Nontargeted Tandem Mass Spectrometry Analysis Reveals Diversity and Variability in Aerosol Functional Groups across Multiple Sites, Seasons, and Times of Day
- Jenna C. DittoJenna C. DittoDepartment of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06511, United StatesMore by Jenna C. Ditto,
- Taekyu JooTaekyu JooSchool of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia 30332, United StatesMore by Taekyu Joo,
- Jonathan H. SladeJonathan H. SladeDepartment of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92093, United StatesMore by Jonathan H. Slade,
- Paul B. ShepsonPaul B. ShepsonSchool of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, New York 11794, United StatesMore by Paul B. Shepson,
- Nga L. NgNga L. NgSchool of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia 30332, United StatesSchool of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United StatesMore by Nga L. Ng, and
- Drew R. Gentner*Drew R. Gentner*E-mail: [email protected]. Phone: (203) 432-4382.Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06511, United StatesMore by Drew R. Gentner
Abstract
Organic aerosol (OA) is a complex mixture of compounds with diverse elemental and structural features, and its composition affects its health and environmental impacts. A detailed speciation of the functional group distribution in OA is important for constraining atmospheric reaction pathways and products, evaluating chemical mechanisms and models, and understanding OA impacts. We used high-resolution tandem mass spectrometry to perform a nontargeted analysis of OA functional groups from three diverse ambient sites across times of day and seasons. We observed a range of oxygen-, nitrogen-, and/or sulfur-containing functional groups, including oxygenates such as hydroxyls (29–69%) and carboxylic acids (19–59%), that dominated the functional group distribution and that may participate in hydrogen bonding and thus impact the chemical and physical properties of OA (percentages indicate average ion abundance contributions across campaigns). We also observed esters (7–39%) and ethers (13–42%) that suggest the importance of oligomerization. On average, organonitrates represented only 12% of identified nitrogen-containing groups and organosulfates represented 21% of identified sulfur-containing groups, while we observed many other nitrogen- and/or sulfur-containing structures that were important contributors to OA composition (e.g., amines, imines, nitrophenols, and sulfides). Most compounds (81%) were multifunctional and likely multigenerational oxidation products, which typically contained two to five functional groups in total.
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