Molecular Characterization of Organosulfate-Dominated Aerosols over Agricultural Fields from the Southern Great Plains by High-Resolution Mass Spectrometry

Vandergrift, Gregory W.; Shawon, Abu Sayeed Md; Dexheimer, Darielle N.; Zawadowicz, Maria A.; Mei, Fan; China, Swarup

doi:10.1021/acsearthspacechem.2c00043

Title: Molecular Characterization of Organosulfate-Dominated Aerosols over Agricultural Fields from the Southern Great Plains by High-Resolution Mass Spectrometry

Journal Article · Tue May 10 00:00:00 EDT 2022 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.2c00043· OSTI ID:1871194

Vandergrift, Gregory W. ^[1];

^[2]; Dexheimer, Darielle N. ^[3];

^[4];

^[5];

^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL); Michigan Technological Univ., Houghton, MI (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

The molecular composition of organic aerosols, especially for day/nighttime variations of organosulfates above agricultural fields, is not well understood despite profound impacts on regional climate, crop production, air quality, and human health. Here, nanospray desorption electrospray ionization with high-resolution mass spectrometry (nano-DESI-HRMS) is used to interrogate the molecular composition of organic aerosols collected at the Southern Great Plains, located in an agricultural region of Oklahoma. Identified molecular formulae featured carbon, hydrogen, oxygen (CHO), nitrogen (CHNO), and/or sulfur (CHOS, CHNOS), with higher organosulfate proportions during daytime (41%) compared to nighttime (30%). In this work, nighttime aerosols featured increases in CHO, CHNO, and extremely low volatility organic carbon (ELVOC) species. However, due to high relative humidity, the nighttime aerosols phase state was found to be more liquid-like than daytime aerosols using parametrized glass transition temperatures. Aerosol molecular composition from an anthropogenically influenced plume (southerly winds) showed significant increases in CHOS and ELVOC species. By comparison with chamber studies, CHOS species are suspected to be of mixed biogenic and anthropogenic origin, whereas CHNOS species (not identified in the southerly winds) are suggested to predominately be of biogenic origin. Overall, this study provides key insight into organosulfates above agricultural fields, demonstrating dependence upon day/night cycles and episodic anthropogenic emissions.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830; FG03-97ER62338; FG03-00ER62913

OSTI ID:: 1871194

Alternate ID(s):: OSTI ID: 1877105

Report Number(s):: PNNL-SA-170176

Journal Information:: ACS Earth and Space Chemistry, Vol. 6, Issue 7; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Molecular Characterization of Organosulfate-Dominated Aerosols over Agricultural Fields from the Southern Great Plains by High-Resolution Mass Spectrometry

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