Polycyclic aromatic hydrocarbon size distributions in aerosols from appliances of residential wood combustion as determined by direct thermal desorption - GC/MS
Polycyclic aromatic hydrocarbon size distributions in aerosols from appliances of residential wood combustion as determined by direct thermal desorption - GC/MS
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DOI：
10.1016/s0021-8502(03)00080-6
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发表时间：
2003-08-01
影响因子：
4.5
通讯作者：
Kariher, P
中科院分区：
文献类型：
--
作者：
Hays, MD;Smith, ND;Kariher, P
在这项工作中，一个直接的热解吸/气相色谱/质谱（TD/GC/MS）的方法来确定多环芳烃（PAH）的组成（MW = 202-302 amu）的大小隔离的气溶胶从住宅木材燃烧。六燃烧试验进行了两个常见的燃烧木材燃料物种，花旗松（黄杉属）。和白色橡木（Quercus sp.）。气溶胶羽流的大气稀释和冷却是在一个新设计的风洞中模拟的，产生的气溶胶的大小分类与电低压冲击器（ELPI）。ELPI阶段的数据形态TD/GC/MS反演和建模使用对数正态分布函数。重量测定的PM2.5（空气动力学直径[d（a）] < 2.5 μ m的细颗粒）排放率（2.3-10.2 g/kg）与第1-8阶段的矩阵校正ELPI质量测量（2.7-11.8 g/kg）相一致。燃料含水量与PM2.5质量几何平均直径（d（g））线性相关（r（2）= 0.986）。燃烧效率（CO2/CO）和温度，O-2水平，气体稀释温度影响颗粒尺寸分布; dg范围从313到662 nm，表明积累模式。反演ELPI数据的重建和求和允许量化27个单独的多环芳烃（和多环芳烃结构异构体的集群）;多环芳烃表征PM2.5质量的0.01和0.07重量%之间。苯并[a]芘是多环芳烃的主要排放物。PAH的大小分配（d（g）范围= 171-331 nm）与PM2.5质量分配不同，并向更精细的d（a）移动。高分子量和低分子量的多环芳烃优先分离细和粗DA在该顺序。超细模式平均包含大于80%的总测量颗粒数浓度。颗粒物表面积分布的dg值在120和330 nm之间。对于这些测试，PAH质量和PM表面积线性相关（r（2）大于或等于0.913）。应用一个简单的函数来考虑吸附和吸收机制，可以明显看出：（a）相同MW基团的PAR的表面和核心组成随燃烧而变化，（B）较低MW PAH的优先表面吸附是可能的。(C)2003 Elsevier Ltd.保留所有权利。
In this work, a direct thermal desorption/gas chromatography/mass spectrometry (TD/GC/MS) method is implemented to determine the polycyclic aromatic hydrocarbon (PAH) composition (MW = 202-302 amu) in size-segregated aerosols from residential wood combustion. Six combustion tests are performed with two commonly burned wood fuel species, Douglas-fir (Pseudotsuga sp.) and white oak (Quercus sp.). Atmospheric dilution and cooling of the aerosol plume are simulated in a newly designed wind tunnel, and the resulting aerosols are size classified with an electrical low-pressure impactor (ELPI).. ELPI stage data speciated by TD/GC/MS were inverted and modeled using a log normal distribution function. Gravimetrically determined PM2.5 (fine particles with aerodynamic diameters [d(a)] < 2.5 mum) emission rates (2.3-10.2 g/kg) corroborate to matrix-corrected ELPI mass measurements of stages 1-8 (2.7-11.8 g/kg). Fuel moisture content linearly correlates (r(2) = 0.986) to the PM2.5 mass geometric mean diameter (d(g)). Combustion efficiency (CO2/CO) and temperature, O-2 levels, and gas dilution temperature affect particle size distributions; dg ranges from 313 to 662 nm, indicating an accumulation mode. Reconstruction and summation of inverted ELPI data allow for the quantification of 27 individual PAHs (and clusters of structural PAH isomers); PAHs characterize between 0.01 and 0.07 wt% of the PM2.5 mass. Benzo[a]pyrene predominates the PAH emissions. PAH size allocations (d(g) range = 171-331 nm) are out of phase with PM2.5 mass ones and shifted to finer d(a). Higher and lower MW PAHs preferentially segregate to fine and coarse da in that order. The ultrafine mode contains on average greater than 80% of the total measured particle number concentration. Values of dg for particulate matter surface area distributions are between 120 and 330 nm. For these tests, PAH mass and PM surface area linearly correlate (r(2) greater than or equal to 0.913). Application of a simple function to consider adsorption and absorption mechanisms makes apparent that (a) surface and core compositions of PAR of identical MW groups vary with combustion and (b) preferential surface adsorption of lower MW PAH is possible. (C) 2003 Elsevier Ltd. All rights reserved.