Organic aerosol emission ratios from the laboratory combustion of biomass fuels

被引:30
作者
Jolleys, Matthew D. [1 ]
Coe, Hugh [1 ]
McFiggans, Gordon [1 ]
McMeeking, Gavin R. [2 ]
Lee, Taehyoung [2 ]
Kreidenweis, Sonia M. [2 ]
Collett, Jeffrey L., Jr. [2 ]
Sullivan, Amy P. [2 ]
机构
[1] Univ Manchester, Ctr Atmospher Sci, Sch Earth Atmospher & Environm Sci, Manchester, Lancs, England
[2] Colorado State Univ, Dept Atmospher Sci, Ft Collins, CO 80523 USA
基金
英国自然环境研究理事会; 美国国家环境保护局;
关键词
BURNING EMISSIONS; TRACE GASES; FIRE EMISSIONS; SEMIVOLATILE ORGANICS; TROPICAL FOREST; UNITED-STATES; MEXICO; MASS; PARTICLES; AIRBORNE;
D O I
10.1002/2014JD021589
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
Organic aerosol (OA) emission ratios (ER) have been characterized for 67 burns during the second Fire Laboratory at Missoula Experiment. These fires involved 19 different species representing 6 major fuels, each of which forms an important contribution to the U.S. biomass burning inventory. Average normalized Delta OA/Delta CO ratios show a high degree of variability, both between and within different fuel types and species, typically exceeding differen-ces between separate plumes in ambient measurements. This variability is strongly influenced by highly contrasting Delta OA levels between burns and the increased partitioning of semivolatile organic compounds to the particle phase at high Delta OA concentrations. No correlation across all fires was observed between Delta OA/Delta CO and modified combustion efficiency (MCE), which acts as an indicator of the proportional contributions of flaming and smoldering combustion phases throughout each burn. However, a negative correlation exists with MCE for some coniferous species, most notably Douglas fir, for which there is also an influence from fuel moisture content. Changes in fire efficiency were also shown to dramatically alter emissions for fires with very similar initial conditions. Although the relationship with MCE is variable between species, there is greater consistency with the level of oxygenation in OA. The ratio of the m/z 44 fragment to total OA mass concentration (f(44)) as measured by aerosol mass spectrometer provides an indication of oxygenation as influenced by combustion processes at source, with Delta OA/Delta CO decreasing with increasing f(44) for all fuel types. Inconsistencies in the magnitude of the effects associated with each potential influence on Delta OA/Delta CO emphasize the lack of a single dominant control on fire emissions, and a dependency on both fuel properties and combustion conditions.
引用
收藏
页码:12850 / 12871
页数:22
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