Baumann Karsten, Jayanty R K M, Flanagan James B
Research Triangle Institute International, Research Triangle Park, NC, USA.
J Air Waste Manag Assoc. 2008 Jan;58(1):27-44. doi: 10.3155/1047-3289.58.1.27.
The Positive Matrix Factorization (PMF) receptor model version 1.1 was used with data from the fine particulate matter (PM2.5) Chemical Speciation Trends Network (STN) to estimate source contributions to ambient PM2.5 in a highly industrialized urban setting in the southeastern United States. Model results consistently resolved 10 factors that are interpreted as two secondary, five industrial, one motor vehicle, one road dust, and one biomass burning sources. The STN dataset is generally not corrected for field blank levels, which are significant in the case of organic carbon (OC). Estimation of primary OC using the elemental carbon (EC) tracer method applied on a seasonal basis significantly improved the model's performance. Uniform increase of input data uncertainty and exclusion of a few outlier samples (associated with high potassium) further improved the model results. However, it was found that most PMF factors did not cleanly represent single source types and instead are "contaminated" by other sources, a situation that might be improved by controlling rotational ambiguity within the model. Secondary particulate matter formed by atmospheric processes, such as sulfate and secondary OC, contribute the majority of ambient PM2.5 and exhibit strong seasonality (37 +/- 10% winter vs. 55 +/- 16% summer average). Motor vehicle emissions constitute the biggest primary PM2.5 mass contribution with almost 25 +/- 2% long-term average and winter maximum of 29 +/- 11%. PM2.5 contributions from the five identified industrial sources vary little with season and average 14 +/- 1.3%. In summary, this study demonstrates the utility of the EC tracer method to effectively blank-correct the OC concentrations in the STN dataset. In addition, examination of the effect of input uncertainty estimates on model results indicates that the estimated uncertainties currently being provided with the STN data may be somewhat lower than the levels needed for optimum modeling results.
正矩阵因子分解(PMF)受体模型1.1版被用于分析来自细颗粒物(PM2.5)化学形态趋势网络(STN)的数据,以估算美国东南部一个高度工业化城市环境中,各类源对环境空气中PM2.5的贡献。模型结果一致解析出10个因子,分别被解释为两个二次源、五个工业源、一个机动车源、一个道路扬尘源和一个生物质燃烧源。STN数据集通常未针对现场空白水平进行校正,而这在有机碳(OC)的情况下较为显著。使用基于季节应用的元素碳(EC)示踪法估算一次有机碳,显著改善了模型的性能。统一增加输入数据的不确定性,并排除一些异常样本(与高钾相关),进一步改善了模型结果。然而,研究发现大多数PMF因子并不能清晰地代表单一源类型,而是被其他源“污染”,这种情况可能通过控制模型内的旋转模糊性得到改善。由大气过程形成的二次颗粒物,如硫酸盐和二次有机碳,占环境空气中PM2.5的大部分,并呈现出强烈的季节性(冬季平均为37±10%,夏季平均为55±16%)。机动车排放构成了一次PM2.5质量贡献的最大部分,长期平均贡献约为25±2%,冬季最高可达29±11%。五个已识别工业源的PM2.5贡献随季节变化不大,平均为14±1.3%。总之,本研究证明了EC示踪法在有效校正STN数据集中OC浓度方面的实用性。此外,对输入不确定性估计对模型结果影响的检验表明,目前随STN数据提供的估计不确定性可能略低于获得最佳建模结果所需的水平。