Modeling Biomass Burning Organic Aerosol Atmospheric Evolution and Chemical Aging

被引:3
作者
Patoulias, David [1 ,2 ]
Kallitsis, Evangelos [3 ]
Posner, Laura [4 ]
Pandis, Spyros N. [1 ,2 ]
机构
[1] Univ Patras, Dept Chem Engn, Patras 26504, Greece
[2] Fdn Res & Technol Hellas FORTH ICE HT, Inst Chem Engn Sci, Patras 26504, Greece
[3] Imperial Coll London, Dept Earth Sci & Engn, London SW7 2AZ, England
[4] Carnegie Mellon Univ, Dept Chem Engn, Pittsburgh, PA 15213 USA
关键词
volatility basis set; biomass burning; air quality modeling; PRESCRIBED FIRE; AIR-POLLUTION; EMISSIONS; CHEMISTRY; FOREST; SMOKE; SIMULATION; TRANSPORT; OXIDATION; AIRCRAFT;
D O I
10.3390/atmos12121638
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The changes in the concentration and composition of biomass-burning organic aerosol (OA) downwind of a major wildfire are simulated using the one-dimensional Lagrangian chemical transport model PMCAMx-Trj. A base case scenario is developed based on realistic fire-plume conditions and a series of sensitivity tests are performed to quantify the effects of different conditions and processes. Temperature, oxidant concentration and dilution rate all affect the evolution of biomass burning OA after its emission. The most important process though is the multi-stage oxidation of both the originally emitted organic vapors (volatile and intermediate volatility organic compounds) and those resulting from the evaporation of the OA as it is getting diluted. The emission rates of the intermediate volatility organic compounds (IVOCs) and their chemical fate have a large impact on the formed secondary OA within the plume. The assumption that these IVOCs undergo only functionalization leads to an overestimation of the produced SOA suggesting that fragmentation is also occurring. Assuming a fragmentation probability of 0.2 resulted in predictions that are more consistent with available observations. Dilution leads to OA evaporation and therefore reduction of the OA levels downwind of the fire. However, the evaporated material can return to the particulate phase later on after it gets oxidized and recondenses. The sensitivity of the OA levels and total mass balance on the dilution rate depends on the modeling assumptions. The high variability of OA mass enhancement observed in past field studies downwind of fires may be partially due to the variability of the dilution rates of the plumes.
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页数:18
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