Predicting secondary organic aerosol phase state and viscosity and its effect on multiphase chemistry in a regional-scale air quality model
Abstract
Atmospheric aerosols are a significant public health hazard and have substantial impacts on the climate. Secondary organic aerosols (SOAs) have been shown to phase separate into a highly viscous organic outer layer surrounding an aqueous core. This phase separation can decrease the partitioning of semi-volatile and low-volatile species to the organic phase and alter the extent of acid-catalyzed reactions in the aqueous core. A new algorithm that can determine SOA phase separation based on their glass transition temperature (Tg), oxygen to carbon (O:C) ratio and organic mass to sulfate ratio, and meteorological conditions was implemented into the Community Multiscale Air Quality Modeling (CMAQ) system version 5.2.1 and was used to simulate the conditions in the continental United States for the summer of 2013. SOA formed at the ground/surface level was predicted to be phase separated with core–shell morphology, i.e., aqueous inorganic core surrounded by organic coating 65.4 % of the time during the 2013 Southern Oxidant and Aerosol Study (SOAS) on average in the isoprene-rich southeastern United States. Our estimate is in proximity to the previously reported ~70 % in literature. The phase states of organic coatings switched between semi-solid and liquid states, depending on the environmental conditions. The semi-solid shellmore »
- Authors:
-
- Univ. of North Carolina, Chapel Hill, NC (United States)
- Univ. of North Carolina, Chapel Hill, NC (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Univ. of North Carolina, Chapel Hill, NC (United States); Aerodyne Research, Inc., Billerica, MA (United States)
- Univ. of North Carolina, Chapel Hill, NC (United States); US Environmental Protection Agency (EPA), Research Triangle Park, NC (United States)
- Univ. of California, Riverside, CA (United States)
- Univ. of Washington, Seattle, WA (United States)
- Univ. of California, Berkeley, CA (United States)
- 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); National Institutes of Health (NIH)
- OSTI Identifier:
- 1650723
- Report Number(s):
- PNNL-SA-153998
Journal ID: ISSN 1680-7324
- Grant/Contract Number:
- AC05-76RL01830; AGS-1524731; AGS-1250569; AGS-1644406; AGS-1703535; SC0018221
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Atmospheric Chemistry and Physics (Online)
- Additional Journal Information:
- Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 20; Journal Issue: 13; Journal ID: ISSN 1680-7324
- Publisher:
- European Geosciences Union
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Aerosol dynamics; aerosol phase state and morphology; atmospheric modeling; tropospheric chemistry; reactive uptake
Citation Formats
Schmedding, Ryan, Rasool, Quazi Z., Zhang, Yue, Pye, Havala O. T., Zhang, Haofei, Chen, Yuzhi, Surratt, Jason D., Lopez-Hilfiker, Felipe D., Thornton, Joel A., Goldstein, Allen H., and Vizuete, William. Predicting secondary organic aerosol phase state and viscosity and its effect on multiphase chemistry in a regional-scale air quality model. United States: N. p., 2020.
Web. doi:10.5194/acp-20-8201-2020.
Schmedding, Ryan, Rasool, Quazi Z., Zhang, Yue, Pye, Havala O. T., Zhang, Haofei, Chen, Yuzhi, Surratt, Jason D., Lopez-Hilfiker, Felipe D., Thornton, Joel A., Goldstein, Allen H., & Vizuete, William. Predicting secondary organic aerosol phase state and viscosity and its effect on multiphase chemistry in a regional-scale air quality model. United States. https://doi.org/10.5194/acp-20-8201-2020
Schmedding, Ryan, Rasool, Quazi Z., Zhang, Yue, Pye, Havala O. T., Zhang, Haofei, Chen, Yuzhi, Surratt, Jason D., Lopez-Hilfiker, Felipe D., Thornton, Joel A., Goldstein, Allen H., and Vizuete, William. Thu .
"Predicting secondary organic aerosol phase state and viscosity and its effect on multiphase chemistry in a regional-scale air quality model". United States. https://doi.org/10.5194/acp-20-8201-2020. https://www.osti.gov/servlets/purl/1650723.
