Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions
Abstract
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 findmore »
- Authors:
-
[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)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF)
- OSTI Identifier:
- 1970743
- Report Number(s):
- PNNL-SA-180012
Journal ID: ISSN 2472-3452
- Grant/Contract Number:
- AC05-76RL01830; AGS-2039788
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Earth and Space Chemistry
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 4; Journal ID: ISSN 2472-3452
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; IEPOX-SOA; reactive uptake; acid-driven reactions; tetrol oligomerization; elevated relative humidity
Citation Formats
Zhang, Jie, Shrivastava, Manish, Zelenyuk, Alla, Zaveri, Rahul A., Surratt, Jason D., Riva, Matthieu, Bell, David M., and Glasius, Marianne. Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions. United States: N. p., 2023.
Web. doi:10.1021/acsearthspacechem.2c00358.
Zhang, Jie, Shrivastava, Manish, Zelenyuk, Alla, Zaveri, Rahul A., Surratt, Jason D., Riva, Matthieu, Bell, David M., & Glasius, Marianne. Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions. United States. https://doi.org/10.1021/acsearthspacechem.2c00358
Zhang, Jie, Shrivastava, Manish, Zelenyuk, Alla, Zaveri, Rahul A., Surratt, Jason D., Riva, Matthieu, Bell, David M., and Glasius, Marianne. Wed .
"Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions". United States. https://doi.org/10.1021/acsearthspacechem.2c00358. https://www.osti.gov/servlets/purl/1970743.
@article{osti_1970743,
title = {Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions},
author = {Zhang, Jie and Shrivastava, Manish and Zelenyuk, Alla and Zaveri, Rahul A. and Surratt, Jason D. and Riva, Matthieu and Bell, David M. and Glasius, Marianne},
abstractNote = {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.},
doi = {10.1021/acsearthspacechem.2c00358},
journal = {ACS Earth and Space Chemistry},
number = 4,
volume = 7,
place = {United States},
year = {Wed Mar 29 00:00:00 EDT 2023},
month = {Wed Mar 29 00:00:00 EDT 2023}
}
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