Sinha Aditya, George Ingrid, Holder Amara, Preston William, Hays Michael, Grieshop Andrew P
Department of Civil and Environmental Engineering, North Carolina State University, Raleigh, NC, USA.
Center for Environmental Measurement and Modeling, US Environmental Protection Agency, Durham, NC, USA.
Environ Sci Atmos. 2023 Jan 1;3(1):11-23. doi: 10.1039/d2ea00080f. Epub 2022 Oct 7.
The volatility distribution of organic emissions from biomass burning and other combustion sources can determine their atmospheric evolution due to partitioning/aging. The gap between measurements and models predicting secondary organic aerosol has been partially attributed to the absence of semi- and intermediate volatility organic compounds (S/I-VOC) in models and measurements. However, S/I-VOCs emitted from these sources and typically quantified using the volatility basis framework (VBS) are not well understood. For example, the amount and composition of S/I-VOCs and their variability across different biomass burning sources such as residential woodstoves, open field burns, and laboratory simulated open burning are uncertain. To address this, a novel filter-in-tube sorbent tube sampling method collected S/I-VOC samples from biomass burning experiments for a range of fuels and combustion conditions. Filter-in-tube samples were analyzed using thermal desorption-gas chromatography-mass spectrometry (TD/GC/MS) for compounds across a wide range of volatilities (saturation concentration; -2 ≤ * ≤ 6). The S/I-VOC measurements were used to calculate volatility distributions for each emissions source. The distributions were broadly consistent across the sources with IVOCs accounting for 75% - 90% of the total captured organic matter, while SVOCs and LVOCs were responsible for 6% - 13% and 1% - 12%, respectively. The distributions and predicted partitioning were generally consistent with literature. Particulate matter emission factors spanned two orders of magnitude across the sources. This work highlights the potential of inferring gas-particle partitioning behavior of biomass burning emissions using filter-in-tube sorbent samples analyzed offline. This simplifies both sampling and analysis of S/I-VOCs for studies focused on capturing the full range of organics emitted.
生物质燃烧及其他燃烧源产生的有机排放物的挥发性分布,可因其分配/老化过程决定其在大气中的演化。测量值与预测二次有机气溶胶的模型之间的差距,部分归因于模型和测量中缺乏半挥发性和中挥发性有机化合物(S/I-VOC)。然而,这些源排放的且通常使用挥发性基准框架(VBS)进行量化的S/I-VOC尚未得到充分理解。例如,S/I-VOC的数量和组成及其在不同生物质燃烧源(如家用木炉、野外焚烧和实验室模拟露天燃烧)之间的变异性尚不确定。为解决这一问题,一种新型的滤管内吸附剂管采样方法,针对一系列燃料和燃烧条件,从生物质燃烧实验中采集了S/I-VOC样本。使用热脱附-气相色谱-质谱联用仪(TD/GC/MS)对滤管内样本中广泛挥发性范围(饱和浓度;-2≤*≤6)的化合物进行分析。S/I-VOC测量结果用于计算每个排放源的挥发性分布。各排放源的分布大致一致,中间挥发性有机化合物(IVOC)占捕获的总有机物的75%-90%,而半挥发性有机化合物(SVOC)和低挥发性有机化合物(LVOC)分别占6%-13%和1%-12%。这些分布和预测的分配情况总体上与文献一致。各排放源的颗粒物排放因子跨越两个数量级。这项工作突出了使用离线分析的滤管内吸附剂样本推断生物质燃烧排放的气粒分配行为的潜力。这简化了针对旨在捕获所排放的全范围有机物的研究中S/I-VOC的采样和分析。