Determining Activity Coefficients of SOA from Isothermal Evaporation in a Laboratory Chamber

Liu, Xiaoxi; Day, Douglas A.; Krechmer, Jordan E.; Ziemann, Paul J.; Jimenez, Jose L.

doi:10.1021/acs.estlett.0c00888

Determining Activity Coefficients of SOA from Isothermal Evaporation in a Laboratory Chamber

Journal Article · Tue Dec 29 00:00:00 EST 2020 · Environmental Science & Technology Letters (Online)

DOI:https://doi.org/10.1021/acs.estlett.0c00888· OSTI ID:1773505

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Univ. of Colorado, Boulder, CO (United States)

Nonideal molecular interactions in aerosol particles influence the partitioning of semivolatile organic compounds (SVOCs). However, few direct measurements exist that determine activity coefficients (γ), which quantify nonideality, for individual organic compounds in different atmospheric mixtures. By measuring the isothermal evaporation of SOA formed from multifunctional SVOCs in an environmental chamber, this study determines the mole-fraction-based γ of the bulk SOA in a variety of pre-existing chemically complex particles, approximated as if the bulk SOA behaved like a single SVOC. These multicomponent mixtures contain molecular structures commonly found in the atmosphere. When treated as a single liquid phase, γ of the bulk SOA tends to increase from ~1 to ~5 as the organic seeds and the SOA have more differing polarities. A high computed γ value of 74 for a wet ammonium sulfate-SOA system indicates phase separation. The γ for some individual species was also quantified based on gas-phase measurements and AIOMFAC model predictions. However, the bulk SOA γ cannot be explained by the simplified speciated SVOC–seed interactions, suggesting incomplete compositional understanding of the bulk SOA. In this work, these results demonstrate a method to quantify nonideal behavior and show that it can occur in multicomponent mixtures and therefore influence OA formation, evolution, and lifetimes.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM), Data Center

Sponsoring Organization:: Cooperative Institute for Research in Environmental Sciences (CIRES); National Science Foundation (NSF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Contributing Organization:: Argonne National Laboratory (ANL); Brookhaven National Laboratory (BNL); Oak Ridge National Laboratory (ORNL); Pacific Northwest National Laboratory (PNNL)

Grant/Contract Number:: SC0016559

OSTI ID:: 1773505

Journal Information:: Environmental Science & Technology Letters (Online), Journal Name: Environmental Science & Technology Letters (Online) Journal Issue: 3 Vol. 8; ISSN 2328-8930

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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