Date of Award

Spring 1-1-2013

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Mechanical Engineering

First Advisor

Michael P. Hannigan

Second Advisor

Shelly L. Miller

Third Advisor

Jana B. Milford

Fourth Advisor

Fernando L. Rosario-Ortiz

Fifth Advisor

Daven K. Henze

Abstract

Particulate matter in the troposphere adversely impacts human health when inhaled and alters climate through cloud formation processes and by absorbing/scattering light. Particles smaller than 2.5 μm in diameter (fine particulate matter; PM10-2.5), are typically emitted from combustion-related sources and can form and grow through secondary processing in the atmosphere. Coarse particles (PM10-2.5), ranging 2.5 to 10 μm, are typically generated through abrasive processes, such as erosion of road surfaces, entrained via resuspension, and settle quickly out of the atmosphere due to their large size. After deciding against regulating PM10-2.5 in 2006 citing, among other reasons, mixed results from epidemiological studies of the pollutant and lack of knowledge on health impacts in rural areas, the United States Environmental Protection Agency (US EPA) funded a series of studies that investigated the ambient composition, toxicology, and epidemiology of PM10-2.5. One such study, The Colorado Coarse Rural-Urban Sources and Health (CCRUSH) study, aimed to characterize the composition, sources, and health effects of PM10-2.5 in semi-arid northeastern Colorado and consisted of two field campaigns and an epidemiological study. Summarized here are the results from the two field campaigns, the first of which included over three years of continuous PM10-2.5 and PM2.5 mass concentration monitoring at multiple sites in urban-Denver and rural-Greeley, Colorado. This data set was used to characterize the spatiotemporal variability of PM10-2.5 and PM2.5. During the second year of continuous monitoring, PM10-2.5 and PM2.5 filter samples were collected for compositional analyses that included: elemental composition, bulk elemental and organic carbon concentrations, water-soluble organic carbon concentrations, UV-vis absorbance, fluorescence spectroscopy, and endotoxin content. Elemental composition was used to understand enrichment of trace elements in atmospheric particles and to identify sources via positive matrix factorization (PMF). The organic fraction of both particulate size ranges was explored with a variety of bulk characterization techniques commonly utilized in analysis of soil and aquatic natural organic matter. To date, the CCRUSH study is one of the largest research efforts devoted to understanding PM10-2.5 and provides the US EPA with vital information that will be used in future policy making decisions regarding the regulation of this pollutant.

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