Air Quality Models and Unusually Large Ozone Increases: Identifying Model Failures, Understanding Environmental Causes, and Improving Modeled Chemistry Public Deposited

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Last Modified
  • March 21, 2019
Creator
  • Couzo, Evan Andrew
    • Affiliation: Gillings School of Global Public Health, Department of Environmental Sciences and Engineering
Abstract
  • Several factors combine to make ozone (O3) pollution in Houston, Texas, unique when compared to other metropolitan areas. These include complex meteorology, intense clustering of industrial activity, and significant precursor emissions from the heavily urbanized eight-county area. Decades of air pollution research have borne out two different causes, or conceptual models, of O3 formation. One conceptual model describes a gradual region-wide increase in O3 concentrations "typical" of many large U.S. cities. The other conceptual model links episodic emissions of volatile organic compounds to spatially limited plumes of high O3, which lead to large hourly increases that have exceeded 100 parts per billion (ppb) per hour. These large hourly increases are known to lead to violations of the federal O3 standard and impact Houston's status as a non-attainment area. There is a need to further understand and characterize the causes of peak O3 levels in Houston and simulate them correctly so that environmental regulators can find the most cost-effective pollution controls. This work provides a detailed understanding of unusually large O3 increases in the natural and modeled environments. First, we probe regulatory model simulations and assess their ability to reproduce the observed phenomenon. As configured for the purpose of demonstrating future attainment of the O3 standard, the model fails to predict the spatially limited O3 plumes observed in Houston. Second, we combine ambient meteorological and pollutant measurement data to identify the most likely geographic origins and preconditions of the concentrated O3 plumes. We find evidence that the O3 plumes are the result of photochemical activity accelerated by industrial emissions. And, third, we implement changes to the modeled chemistry to add missing formation mechanisms of nitrous acid, which is an important radical precursor. Radicals control the chemical reactivity of atmospheric systems, and perturbations to radical budgets can shift chemical pathways. The mechanism additions increase the concentrations of nitrous acid, especially right after sunrise. The overall effect on O3 is small (up to three ppb), but we demonstrate the successful implementation of a surface sub-model that chemically processes adsorbed compounds. To our knowledge, this is the first time that chemical processing on surfaces has been used in a three-dimensional regulatory air quality model.
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  • In Copyright
Advisor
  • Vizuete, William
Degree
  • Doctor of Philosophy
Graduation year
  • 2013
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