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DOI10.5194/acp-19-9715-2019
Secondary organic aerosol formation from alpha-pinene, alkanes, and oil-sands-related precursors in a new oxidation flow reactor
Li, Kun; Liggio, John; Lee, Patrick; Han, Chong; Liu, Qifan; Li, Shao-Meng
发表日期2019
ISSN1680-7316
EISSN1680-7324
卷号19期号:15页码:9715-9731
英文摘要

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 alpha-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 alpha-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 similar to 0.6-0.7) are significantly higher than those from the vapors from solvent use (naphtha), effluent from OS processing (tailings pond water), and from the solvent diluted bitumen (dilbit; maximum of similar to 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 tailings 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.


WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
来源期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/101339
作者单位Environm & Climate Change Canada, Air Qual Res Div, Toronto, ON M3H 5T4, Canada
推荐引用方式
GB/T 7714
Li, Kun,Liggio, John,Lee, Patrick,et al. Secondary organic aerosol formation from alpha-pinene, alkanes, and oil-sands-related precursors in a new oxidation flow reactor[J],2019,19(15):9715-9731.
APA Li, Kun,Liggio, John,Lee, Patrick,Han, Chong,Liu, Qifan,&Li, Shao-Meng.(2019).Secondary organic aerosol formation from alpha-pinene, alkanes, and oil-sands-related precursors in a new oxidation flow reactor.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(15),9715-9731.
MLA Li, Kun,et al."Secondary organic aerosol formation from alpha-pinene, alkanes, and oil-sands-related precursors in a new oxidation flow reactor".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.15(2019):9715-9731.
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