@article{osti_1650723,
title = {Predicting secondary organic aerosol phase state and viscosity and its effect on multiphase chemistry in a regional-scale air quality model},
author = {Schmedding, Ryan and Rasool, Quazi Z. and Zhang, Yue and Pye, Havala O. T. and Zhang, Haofei and Chen, Yuzhi and Surratt, Jason D. and Lopez-Hilfiker, Felipe D. and Thornton, Joel A. and Goldstein, Allen H. and Vizuete, William},
abstractNote = {Atmospheric aerosols are a significant public health hazard and have substantial impacts on the climate. Secondary organic aerosols (SOAs) have been shown to phase separate into a highly viscous organic outer layer surrounding an aqueous core. This phase separation can decrease the partitioning of semi-volatile and low-volatile species to the organic phase and alter the extent of acid-catalyzed reactions in the aqueous core. A new algorithm that can determine SOA phase separation based on their glass transition temperature (Tg), oxygen to carbon (O:C) ratio and organic mass to sulfate ratio, and meteorological conditions was implemented into the Community Multiscale Air Quality Modeling (CMAQ) system version 5.2.1 and was used to simulate the conditions in the continental United States for the summer of 2013. SOA formed at the ground/surface level was predicted to be phase separated with core–shell morphology, i.e., aqueous inorganic core surrounded by organic coating 65.4 % of the time during the 2013 Southern Oxidant and Aerosol Study (SOAS) on average in the isoprene-rich southeastern United States. Our estimate is in proximity to the previously reported ~70 % in literature. The phase states of organic coatings switched between semi-solid and liquid states, depending on the environmental conditions. The semi-solid shell occurring with lower aerosol liquid water content (western United States and at higher altitudes) has a viscosity that was predicted to be 102–1012 Pa s, which resulted in organic mass being decreased due to diffusion limitation. Organic aerosol was primarily liquid where aerosol liquid water was dominant (eastern United States and at the surface), with a viscosity <102 Pa s. Phase separation while in a liquid phase state, i.e., liquid–liquid phase separation (LLPS), also reduces reactive uptake rates relative to homogeneous internally mixed liquid morphology but was lower than aerosols with a thick viscous organic shell. The sensitivity cases performed with different phase-separation parameterization and dissolution rate of isoprene epoxydiol (IEPOX) into the particle phase in CMAQ can have varying impact on fine particulate matter (PM2.5) organic mass, in terms of bias and error compared to field data collected during the 2013 SOAS. This highlights the need to better constrain the parameters that govern phase state and morphology of SOA, as well as expand mechanistic representation of multiphase chemistry for non-IEPOX SOA formation in models aided by novel experimental insights.},
doi = {10.5194/acp-20-8201-2020},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 13,
volume = 20,
place = {United States},
year = {Thu Jul 16 00:00:00 EDT 2020},
month = {Thu Jul 16 00:00:00 EDT 2020}
}
Web of Science
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Kinetics and Products of the Acid-Catalyzed Ring-Opening of Atmospherically Relevant Butyl Epoxy Alcohols
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On the relationship between aerosol model uncertainty and radiative forcing uncertainty
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Unexpected Epoxide Formation in the Gas-Phase Photooxidation of Isoprene
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Diagnosis of venous disease and use of Doppler assessment
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Are diffusion coefficients calculated using the Stokes-Einstein equation combined with viscosities consistent with measured diffusion coefficients of tracer organics within organics-water mediums?
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Effect of relative humidity on SOA formation from isoprene/NO photooxidation: enhancement of 2-methylglyceric acid and its corresponding oligoesters under dry conditions
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Coupling of organic and inorganic aerosol systems and the effect on gas–particle partitioning in the southeastern US
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Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes–Einstein and fractional Stokes–Einstein relations
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Viscosities, diffusion coefficients, and mixing times of intrinsic fluorescent organic molecules in brown limonene secondary organic aerosol and tests of the Stokes–Einstein equation
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Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature)
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