ◽  
Aerosol Formation ◽  
Photochemical Aging

Abstract. Ambient air was oxidized by OH radicals in an oxidation flow reactor (OFR) located in a montane pine forest during the BEACHON-RoMBAS campaign to study biogenic secondary organic aerosol (SOA) formation and aging. High OH concentrations and short residence times allowed for semi-continuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative time scales of condensation of low volatility organic compounds (LVOCs) onto particles, condensational loss to the walls, and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 4 μg m-3 when LVOC fate corrected) compared to daytime (average 1 μg m-3 when LVOC fate corrected), with maximum formation observed at 0.4–1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene + p-cymene concentrations, including a substantial increase just after sunrise at 07:00 LT. Higher photochemical aging (> 10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small oxidized organic compounds, and net production at lower ages followed by net consumption of terpenoid oxidation products as photochemical age increased. New particle formation was observed in the reactor after oxidation, especially during times when precursor gas concentrations and SOA formation were largest. Approximately 6 times more SOA was formed in the reactor from OH oxidation than could be explained by the VOCs measured in ambient air. Several recently-developed instruments quantified ambient semi- and intermediate-volatility organic compounds (S/IVOCs) that were not detected by a PTR-TOF-MS. An SOA yield of 24–80 % from those compounds can explain the observed SOA, suggesting that these typically unmeasured S/IVOCs play a substantial role in ambient SOA formation. Our results allow ruling out condensation sticking coefficients much lower than 1. Our measurements help clarify the magnitude of SOA formation in forested environments, and demonstrate methods for interpretation of ambient OFR measurements.

scholarly journals Synergetic formation of secondary inorganic and organic aerosol: Influence of SO<sub>2</sub> and/or NH<sub>3</sub> in the heterogeneous process

2016 ◽  
Author(s):  
Biwu Chu ◽  
Xiao Zhang ◽  
Yongchun Liu ◽  
Hong He ◽  
Yele Sun ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Synergistic Effects ◽  
Particle Growth ◽  
Organic Aerosol ◽  
Interactive Effects ◽  
Aerosol Formation ◽  
Secondary Aerosol ◽  
Heterogeneous Process ◽  
So2 Concentration ◽  
Inorganic And Organic

Abstract. The effects of SO2 and NH3 on secondary organic aerosol formation have rarely been investigated together, while the interactive effects between inorganic and organic species under highly complex pollution conditions remain uncertain. Here we studied the effects of SO2 and NH3 on secondary aerosol formation in the photooxidation system of toluene/NOx in the presence or absence of Al2O3 seed aerosols in a 2 m3 smog chamber. The presence of SO2 increased new particle formation and particle growth significantly, regardless of whether NH3 was present or not. Sulfate, organic aerosol, nitrate and ammonium were all found to increase linearly with increasing SO2 concentrations. The increases in these four species were more obvious under NH3-rich conditions, and the generation of nitrate, ammonium and organic aerosol increased more significantly than sulfate with respect to SO2 concentration, while sulfate was the most sensitive species under NH3-poor conditions. The synergistic effects between SO2 and NH3 in the heterogeneous process contributed greatly to secondary aerosol formation. Specifically, the generation of NH4NO3 was found to be highly dependent on the surface area concentration of suspended particles, and increased most significantly among the four species with respect to SO2 concentration under ammonia-rich conditions. Meanwhile, the absorbed NH3 might provide a liquid surface layer for the absorption and subsequent reaction of SO2 and organic products, and therefore, enhance sulfate and secondary organic aerosol (SOA) formation. This effect mainly occurred in the heterogeneous process and resulted in a significantly higher growth rate of seed aerosols compared to that without NH3. By applying positive matrix factorization (PMF) analysis to the AMS data, two factors were identified for the generated SOA. One factor, assigned to less-oxidized organic aerosol and some oligomers, increased with increasing SO2 under NH3-poor conditions, mainly due to the well-known acid catalytic effect of the acid products on SOA formation in the heterogeneous process. The other factor, assigned to the highly oxidized organic component and some nitrogen-containing organics (NOC), increased with SO2 under a NH3-rich environment, with NOC (organonitrates and NOC with reduced N) contributing most of the increase.

scholarly journals Summertime and wintertime atmospheric processes of secondary aerosol in Beijing

