In 2005, Park et al., developed a new Pseudo-Deterministic Receptor Model (PDRM) to apportion SO2 and ambient particulate matter (PM) constituents to local sources near Tampa Bay. Ambient pollutant measurements were fit to products of emission rates and dispersion factors constrained with a Gaussian plume model for individual sources. In our study, the original samples were reanalyzed by ICPMS for 10 additional elements to improve the resolving power. Chemical mass balance (CMB) terms were added to PDRM to allow fitting of background aerosol sources. More accurate curvilinear plume trajectories were computed to predict arrival times in both surface and aloft layers. This allowed application of the PDRM to complicated meteorological conditions, e.g. wind shifts. Predicted emission rates for particle-bound elements were constrained using chemical compositional information obtained from published source profiles for generic source types. Constraints applied to emissions of known tracer species allowed the "conditioning" of dispersion factor temporal profiles to tracer species concentration profiles. This enabled the model to apportion pollutants to individual sources with intermittent emissions, the omission of which in Park et al. lead to significant residuals. Excellent fits were obtained for all modeled pollutants: 14 of 22 species have Normalized Mean Square Errors (NMSE) < 2.5%, and 21 of 22 have values < 8%. These were improved for SO 2 and 8 of 10 elements (by 7-35% for Al, Cu, Ni, Pb, and Zn) modeled by Park et al. Our predicted emission rates are in much better agreement with chemical compositions for generic source types. Key results include: (1) predicted SO2 contributions to ambient levels from a small, lead battery recycling plant were reduced from 50-59% at its peak influence to a more reasonable 2-4%, (2) Pb/Zn ratios from that plant increased from 1.0 to 734 and better agree with published ratios of 67-440, (3) predicted Ni emission rates for one of the oil-fired power plants (OFPP) was increased by 100-fold (larger than Park's), and now better agrees with its published National Emissions Inventory (NEI) emission rate and with X/Ni ratios for generic OFPP emissions derived from EPA's SPECIATE database, and (4) our predicted emission rates for hazardous air pollutants and toxics from power plants agree within a factor of 5 for ∼75% of the annual emission rates reported in the NEI and Toxic Release Inventories (TRI). This suggests that NEI and TRI data provide good qualitative emission estimates, but should not be treated as accurate in a predictive model to quantify source emissions. It was also observed that the TRI values for As emission rates from coal-fired power plants are more accurate that their NEI values.
|Advisor:||Ondov, John M.|
|Commitee:||Blough, Neil, Hudson, Robert, Mignerey, Alice, Walters, William|
|School:||University of Maryland, College Park|
|School Location:||United States -- Maryland|
|Source:||DAI-B 71/03, Dissertation Abstracts International|
|Subjects:||Analytical chemistry, Environmental science|
|Keywords:||Ambient particulate matter, ICPMS slurry analysis, Plume dispersion, Point source emission rates, Receptor modeling, Source apportionment, Trace elemental analysis|
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