Predictions of the glass transition temperature and viscosity of organic aerosols from volatility distributions
Abstract
Volatility and viscosity are important properties of organic aerosols (OA), affecting aerosol processes such as formation, evolution, and partitioning of OA. Volatility distributions of ambient OA particles have often been measured, while viscosity measurements are scarce. We have previously developed a method to estimate the glass transition temperature (Tg) of an organic compound containing carbon, hydrogen, and oxygen. Based on analysis of over 2400 organic compounds including oxygenated organic compounds, as well as nitrogen- and sulfur-containing organic compounds, we extend this method to include nitrogen- and sulfur-containing compounds based on elemental composition. In addition, parameterizations are developed to predict Tg as a function of volatility and the atomic oxygen-to-carbon ratio based on a negative correlation between Tg and volatility. This prediction method of Tg is applied to ambient observations of volatility distributions at 11 field sites. The predicted Tg values of OA under dry conditions vary mainly from 290 to 339 K and the predicted viscosities are consistent with the results of ambient particle-phase-state measurements in the southeastern US and the Amazonian rain forest. Reducing the uncertainties in measured volatility distributions would improve predictions of viscosity, especially at low relative humidity. We also predict the Tg of OA components identifiedmore »
- Authors:
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1638300
- Alternate Identifier(s):
- OSTI ID: 1756446
- Grant/Contract Number:
- SC0018349; SC0016559; AGS-1654104; AGS-1822664
- Resource Type:
- Published Article
- 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:
- Copernicus Publications, EGU
- Country of Publication:
- Germany
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES
Citation Formats
Li, Ying, Day, Douglas A., Stark, Harald, Jimenez, Jose L., and Shiraiwa, Manabu. Predictions of the glass transition temperature and viscosity of organic aerosols from volatility distributions. Germany: N. p., 2020.
Web. doi:10.5194/acp-20-8103-2020.
Li, Ying, Day, Douglas A., Stark, Harald, Jimenez, Jose L., & Shiraiwa, Manabu. Predictions of the glass transition temperature and viscosity of organic aerosols from volatility distributions. Germany. https://doi.org/10.5194/acp-20-8103-2020
Li, Ying, Day, Douglas A., Stark, Harald, Jimenez, Jose L., and Shiraiwa, Manabu. Mon .
"Predictions of the glass transition temperature and viscosity of organic aerosols from volatility distributions". Germany. https://doi.org/10.5194/acp-20-8103-2020.
@article{osti_1638300,
title = {Predictions of the glass transition temperature and viscosity of organic aerosols from volatility distributions},
author = {Li, Ying and Day, Douglas A. and Stark, Harald and Jimenez, Jose L. and Shiraiwa, Manabu},
abstractNote = {Volatility and viscosity are important properties of organic aerosols (OA), affecting aerosol processes such as formation, evolution, and partitioning of OA. Volatility distributions of ambient OA particles have often been measured, while viscosity measurements are scarce. We have previously developed a method to estimate the glass transition temperature (Tg) of an organic compound containing carbon, hydrogen, and oxygen. Based on analysis of over 2400 organic compounds including oxygenated organic compounds, as well as nitrogen- and sulfur-containing organic compounds, we extend this method to include nitrogen- and sulfur-containing compounds based on elemental composition. In addition, parameterizations are developed to predict Tg as a function of volatility and the atomic oxygen-to-carbon ratio based on a negative correlation between Tg and volatility. This prediction method of Tg is applied to ambient observations of volatility distributions at 11 field sites. The predicted Tg values of OA under dry conditions vary mainly from 290 to 339 K and the predicted viscosities are consistent with the results of ambient particle-phase-state measurements in the southeastern US and the Amazonian rain forest. Reducing the uncertainties in measured volatility distributions would improve predictions of viscosity, especially at low relative humidity. We also predict the Tg of OA components identified via positive matrix factorization of aerosol mass spectrometer (AMS) data. The predicted viscosity of oxidized OA is consistent with previously reported viscosity of secondary organic aerosols (SOA) derived from α-pinene, toluene, isoprene epoxydiol (IEPOX), and diesel fuel. Comparison of the predicted viscosity based on the observed volatility distributions with the viscosity simulated by a chemical transport model implies that missing low volatility compounds in a global model can lead to underestimation of OA viscosity at some sites. The relation between volatility and viscosity can be applied in the molecular corridor or volatility basis set approaches to improve OA simulations in chemical transport models by consideration of effects of particle viscosity in OA formation and evolution.},
doi = {10.5194/acp-20-8103-2020},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 13,
volume = 20,
place = {Germany},
year = {Mon Jul 13 00:00:00 EDT 2020},
month = {Mon Jul 13 00:00:00 EDT 2020}
}
https://doi.org/10.5194/acp-20-8103-2020
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- Petters, M. D.; Kreidenweis, S. M.