2019 ◽  
Author(s):  
Jing Duan ◽  
Ru-Jin Huang ◽  
Yongjie Li ◽  
Qi Chen ◽  
Yan Zheng ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Seasonal Variations ◽  
Chemical Speciation ◽  
Fine Particles ◽  
Large Fraction ◽  
Formation Mechanisms ◽  
Urban Air ◽  
Aerosol Formation ◽  
Secondary Aerosol ◽  
Atmospheric Processes

Abstract. Secondary aerosol constitutes a large fraction of fine particles in urban air of China. However, its formation mechanisms and atmospheric processes remain largely uncertain despite considerable studies in recent years. To elucidate the seasonal variations of fine particles composition and secondary aerosol formation, an Aerodyne quadrupole aerosol chemical speciation monitor (Q-ACSM) combined with other online instruments were used to characterize the submicron particulate matter (diameter 

scholarly journals Mapping gas-phase organic reactivity and concomitant secondary organic aerosol formation: chemometric dimension reduction techniques for the deconvolution of complex atmospheric data sets

2015 ◽  
Vol 15 (14) ◽  
pp. 8077-8100 ◽  
Author(s):  
K. P. Wyche ◽  
P. S. Monks ◽  
K. L. Smallbone ◽  
J. F. Hamilton ◽  
M. R. Alfarra ◽  
...  
Keyword(s):  
Phase Composition ◽  
Dimension Reduction ◽  
Gas Phase ◽  
Secondary Organic Aerosol ◽  
Ambient Air ◽  
Organic Aerosol ◽  
Chemical Mechanism ◽  
Particle Phase ◽  
Aerosol Formation ◽  
Holistic View

Abstract. Highly non-linear dynamical systems, such as those found in atmospheric chemistry, necessitate hierarchical approaches to both experiment and modelling in order to ultimately identify and achieve fundamental process-understanding in the full open system. Atmospheric simulation chambers comprise an intermediate in complexity, between a classical laboratory experiment and the full, ambient system. As such, they can generate large volumes of difficult-to-interpret data. Here we describe and implement a chemometric dimension reduction methodology for the deconvolution and interpretation of complex gas- and particle-phase composition spectra. The methodology comprises principal component analysis (PCA), hierarchical cluster analysis (HCA) and positive least-squares discriminant analysis (PLS-DA). These methods are, for the first time, applied to simultaneous gas- and particle-phase composition data obtained from a comprehensive series of environmental simulation chamber experiments focused on biogenic volatile organic compound (BVOC) photooxidation and associated secondary organic aerosol (SOA) formation. We primarily investigated the biogenic SOA precursors isoprene, α-pinene, limonene, myrcene, linalool and β-caryophyllene. The chemometric analysis is used to classify the oxidation systems and resultant SOA according to the controlling chemistry and the products formed. Results show that "model" biogenic oxidative systems can be successfully separated and classified according to their oxidation products. Furthermore, a holistic view of results obtained across both the gas- and particle-phases shows the different SOA formation chemistry, initiating in the gas-phase, proceeding to govern the differences between the various BVOC SOA compositions. The results obtained are used to describe the particle composition in the context of the oxidised gas-phase matrix. An extension of the technique, which incorporates into the statistical models data from anthropogenic (i.e. toluene) oxidation and "more realistic" plant mesocosm systems, demonstrates that such an ensemble of chemometric mapping has the potential to be used for the classification of more complex spectra of unknown origin. More specifically, the addition of mesocosm data from fig and birch tree experiments shows that isoprene and monoterpene emitting sources, respectively, can be mapped onto the statistical model structure and their positional vectors can provide insight into their biological sources and controlling oxidative chemistry. The potential to extend the methodology to the analysis of ambient air is discussed using results obtained from a zero-dimensional box model incorporating mechanistic data obtained from the Master Chemical Mechanism (MCMv3.2). Such an extension to analysing ambient air would prove a powerful asset in assisting with the identification of SOA sources and the elucidation of the underlying chemical mechanisms involved.

scholarly journals Secondary organic aerosol formation exceeds primary particulate matter emissions for light-duty gasoline vehicles

2013 ◽  
Vol 13 (9) ◽  
pp. 23173-23216 ◽  
Author(s):  
T. D. Gordon ◽  
A. A. Presto ◽  
A. A. May ◽  
N. T. Nguyen ◽  
E. M. Lipsky ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Secondary Organic Aerosol ◽  
Cold Start ◽  
Organic Aerosol ◽  
Smog Chamber ◽  
Aerosol Formation ◽  
Gas Emissions ◽  
Light Duty ◽  
Gasoline Vehicles ◽  
Diesel Trucks

