Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions

Zhang, Jie; Shrivastava, Manish; Zelenyuk, Alla; Zaveri, Rahul A.; Surratt, Jason D.; Riva, Matthieu; Bell, David M.; Glasius, Marianne

doi:10.1021/acsearthspacechem.2c00358

Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions

Journal Article · Wed Mar 29 00:00:00 EDT 2023 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.2c00358· OSTI ID:1970743

Zhang, Jie ^[1]; ^[1]; Zelenyuk, Alla ^[1]; ^[1]; ^[2]; ^[3]; ^[4];

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
University of North Carolina, Chapel Hill, NC (United States)
University of Lyon (France)
Paul Scherrer Institute (PSI), Villigen (Switzerland)

Isoprene is the non-methane volatile organic compound (VOC) emitted in largest amounts to the atmosphere, and it is a significant source of secondary organic aerosol (SOA) mass. The uptake of isoprene oxidation products followed by multiphase chemistry in fine particles is the key pathway to form isoprene epoxydiol-derived SOA (IEPOX-SOA). However, many parameters that relate to diffusion and reaction of IEPOX in the particle phase remain uncertain, since reaction kinetics previously measured in bulk aqueous phase solutions might be different from atmospheric aerosols. Here, we use simultaneous environmental chamber measurements of multiple parameters governing IEPOX-SOA formation at timescales of ~hours: particle size distribution, composition, and volatility of IEPOX-SOA to constrain the key parameters governing IE-POX-SOA formation under humid (i.e., 50% relative humidity, RH) and varying seed aerosol acidity conditions. Reducing the 2-methyltetrol (tetrol) reaction rate constants by a factor of 4 brings the model predictions in agreement with the IEPOX-SOA measurements with acidified ammonium bisulfate seed aerosols. For less acidic ammonium sulfate aerosols both the organo-sulfate (OS) and tetrol reaction rate constants need to be reduced to bring model predictions closer to chamber observations. Using the measured non-volatile content of IEPOX-SOA we constrain the oligomerization timescale of 2-methyltetrols. We find that the oligomerization timescale is 4 hours with acidified seed aerosols, but a much longer time scale of 24 hours is needed for non-acidified seed aerosols, indicating that the aerosol acidity greatly affects the oligomerization rate of tetrols. Here we show that the actual kinetics of IEPOX-SOA formation rate on aerosol seeds consisting of both ammonium bisulfate and ammonium sulfate are a factor of 4~5 slower under 50-60% RH conditions compared to their application in previous models, which were based on bulk aqueous solution measurements.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

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

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1970743

Report Number(s):: PNNL-SA-180012

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 4 Vol. 7; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
IEPOX-SOA
acid-driven reactions
elevated relative humidity
reactive uptake
tetrol oligomerization

Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions

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