Murphy Benjamin N, Sonntag Darrell, Seltzer Karl M, Pye Havala O T, Allen Christine, Murray Evan, Toro Claudia, Gentner Drew R, Huang Cheng, Jathar Shantanu, Li Li, May Andrew A, Robinson Allen L
Center for Environmental Measurement and Modeling, U.S. Environmental Protection Agency, Research Triangle Park, NC 27711, United States.
Department of Civil and Construction Engineering, Brigham Young University, Provo, UT 84602, United States.
Atmos Chem Phys. 2023 Oct 25;23(20):13469-13483. doi: 10.5194/acp-23-13469-2023.
Mobile sources are responsible for a substantial controllable portion of the reactive organic carbon (ROC) emitted to the atmosphere, especially in urban environments of the United States. We update existing methods for calculating mobile source organic particle and vapor emissions in the United States with over a decade of laboratory data that parameterize the volatility and organic aerosol (OA) potential of emissions from on-road vehicles, nonroad engines, aircraft, marine vessels, and locomotives. We find that existing emission factor information from Teflon filters combined with quartz filters collapses into simple relationships and can be used to reconstruct the complete volatility distribution of ROC emissions. This new approach consists of source-specific filter artifact corrections and state-of-the-science speciation including explicit intermediate-volatility organic compounds (IVOCs), yielding the first bottom-up volatility-resolved inventory of US mobile source emissions. Using the Community Multiscale Air Quality model, we estimate mobile sources account for 20 %-25 % of the IVOC concentrations and 4.4 %-21.4 % of ambient OA. The updated emissions and air quality model reduce biases in predicting fine-particle organic carbon in winter, spring, and autumn throughout the United States (4.3 %-11.3 % reduction in normalized bias). We identify key uncertain parameters that align with current state-of-the-art research measurement challenges.
移动源是排放到大气中的活性有机碳(ROC)的一个相当大的可控部分的来源,尤其是在美国的城市环境中。我们利用十多年的实验室数据更新了美国计算移动源有机颗粒物和蒸汽排放的现有方法,这些数据对道路车辆、非道路发动机、飞机、船舶和机车排放的挥发性和有机气溶胶(OA)潜力进行了参数化。我们发现,来自聚四氟乙烯过滤器与石英过滤器的现有排放因子信息可归纳为简单关系,并可用于重建ROC排放的完整挥发性分布。这种新方法包括特定源的过滤器伪影校正和最新的物种形成,包括明确的中挥发性有机化合物(IVOCs),从而产生了美国移动源排放的第一个自下而上的挥发性解析清单。使用社区多尺度空气质量模型,我们估计移动源占IVOC浓度的20%-25%,占环境OA的4.4%-21.4%。更新后的排放和空气质量模型减少了在美国冬季、春季和秋季预测细颗粒有机碳时的偏差(归一化偏差降低4.3%-11.3%)。我们确定了与当前最先进的研究测量挑战相一致的关键不确定参数。