Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors
Abstract
Information on liquid–liquid phase separation (LLPS) and viscosity (or diffusion) within secondary organic aerosol (SOA) is needed to improve predictions of particle size, mass, reactivity, and cloud nucleating properties in the atmosphere. Here we report on LLPS and viscosities within SOA generated by the photooxidation of diesel fuel vapors. Diesel fuel contains a wide range of volatile organic compounds, and SOA generated by the photooxidation of diesel fuel vapors may be a good proxy for SOA from anthropogenic emissions. In our experiments, LLPS occurred over the relative humidity (RH) range of ~70 % to ~100 %, resulting in an organic-rich outer phase and a water-rich inner phase. These results may have implications for predicting the cloud nucleating properties of anthropogenic SOA since the presence of an organic-rich outer phase at high-RH values can lower the supersaturation with respect to water required for cloud droplet formation. At ≤10 % RH, the viscosity was ≥1×108 Pa s, which corresponds to roughly the viscosity of tar pitch. At 38 %–50 % RH, the viscosity was in the range of 1×108 to 3×105 Pa s. These measured viscosities are consistent with predictions based on oxygen to carbon elemental ratio (O:C) and molar mass asmore »
- Authors:
- Publication Date:
- Research Org.:
- Univ. of California, Irvine, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1571302
- Alternate Identifier(s):
- OSTI ID: 1803373
- Grant/Contract Number:
- SC0018349
- Resource Type:
- Published Article
- Journal Name:
- Atmospheric Chemistry and Physics (Online)
- Additional Journal Information:
- Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 19 Journal Issue: 19; Journal ID: ISSN 1680-7324
- Publisher:
- Copernicus Publications, EGU
- Country of Publication:
- Germany
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Song, Mijung, Maclean, Adrian M., Huang, Yuanzhou, Smith, Natalie R., Blair, Sandra L., Laskin, Julia, Laskin, Alexander, DeRieux, Wing-Sy Wong, Li, Ying, Shiraiwa, Manabu, Nizkorodov, Sergey A., and Bertram, Allan K. Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors. Germany: N. p., 2019.
Web. doi:10.5194/acp-19-12515-2019.
Song, Mijung, Maclean, Adrian M., Huang, Yuanzhou, Smith, Natalie R., Blair, Sandra L., Laskin, Julia, Laskin, Alexander, DeRieux, Wing-Sy Wong, Li, Ying, Shiraiwa, Manabu, Nizkorodov, Sergey A., & Bertram, Allan K. Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors. Germany. https://doi.org/10.5194/acp-19-12515-2019
Song, Mijung, Maclean, Adrian M., Huang, Yuanzhou, Smith, Natalie R., Blair, Sandra L., Laskin, Julia, Laskin, Alexander, DeRieux, Wing-Sy Wong, Li, Ying, Shiraiwa, Manabu, Nizkorodov, Sergey A., and Bertram, Allan K. Tue .
"Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors". Germany. https://doi.org/10.5194/acp-19-12515-2019.
@article{osti_1571302,
title = {Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors},
author = {Song, Mijung and Maclean, Adrian M. and Huang, Yuanzhou and Smith, Natalie R. and Blair, Sandra L. and Laskin, Julia and Laskin, Alexander and DeRieux, Wing-Sy Wong and Li, Ying and Shiraiwa, Manabu and Nizkorodov, Sergey A. and Bertram, Allan K.},
abstractNote = {Information on liquid–liquid phase separation (LLPS) and viscosity (or diffusion) within secondary organic aerosol (SOA) is needed to improve predictions of particle size, mass, reactivity, and cloud nucleating properties in the atmosphere. Here we report on LLPS and viscosities within SOA generated by the photooxidation of diesel fuel vapors. Diesel fuel contains a wide range of volatile organic compounds, and SOA generated by the photooxidation of diesel fuel vapors may be a good proxy for SOA from anthropogenic emissions. In our experiments, LLPS occurred over the relative humidity (RH) range of ~70 % to ~100 %, resulting in an organic-rich outer phase and a water-rich inner phase. These results may have implications for predicting the cloud nucleating properties of anthropogenic SOA since the presence of an organic-rich outer phase at high-RH values can lower the supersaturation with respect to water required for cloud droplet formation. At ≤10 % RH, the viscosity was ≥1×108 Pa s, which corresponds to roughly the viscosity of tar pitch. At 38 %–50 % RH, the viscosity was in the range of 1×108 to 3×105 Pa s. These measured viscosities are consistent with predictions based on oxygen to carbon elemental ratio (O:C) and molar mass as well as predictions based on the number of carbon, hydrogen, and oxygen atoms. Based on the measured viscosities and the Stokes–Einstein relation, at ≤10 % RH diffusion coefficients of organics within diesel fuel SOA is ≤5.4×10-17 cm2 s-1 and the mixing time of organics within 200 nm diesel fuel SOA particles (τmixing) is 50 h. These small diffusion coefficients and large mixing times may be important in laboratory experiments, where SOA is often generated and studied using low-RH conditions and on timescales of minutes to hours. At 38 %–50 % RH, the calculated organic diffusion coefficients are in the range of 5.4×10-17 to 1.8×10-13 cm2 s-1 and calculated τmixing values are in the range of ~0.01 h to ~50 h. These values provide important constraints for the physicochemical properties of anthropogenic SOA.},
doi = {10.5194/acp-19-12515-2019},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 19,
volume = 19,
place = {Germany},
year = {Tue Oct 08 00:00:00 EDT 2019},
month = {Tue Oct 08 00:00:00 EDT 2019}
}
https://doi.org/10.5194/acp-19-12515-2019
Web of Science
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- Journal of the American Chemical Society, Vol. 135, Issue 43
Relative humidity-dependent viscosities of isoprene-derived secondary organic material and atmospheric implications for isoprene-dominant forests
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- Song, M.; Liu, P. F.; Hanna, S. J.
