Fine Particulate Matter Source Apportionment for the Chemical Speciation Trends Network Site at Birmingham, Alabama, Using Positive Matrix Factorization

摘要

The Positive Matrix Factorization (PMF) receptor model version 1.1 was used with data from the fine particulate matter (PM_(2.5)) Chemical Speciation Trends Network (STN) to estimate source contributions to ambient PM_(2.5) 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 PM_(2.5) and exhibit strong seasonality (37 ± 10% winter vs. 55 ± 16% summer average). Motor vehicle emissions constitute the biggest primary PM_(2.5) mass contribution with almost 25 ± 2% long-term average and winter maximum of 29 ± 11%. PM_(2.5) 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.