Source- and Age-Resolved Mechanistic Air Quality Models: Model Development and Application in Southeast Texas

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2012-07-16

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Abstract

Ozone (O3) and particulate matter (PM) existing in the atmosphere have adverse effects to human and environment. Southeast Texas experiences high O3 and PM events due to special meteorological conditions and high emission rates of volatile organic compounds (VOCs) and nitrogen oxides (NOx). Quantitative knowledge of the contributions of different emissions sources to O3 and PM is helpful to better understand their formation mechanisms and develop effective control strategies. Tagged reactive tracer techniques are developed and coupled into two chemical transport models (UCD/CIT model and CMAQ) to conduct source apportionment of O3, primary PM, secondary inorganic PM, and secondary organic aerosol (SOA) and aging distribution of elemental carbon (EC) and organic carbon (OC). Ozone (O3) and particulate matter (PM) existing in the atmosphere have adverse effects to human and environment. Southeast Texas experiences high O3 and PM events due to special meteorological conditions and high emission rates of volatile organic compounds (VOCs) and nitrogen oxides (NOx). Quantitative knowledge of the contributions of different emissions sources to O3 and PM is helpful to better understand their formation mechanisms and develop effective control strategies. Tagged reactive tracer techniques are developed and coupled into two chemical transport models (UCD/CIT model and CMAQ) to conduct source apportionment of O3, primary PM, secondary inorganic PM, and secondary organic aerosol (SOA) and aging distribution of elemental carbon (EC) and organic carbon (OC). Models successfully reproduce the concentrations of gas phase and PM phase species. Vehicles, natural gas, industries, and coal combustion are important O3 sources. Upwind sources have non-negligible influences (20-50%) on daytime O3, indicating that regional NOx emission controls are necessary to reduce O3 in Southeast Texas. EC is mainly from diesel engines while majority of primary OC is from internal combustion engines and industrial sources. Open burning, road dust, internal combustion engines and industries are the major sources of primary PM2.5. Wildfire dominates primary PM near fire locations. Over 80% of sulfate is produced in upwind areas and coal combustion contributes most. Ammonium ion is mainly from agriculture sources. The SOA peak values can be better predicted when the emissions are adjusted by a factor of 2. 20% of the total SOA is due to anthropogenic sources. Solvent and gasoline engines are the major sources. Oligomers from biogenic SOA account for 30-58% of the total SOA, indicating that long range transport is important. PAHs from anthropogenic sources can produce 4% of total anthropogenic SOA. Wild fire, vehicles, solvent and industries are the major sources. EC and OC emitted within 0-3 hours contribute approximately 70-90% in urban Houston and about 20-40% in rural areas. Significant diurnal variations in the relative contributions to EC are predicted. Fresh particles concentrations are high at morning and early evening. The concentrations of EC and OC that spend more than 9 hours in the air are low over land but almost accounts for 100% of the total EC and OC over the ocean.

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chemical transport model, source apportionment technique, ozone, particulate matter, aging distribution, Southeast Texas

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