- Atmospheric Chemistry and Physics, Vol. 15, Issue 9
Diffusion coefficients of organic molecules in sucrose–water solutions and comparison with Stokes–Einstein predictions
journal, January 2017
- Chenyakin, Yuri; Ullmann, Dagny A.; Evoy, Erin
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Mixing times of organic molecules within secondary organic aerosol particles: a global planetary boundary layer perspective
journal, January 2017
- Maclean, Adrian M.; Butenhoff, Christopher L.; Grayson, James W.
- Atmospheric Chemistry and Physics, Vol. 17, Issue 21
Hygroscopic Influence on the Semisolid-to-Liquid Transition of Secondary Organic Materials
journal, November 2014
- Bateman, Adam P.; Bertram, Allan K.; Martin, Scot T.
- The Journal of Physical Chemistry A, Vol. 119, Issue 19
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity
journal, January 2007
- Petters, M. D.; Kreidenweis, S. M.
- Atmospheric Chemistry and Physics, Vol. 7, Issue 8
Combined Determination of the Chemical Composition and of Health Effects of Secondary Organic Aerosols: The POLYSOA Project
journal, February 2008
- Baltensperger, Urs; Dommen, Josef; Alfarra, M. Rami
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Diffusivity measurements of volatile organics in levitated viscous aerosol particles
journal, January 2017
- Bastelberger, Sandra; Krieger, Ulrich K.; Luo, Beiping
- Atmospheric Chemistry and Physics, Vol. 17, Issue 13
Relationship between aerosol oxidation level and hygroscopic properties of laboratory generated secondary organic aerosol (SOA) particles: HYGROSCOPICITY OF LABORATORY SOA
journal, December 2010
- Massoli, P.; Lambe, A. T.; Ahern, A. T.
- Geophysical Research Letters, Vol. 37, Issue 24
Phase Changes during Hygroscopic Cycles of Mixed Organic/Inorganic Model Systems of Tropospheric Aerosols
journal, February 2006
- Marcolli, Claudia; Krieger, Ulrich K.
- The Journal of Physical Chemistry A, Vol. 110, Issue 5
Eddy covariance flux measurements of pollutant gases in urban Mexico City
journal, January 2009
- Velasco, E.; Pressley, S.; Grivicke, R.
- Atmospheric Chemistry and Physics, Vol. 9, Issue 19
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
Diffusion and reactivity in ultraviscous aerosol and the correlation with particle viscosity
journal, January 2016
- Marshall, Frances H.; Miles, Rachael E. H.; Song, Young-Chul
- Chemical Science, Vol. 7, Issue 2
An overview of the Amazonian Aerosol Characterization Experiment 2008 (AMAZE-08)
journal, January 2010
- Martin, S. T.; Andreae, M. O.; Althausen, D.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 23
Simulation and analysis of secondary organic aerosol dynamics in the South Coast Air Basin of California: SOA DYNAMICS IN SOUTHERN CALIFORNIA
journal, May 2006
- Vutukuru, Satish; Griffin, Robert J.; Dabdub, Donald
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Modeling the effect of non-ideality, dynamic mass transfer and viscosity on SOA formation in a 3-D air quality model
journal, January 2019
- Kim, Youngseob; Sartelet, Karine; Couvidat, Florian
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