Aqueous OH photooxidation of atmospherically-relevant precursor-systems through laboratory experiments
Citation & Export
Hide
Simple citation
Kirkland, Jeffrey R..
Aqueous OH photooxidation of atmospherically-relevant precursor-systems through laboratory experiments. Retrieved from
https://doi.org/doi:10.7282/T3W094DM
Export
Description
TitleAqueous OH photooxidation of atmospherically-relevant precursor-systems through laboratory experiments
Date Created2014
Other Date2014-10 (degree)
Extent1 online resource (xv, 212 p. : ill.)
DescriptionChemistry in atmospheric waters (e.g., clouds, fogs, wet aerosols) is a critical component of our complex atmospheric system which affects global environmental health (e.g., climate, air quality). Laboratory, field, and modeling studies have shown that chemistry in atmospheric waters can alter gas-phase budgets of atmospheric oxidants (e.g., HO2) and change the mass and properties of organic aerosols. However, nearly half of organic matter dissolved in atmospheric waters remains uncharacterized and its chemistry unexplored. The result is error within predictive atmospheric models used to inform policymakers and mitigate harmful gas and particle exposures. To improve model predictions and implement appropriate policies, we must identify and include more detailed chemistry taking place in the atmosphere, specifically in atmospheric waters. This dissertation is focused on characterizing changes in dissolved organic matter during aqueous-phase chemical reactions (i.e., aqueous processing) and has implications for SOA contributions and atmospheric burdens of gas-phase species. First, the effects of ammonium and nitrate on dilute glyoxal plus hydroxyl radical (OH) chemistry in clouds are explored and support for radical-radical oligomer formation (e.g., tartarate) in wet aerosols is provided. Next, aqueous photooxidation of ambient water-soluble gases collected in the Po Valley, Italy is explored and amines are identified as potentially important participants in aqueous processing. These experiments also demonstrate formation of particle components (i.e., pyruvate, oxalate) explicitly from aqueous processing of ambient mixtures of water-soluble gases. Finally, aqueous processing of authentic fog waters from Fresno, California and the Po Valley, Italy is explored. Pyruvate and oxalate formation is again observed and precursors to aqueous processing are identified and compared to dissolved organic matter detected by others in fog and rainwater. This dissertation identifies potentially important precursors and products of aqueous processing; this contributes to an improved understanding of chemistry in atmospheric waters and the related environmental health effects. Precursors identified in this work are likely candidates for future laboratory experiments designed to elicit detailed aqueous chemistry for inclusion in predictive models.
NotePh.D.
NoteIncludes bibliographical references
Noteby Jeffrey R. Kirkland
Genretheses, ETD doctoral
Languageeng
CollectionGraduate School - New Brunswick Electronic Theses and Dissertations
Organization NameRutgers, The State University of New Jersey
RightsThe author owns the copyright to this work.