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Polycyclic aromatic hydrocarbon (PAH) redistribution in extreme dust storms and processing in clouds
Description
Dust storms known as 'haboobs' occur in the City of Tempe, AZ during the North American monsoon season. A haboob classification method based on meteorological and air quality measurements is described. There were from 3 to 20 haboob events per year over the period from 2005 to 2014. The calculated annual TSP (total suspended particulate) dry deposition during haboobs is estimated to contribute 74% of the total particulate mass deposited in Tempe, AZ.
Dry deposition is compared with the aqueous chemistry of Tempe Town Lake. Water management and other factors may have a stronger impact on Tempe Town Lake chemistry than haboob dry-deposition. Haboobs alter the Polycyclic Aromatic Hydrocarbon (PAH) concentrations and distributions in Tempe, AZ. PAH isomer ratios suggest PM2.5 (particulate matter with aerodynamic diameters less than or equal to 2.5 μm) sources consistent with approximate thunderstorm outflow paths.
The importance of the atmospheric aqueous phase, fogs and clouds, for the processing and removal of PAHs is not well known. A multiphase model was developed to determine the fate and lifetime of PAHs in fogs and clouds. The model employed literature values that describe the partitioning between three phases (aqueous, liquid organic, and gas), in situ PAH measurements, and experimental and estimated (photo)oxidation rates. At 25 °C, PAHs with two, three and four rings were predicted to be primarily gas phase (fraction in the gas phase xg > 90 %) while five- and six-ring PAHs partitioned significantly into droplets (xg < 60 %) with aqueous phase fractions of 1 to 6 % and liquid organic phase fractions of 31 to 91 %. The predicted atmospheric lifetimes of PAHs in the presence of fog or cloud droplets (< 5 hours) were significantly shorter than literature predictions of PAH wet and dry deposition lifetimes (1 to 14 days and 5 to 15 months respectively) and shorter than or equal to predicted PAH gas phase / particle phase atmospheric lifetimes (1 to 300 hours). The aqueous phase cannot be neglected as a PAH sink due to the large aqueous volume (vs. organic volume) and the relatively fast aqueous reactions.
Dry deposition is compared with the aqueous chemistry of Tempe Town Lake. Water management and other factors may have a stronger impact on Tempe Town Lake chemistry than haboob dry-deposition. Haboobs alter the Polycyclic Aromatic Hydrocarbon (PAH) concentrations and distributions in Tempe, AZ. PAH isomer ratios suggest PM2.5 (particulate matter with aerodynamic diameters less than or equal to 2.5 μm) sources consistent with approximate thunderstorm outflow paths.
The importance of the atmospheric aqueous phase, fogs and clouds, for the processing and removal of PAHs is not well known. A multiphase model was developed to determine the fate and lifetime of PAHs in fogs and clouds. The model employed literature values that describe the partitioning between three phases (aqueous, liquid organic, and gas), in situ PAH measurements, and experimental and estimated (photo)oxidation rates. At 25 °C, PAHs with two, three and four rings were predicted to be primarily gas phase (fraction in the gas phase xg > 90 %) while five- and six-ring PAHs partitioned significantly into droplets (xg < 60 %) with aqueous phase fractions of 1 to 6 % and liquid organic phase fractions of 31 to 91 %. The predicted atmospheric lifetimes of PAHs in the presence of fog or cloud droplets (< 5 hours) were significantly shorter than literature predictions of PAH wet and dry deposition lifetimes (1 to 14 days and 5 to 15 months respectively) and shorter than or equal to predicted PAH gas phase / particle phase atmospheric lifetimes (1 to 300 hours). The aqueous phase cannot be neglected as a PAH sink due to the large aqueous volume (vs. organic volume) and the relatively fast aqueous reactions.
ContributorsEagar, Jershon (Author) / Herckes, Pierre (Thesis advisor) / Hayes, Mark (Committee member) / Shock, Everett (Committee member) / Arizona State University (Publisher)
Created2016