- Atmospheric Chemistry and Physics, Vol. 7, Issue 8
Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities
journal, January 2019
- Li, Ying; Shiraiwa, Manabu
- Atmospheric Chemistry and Physics, Vol. 19, Issue 9
Chamber-based insights into the factors controlling epoxydiol (IEPOX) secondary organic aerosol (SOA) yield, composition, and volatility
journal, January 2019
- D'Ambro, Emma L.; Schobesberger, Siegfried; Gaston, Cassandra J.
- Atmospheric Chemistry and Physics, Vol. 19, Issue 17
Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates
journal, January 2015
- Xu, L.; Suresh, S.; Guo, H.
- Atmospheric Chemistry and Physics, Vol. 15, Issue 13
Isoprene Epoxydiols as Precursors to Secondary Organic Aerosol Formation: Acid-Catalyzed Reactive Uptake Studies with Authentic Compounds
journal, November 2011
- Lin, Ying-Hsuan; Zhang, Zhenfa; Docherty, Kenneth S.
- Environmental Science & Technology, Vol. 46, Issue 1
Comparison of Approaches for Measuring and Predicting the Viscosity of Ternary Component Aerosol Particles
journal, February 2019
- Rovelli, Grazia; Song, Young-Chul; Maclean, Adrian M.
- Analytical Chemistry, Vol. 91, Issue 8
Synthesis of the Southeast Atmosphere Studies: Investigating Fundamental Atmospheric Chemistry Questions
journal, March 2018
- Carlton, Annmarie G.; de Gouw, Joost; Jimenez, Jose L.
- Bulletin of the American Meteorological Society, Vol. 99, Issue 3
Lability of secondary organic particulate matter
journal, October 2016
- Liu, Pengfei; Li, Yong Jie; Wang, Yan
- Proceedings of the National Academy of Sciences, Vol. 113, Issue 45
Direct measurements of semi-volatile organic compound dynamics show near-unity mass accommodation coefficients for diverse aerosols
journal, August 2019
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- Communications Chemistry, Vol. 2, Issue 1
Molecular and physical characteristics of aerosol at a remote free troposphere site: implications for atmospheric aging
journal, January 2018
- Schum, Simeon K.; Zhang, Bo; Džepina, Katja
- Atmospheric Chemistry and Physics, Vol. 18, Issue 19
Molecular chemistry of organic aerosols through the application of high resolution mass spectrometry
journal, January 2011
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Volatility of organic aerosol and its components in the megacity of Paris
journal, January 2016
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- Atmospheric Chemistry and Physics, Vol. 16, Issue 4
Methods to extract molecular and bulk chemical information from series of complex mass spectra with limited mass resolution
journal, October 2015
- Stark, Harald; Yatavelli, Reddy L. N.; Thompson, Samantha L.
- International Journal of Mass Spectrometry, Vol. 389
Integrating phase and composition of secondary organic aerosol from the ozonolysis of -pinene
journal, May 2014
- Kidd, C.; Perraud, V.; Wingen, L. M.
- Proceedings of the National Academy of Sciences, Vol. 111, Issue 21
Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations
journal, January 2009
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- Atmospheric Chemistry and Physics, Vol. 9, Issue 24
Kinetically controlled glass transition measurement of organic aerosol thin films using broadband dielectric spectroscopy
journal, January 2018
- Zhang, Yue; Katira, Shachi; Lee, Andrew
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Direct Measurements of Gas/Particle Partitioning and Mass Accommodation Coefficients in Environmental Chambers
journal, September 2017
- Krechmer, Jordan E.; Day, Douglas A.; Ziemann, Paul J.
- Environmental Science & Technology, Vol. 51, Issue 20