Document Type

Dissertation

Date of Degree

Summer 2016

Degree Name

PhD (Doctor of Philosophy)

Degree In

Chemistry

First Advisor

Elizabeth A. Stone

Abstract

When inhaled, bioaerosols exacerbate respiratory symptoms and diseases. Mitigating the negative health impacts of bioaerosols requires a robust understanding of the temporal and spatial dynamics of bioaerosols in the atmosphere as a function of their type (e.g., bacteria, fungal spores, plant pollens) and particle size, which determines their penetration into the respiratory tract. While it is known that bioaerosol concentrations vary by location, season and meteorological conditions, major gaps remain in understanding the co-occurrence of bioaerosols with one another, their size in the atmosphere, and their mass contributions to PM. Overall, research presented in this thesis advances the current knowledge about bioaerosols (including fungal spores, pollens, and bacteria) in following ways: 1) defining background and urban levels of bioaerosol concentrations in the Midwestern US across four seasons, 2) characterizing ambient bioaerosol and co-pollutant mixtures, 3) determining the influence of meteorology on their concentrations and size distributions, and 4) estimating bioaerosol contributions to PM mass.

The spatial analysis of respirable particulate matter (PM10) across urban and background sites in Iowa demonstrated that urban areas are a source of fungal glucans, bacterial endotoxins and total proteins, which gives rise to significantly enhanced bioaerosols in urban locations compared to background sites. Similar urban enhancements in calcium—a crustal element—and its correlation with endotoxins suggested that wind-blown soil is likely the origin. Seasonally, fungal spores peaked in summer with temperature, while bacterial endotoxins peaked in autumn during the row crop harvesting season. Fungal spores, bacterial endotoxins, plant and animal detritus all peaked during the growing season, such that maximum exposures to multiple bioaerosol types concurrently. Under the influence of rain chemical tracers of pollens peaked and decreased in size from coarse (2.5-10 µm) to fine particles (< 2.5 µm), likely due to the osmotic rupture of pollen grains upon wetting. While fine-sized fungal spores also increased during rain events, maximum spore levels were observed in coarse-sized particles post-rain. The comparison of spring to late summer measurements demonstrated these influences of precipitation on bioaerosols also occur during late summer, when fungal spore levels are high and ragweed is the dominant pollen source. The ability to apportion PM mass to bioaerosols was advanced through the development of chemical profiles of pollens and their integration with chemical mass balance (CMB) source apportionment modeling, for the first time. In late-April to early-May in 2013, pollens were estimated to contribute 0.2 - 38% of PM₁₀ (0.04 – 0.8 µg m⁻³) while fungal spores contributed 0.7 – 17% of PM₁₀ (0.1 – 1.5 µg m⁻³). Collectively, this thesis provides insight into spatial, seasonal and daily variations of bioaerosols, and shows elevated outdoor exposures to bioaerosols among urban populations, with maximum levels occurring during growing seasons, periods of high temperature, and during/immediately following rainfall.

Keywords

Bioaerosols, Carbohydrate, Fungal spores, HPAEC-PAD, Midwest, Particulate matter

Pages

xiv, 144

Bibliography

126-144

Copyright

Copyright 2016 Chathurika Mihirani Rathnayake

Included in

Chemistry Commons

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