Graduate Thesis Or Dissertation
 

Trans-Pacific and regional atmospheric transport of anthropogenic semivolatile organic compounds in the western U.S.

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  • The atmospheric transport of anthropogenic semivolatile organic compounds (SOCs) from Asian sources to the Western U.S. was investigated. In addition, the SOC extraction method was optimized. Hansen solubility parameter plots were used to aid in the pressurized liquid extraction (PLE) solvent selection of air sampling media in order to minimize polymeric matrix interferences. To estimate the emissions of anthropogenic semivolatile organic compounds (SOCs) from East Asia and to identify unique SOC molecular markers in Asian air masses, air samples were collected on the island of Okinawa, Japan in Spring 2004. Elevated concentrations of hexachlorobenzene (HCB), hexachlorocyclohexanes (HCHs), dichlorodiphenyltrichloroethanes (DDTs), and particulate-phase polycyclic aromatic hydrocarbons (PAHs) were attributed to air masses from China. A large proportion of the variation in the current use pesticides, gas-phase PAHs, and polychlorinated biphenyl (PCB) concentrations was explained by meteorology. Using measured PAH, carbon monoxide (CO), and black carbon concentrations and estimated CO and black carbon emission inventories, the emission of 6 carcinogenic particulate-phase PAHs were estimated to be 1518-4179 metric tons/year for all of Asia and 778-1728 metric tons/year for only China. Atmospheric measurements of anthropogenic SOCs were made at Mt. Bachelor Observatory (MBO), located in Oregon’s Cascade Range. PAH concentrations at MBO increased with the percentage of air mass time in Asia and, in conjunction with other data, provided strong evidence that particulate-phase PAHs are emitted from Asia and undergo trans-Pacific atmospheric transport to North America. Enhanced HCB, α-HCH, and γ-HCH concentrations also occurred during trans-Pacific atmospheric transport, compared with regional (Western U.S.) air masses during similar time periods. Gas-phase PAH and fluorotelomer alcohol (FTOH) concentrations significantly increased with the percentage of air mass time in California’s urban areas, while retene and PCB concentrations increased with the percentage of air mass time in Oregon and during regional fire events. Regional atmospheric transport in the Western U.S. also resulted in enhanced γ-HCH, dacthal, endosulfan, metribuzin, triallate, trifluralin, and chlorpyrifos concentrations, with episodic concentration enhancements during spring application periods. Elevated ΣPCB, Σchlordane, HCHs, HCB, and trifuralin concentrations were also associated with fires, which may be due to volatization of pesticides deposited to soils and vegetation.
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