Abstract. The effects of photochemical aging on emissions from 15 light-duty gasoline vehicles were investigated using a smog chamber to probe the critical link between the tailpipe and ambient atmosphere. The vehicles were recruited from the California in-use fleet; they represent a wide range of model years (1987 to 2011), vehicle types and emission control technologies. Each vehicle was tested on a chassis dynamometer using the unified cycle. Dilute emissions were sampled into a portable smog chamber and then photochemically aged under urban-like conditions. For every vehicle, substantial secondary organic aerosol (SOA) formation occurred during cold-start tests, with the emissions from some vehicles generating as much as 6 times the amount of SOA as primary particulate matter after three hours of oxidation inside the chamber at typical atmospheric oxidant levels. Therefore, the contribution of light duty gasoline vehicle exhaust to ambient PM levels is likely dominated by secondary PM production (SOA and nitrate). Emissions from hot-start tests formed about a factor of 3–7 less SOA than cold-start tests. Therefore, catalyst warm-up appears to be an important factor in controlling SOA precursor emissions. The mass of SOA generated by photo-oxidizing exhaust from newer (LEV1 and LEV2) vehicles was only modestly lower (38%) than that formed from exhaust emitted by older (pre-LEV) vehicles, despite much larger reductions in non-methane organic gas emissions. These data suggest that a complex and non-linear relationship exists between organic gas emissions and SOA formation, which is not surprising since SOA precursors are only one component of the exhaust. Except for the oldest (pre-LEV) vehicles, the SOA production could not be fully explained by the measured oxidation of speciated (traditional) SOA precursors. Over the time scale of these experiments, the mixture of organic vapors emitted by newer vehicles appear to be more efficient (higher yielding) in producing SOA than the emissions from older vehicles. About 30% of the non-methane organic gas emissions from the newer (LEV1 and LEV2) vehicles could not be speciated, and the majority of the SOA formed from these vehicles appears to be associated with these unspeciated organics. These results for light-duty gasoline vehicles contrast with the results from a companion study of on-road heavy-duty diesel trucks; in that study late model (2007 and later) diesel trucks equipped with catalyzed diesel particulate filters emitted very little primary PM, and the photo-oxidized emissions produced negligible amounts of SOA.

scholarly journals Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

2015 ◽  
Vol 15 (15) ◽  
pp. 21907-21958 ◽  
Author(s):  
A. M. Ortega ◽  
P. L. Hayes ◽  
Z. Peng ◽  
B. B. Palm ◽  
W. Hu ◽  
...  
Keyword(s):  
Los Angeles ◽  
Real Time ◽  
Flow Reactor ◽  
Secondary Organic Aerosol ◽  
Vertical Mixing ◽  
Ambient Air ◽  
Organic Aerosol ◽  
Aerosol Formation ◽  
Scanning Mobility Particle Sizer ◽  
Heterogeneous Oxidation

Abstract. Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA) that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An Oxidation Flow Reactor (OFR) was deployed to study SOA formation in real-time during the CalNex campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS) alternated sampling ambient and reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air, achieving equivalent atmospheric aging from hours up to several weeks in 3 min of processing. OH radical concentration was continuously stepped, obtaining measurements of real-time SOA formation and oxidation at multiple equivalent ages from 0.8 days–6.4 weeks. Enhancement of OA from aging showed a maximum net SOA production between 0.8–6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry, and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and Ox, which along with the short-lived VOC correlation, indicates the importance of relatively reactive (τOH ∼ 0.3 day) SOA precursors in the LA-Basin. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope ∼ -0.65). Oxidation state of carbon (OSC) in reactor SOA increased steeply with age and remained elevated (OSC ∼ 2) at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background) vs. photochemical age is similar to previous studies at low to moderate ages and also extends to higher ages where OA loss dominates. The mass added at low-to-intermediate ages is due primarily to condensation of oxidized species, not heterogeneous oxidation. The OA decrease at high photochemical ages is dominated by heterogeneous oxidation followed by fragmentation/evaporation. A comparison of urban SOA formation in this study with a similar study of vehicle SOA in a tunnel supports the dominance of vehicle emissions in urban SOA. Pre-2007 SOA models underpredict SOA formation by an order of magnitude, while a more recent model performs better but overpredicts at higher ages. These results demonstrate the value of the reactor as a tool for in situ evaluation of the SOA formation potential and OA evolution from ambient air.

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