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DOI | 10.5194/acp-17-5459-2017 |
Secondary organic aerosol formation in biomass-burning plumes: theoretical analysis of lab studies and ambient plumes | |
Bian, Qijing1; Jathar, Shantanu H.2; Kodros, John K.1; Barsanti, Kelley C.3,4; Hatch, Lindsay E.3,4; May, Andrew A.5; Kreidenweis, Sonia M.1; Pierce, Jeffrey R.1,6 | |
2017-04-28 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2017 |
卷号 | 17期号:8 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Canada |
英文摘要 | Secondary organic aerosol (SOA) has been shown to form in biomass-burning emissions in laboratory and field studies. However, there is significant variability among studies in mass enhancement, which could be due to differences in fuels, fire conditions, dilution, and/or limitations of laboratory experiments and observations. This study focuses on understanding processes affecting biomass-burning SOA formation in laboratory smog-chamber experiments and in ambient plumes. Vapor wall losses have been demonstrated to be an important factor that can suppress SOA formation in laboratory studies of traditional SOA precursors; however, impacts of vapor wall losses on biomass-burning SOA have not yet been investigated. We use an aerosol-microphysical model that includes representations of volatility and oxidation chemistry to estimate the influence of vapor wall loss on SOA formation observed in the FLAME III smogchamber studies. Our simulations with base-case assumptions for chemistry and wall loss predict a mean OA mass enhancement (the ratio of final to initial OA mass, corrected for particle-phase wall losses) of 1.8 across all experiments when vapor wall losses are modeled, roughly matching the mean observed enhancement during FLAME III. The mean OA enhancement increases to over 3 when vapor wall losses are turned off, implying that vapor wall losses reduce the apparent SOA formation. We find that this decrease in the apparent SOA formation due to vapor wall losses is robust across the ranges of uncertainties in the key model assumptions for wall-loss and mass-transfer coefficients and chemical mechanisms. We then apply similar assumptions regarding SOA formation chemistry and physics to smoke emitted into the atmosphere. In ambient plumes, the plume dilution rate impacts the organic partitioning between the gas and particle phases, which may impact the potential for SOA to form as well as the rate of SOA formation. We add Gaussian dispersion to our aerosol-microphysical model to estimate how SOA formation may vary under different ambient-plume conditions (e.g., fire size, emission mass flux, atmospheric stability). Smoke from small fires, such as typical prescribed burns, dilutes rapidly, which drives evaporation of organic vapor from the particle phase, leading to more effective SOA formation. Emissions from large fires, such as intense wildfires, dilute slowly, suppressing OA evaporation and subsequent SOA formation in the near field. We also demonstrate that different approaches to the calculation of OA enhancement in ambient plumes can lead to different conclusions regarding SOA formation. OA mass enhancement ratios of around 1 calculated using an inert tracer, such as black carbon or CO, have traditionally been interpreted as exhibiting little or no SOA formation; however, we show that SOA formation may have greatly contributed to the mass in these plumes. In comparison of laboratory and plume results, the possible inconsistency of OA enhancement between them could be in part attributed to the effect of chamber walls and plume dilution. Our results highlight that laboratory and field experiments that focus on the fuel and fire conditions also need to consider the effects of plume dilution or vapor losses to walls. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000400458800001 |
WOS关键词 | VAPOR-WALL DEPOSITION ; SMOG-CHAMBER EXPERIMENTS ; PHOTOCHEMICAL OXIDATION ; MOLECULAR-STRUCTURE ; SIZE DISTRIBUTIONS ; PRESCRIBED FIRE ; TRACE GASES ; EVOLUTION ; EMISSIONS ; YIELDS |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/30648 |
专题 | 地球科学 |
作者单位 | 1.Colorado State Univ, Dept Atmospher Sci, Ft Collins, CO 80523 USA; 2.Colorado State Univ, Dept Mech Engn, Ft Collins, CO 80523 USA; 3.Univ Calif Riverside, Dept Chem & Environm Engn, Riverside, CA 92521 USA; 4.Univ Calif Riverside, Coll Engn, Ctr Environm Res & Technol CE CERT, Riverside, CA 92521 USA; 5.Ohio State Univ, Dept Civil Environm & Geodet Engn, Columbus, OH 43210 USA; 6.Dalhousie Univ, Dept Phys & Atmospher Sci, Halifax, NS, Canada |
推荐引用方式 GB/T 7714 | Bian, Qijing,Jathar, Shantanu H.,Kodros, John K.,et al. Secondary organic aerosol formation in biomass-burning plumes: theoretical analysis of lab studies and ambient plumes[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2017,17(8). |
APA | Bian, Qijing.,Jathar, Shantanu H..,Kodros, John K..,Barsanti, Kelley C..,Hatch, Lindsay E..,...&Pierce, Jeffrey R..(2017).Secondary organic aerosol formation in biomass-burning plumes: theoretical analysis of lab studies and ambient plumes.ATMOSPHERIC CHEMISTRY AND PHYSICS,17(8). |
MLA | Bian, Qijing,et al."Secondary organic aerosol formation in biomass-burning plumes: theoretical analysis of lab studies and ambient plumes".ATMOSPHERIC CHEMISTRY AND PHYSICS 17.8(2017). |
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