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In situ measurements and modeling of reactive trace gases in a small biomass burning plume

机译：在小型生物质燃烧羽流中的反应痕气体的原位测量和建模

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An instrumented NASA P-3B aircraft was used for airborne sampling of trace gases in a plume that had emanated from a small forest understory fire in Georgia, USA. The plume was sampled at its origin to derive emission factors and followed aEuro parts per thousand 13.6 km downwind to observe chemical changes during the first hour of atmospheric aging. The P-3B payload included a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS), which measured non-methane organic gases (NMOGs) at unprecedented spatiotemporal resolution (10 m spatial/0.1 s temporal). Quantitative emission data are reported for CO2, CO, NO, NO2, HONO, NH3, and 16 NMOGs (formaldehyde, methanol, acetonitrile, propene, acetaldehyde, formic acid, acetone plus its isomer propanal, acetic acid plus its isomer glycolaldehyde, furan, isoprene plus isomeric pentadienes and cyclopentene, methyl vinyl ketone plus its isomers crotonaldehyde and methacrolein, methylglyoxal, hydroxy acetone plus its isomers methyl acetate and propionic acid, benzene, 2,3-butanedione, and 2-furfural) with molar emission ratios relative to CO larger than 1 ppbV ppmV(-1). Formaldehyde, acetaldehyde, 2-furfural, and methanol dominated NMOG emissions. No NMOGs with more than 10 carbon atoms were observed at mixing ratios larger than 50 pptV ppmV(-1) CO. Downwind plume chemistry was investigated using the observations and a 0-D photochemical box model simulation. The model was run on a nearly explicit chemical mechanism (MCM v3.3) and initialized with measured emission data. Ozone formation during the first hour of atmospheric aging was well captured by the model, with carbonyls (formaldehyde, acetaldehyde, 2,3-butanedione, methylglyoxal, 2-furfural) in addition to CO and CH4 being the main drivers of peroxy radical chemistry. The model also accurately reproduced the sequestration of NOx into peroxyacetyl nitrate (PAN) and the OH-initiated degradation of furan and 2-furfural at an average OH concentration of 7.45 +/- 1.07 x 10(6)aEuro-cm(-3) in the plume. Formaldehyde, acetone/propanal, acetic acid/glycolaldehyde, and maleic acid/maleic anhydride (tentatively identified) were found to be the main NMOGs to increase during 1 h of atmospheric plume processing, with the model being unable to capture the observed increase. A mass balance analysis suggests that about 50 % of the aerosol mass formed in the downwind plume is organic in nature.
机译：仪器化的NASA P-3B飞机用于在美国佐治亚州格鲁吉亚的小森林林下火灾中散发的羽流中的痕量气体采样。羽毛以其起源进行取样以导出排放因子，然后沿着AEURO零件沿着百万的零件下载，以观察在大气老化的第一个小时内的化学变化。 P-3B有效载荷包括质子转移反应 - 飞行时间质谱仪（PTR-TOF-MS），其在前所未有的时空分辨率下测量非甲烷有机气体（NMOG）（10米空间/ 0.1秒） 。据报道了数量发射数据，用于CO2，CO，NO，NO2，HONO，NH3和16个NMOGS（甲醛，甲醇，乙腈，丙烯​​，乙醛，甲酸，丙酮加上其异构体丙酮，醋酸加上其异构体甘醇醛，呋喃，异戊二烯加异构烯和环戊烯，甲基乙烯基酮加上其异构体裆醛和甲基丙酮，羟基丙酮，甲基乙酸甲酯和丙酸甲酯，苯，2,3-丁二烯，和2-糠醛，相对于CO，摩尔排放比例大于1 ppbv ppmv（-1）。甲醛，乙醛，2糠醛和甲醇主导NMOG排放。在大于50pptV PPMV（-1）CO的混合比中，在混合比下观察到具有超过10个碳原子的NMOG。使用观察结果和0-D光化盒模型模拟研究了下风羽流化学。该模型在几乎明确的化学机制（MCM V3.3）上运行并用测量的发射数据初始化。除了CO和CH4之外，由该模型捕获的第一小时大气老化的臭氧形成良好，用羰基（甲醛，乙醛，2,3-丁二烯，甲基乙二醛，2-糠醛）是过氧自由基化学的主要驱动因素。该模型还将NOx的螯合剂精确地再现为过氧乙酰基硝酸酯（锅）和呋喃和2-糠氏菌的OH-引发的浓度为7.45 +/- 1.07×10（6）Aeuro-cm（-3）在羽毛中。发现甲醛，丙酮/丙酮，醋酸/甘醇/甘醇和马来酸/马来酸酐（暂定鉴定）是在大气羽流处理的1小时内增加的主要NMOG，模型无法捕获观察到的增加。质量平衡分析表明，在下行羽流中形成的约50％的气溶胶块是有机的。

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