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Title: 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 » 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.« less

Authors:
; ; ; ORCiD logo; ORCiD logo; ; ORCiD logo; ; ; ; ORCiD logo; ORCiD logo
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.
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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
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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.
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@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}
}
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Observations and implications of liquid–liquid phase separation at high relative humidities in secondary organic material produced by α -pinene ozonolysis without inorganic salts
journal, January 2016

  • Renbaum-Wolff, Lindsay; Song, Mijung; Marcolli, Claudia
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 12
  • DOI: 10.5194/acp-16-7969-2016

Mixing of secondary organic aerosols versus relative humidity
journal, October 2016

  • Ye, Qing; Robinson, Ellis Shipley; Ding, Xiang
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 45
  • DOI: 10.1073/pnas.1604536113

Chemical Reactivity and Liquid/Nonliquid States of Secondary Organic Material
journal, October 2015

  • Li, Yong Jie; Liu, Pengfei; Gong, Zhaoheng
  • Environmental Science & Technology, Vol. 49, Issue 22
  • DOI: 10.1021/acs.est.5b03392

Secondary Organic Aerosol Formation from Photo-Oxidation of Unburned Fuel: Experimental Results and Implications for Aerosol Formation from Combustion Emissions
journal, November 2013

  • Jathar, Shantanu H.; Miracolo, Marissa A.; Tkacik, Daniel S.
  • Environmental Science & Technology, Vol. 47, Issue 22
  • DOI: 10.1021/es403445q

Humidity-dependent phase state of SOA particles from biogenic and anthropogenic precursors
journal, January 2012

  • Saukko, E.; Lambe, A. T.; Massoli, P.
  • Atmospheric Chemistry and Physics, Vol. 12, Issue 16
  • DOI: 10.5194/acp-12-7517-2012

Surface tension prevails over solute effect in organic-influenced cloud droplet activation
journal, June 2017

  • Ovadnevaite, Jurgita; Zuend, Andreas; Laaksonen, Ari
  • Nature, Vol. 546, Issue 7660
  • DOI: 10.1038/nature22806

Glass-Forming Properties of 3-Methylbutane-1,2,3-tricarboxylic Acid and Its Mixtures with Water and Pinonic Acid
journal, August 2014

  • Dette, Hans P.; Qi, Mian; Schröder, David C.
  • The Journal of Physical Chemistry A, Vol. 118, Issue 34
  • DOI: 10.1021/jp505910w

Influence of Functional Groups on the Viscosity of Organic Aerosol
journal, December 2016

  • Rothfuss, Nicholas E.; Petters, Markus D.
  • Environmental Science & Technology, Vol. 51, Issue 1
  • DOI: 10.1021/acs.est.6b04478

Viscosities, diffusion coefficients, and mixing times of intrinsic fluorescent organic molecules in brown limonene secondary organic aerosol and tests of the Stokes–Einstein equation
journal, January 2019

  • Ullmann, Dagny A.; Hinks, Mallory L.; Maclean, Adrian M.
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 3
  • DOI: 10.5194/acp-19-1491-2019

Molecular Characterization of Organosulfur Compounds in Biodiesel and Diesel Fuel Secondary Organic Aerosol
journal, December 2016

  • Blair, Sandra L.; MacMillan, Amanda C.; Drozd, Greg T.
  • Environmental Science & Technology, Vol. 51, Issue 1
  • DOI: 10.1021/acs.est.6b03304

Organic aerosol and global climate modelling: a review
journal, January 2005

  • Kanakidou, M.; Seinfeld, J. H.; Pandis, S. N.
  • Atmospheric Chemistry and Physics, Vol. 5, Issue 4
  • DOI: 10.5194/acp-5-1053-2005

Testing secondary organic aerosol models using smog chamber data for complex precursor mixtures: influence of precursor volatility and molecular structure
journal, January 2014

  • Jathar, S. H.; Donahue, N. M.; Adams, P. J.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 11
  • DOI: 10.5194/acp-14-5771-2014

Inhibition of efflorescence in mixed organic–inorganic particles at temperatures less than 250 K
journal, January 2010

  • Bodsworth, A.; Zobrist, B.; Bertram, A. K.
  • Physical Chemistry Chemical Physics, Vol. 12, Issue 38
  • DOI: 10.1039/c0cp00572j

Technical note: The role of evolving surface tension in the formation of cloud droplets
journal, January 2019

  • Davies, James F.; Zuend, Andreas; Wilson, Kevin R.
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 5
  • DOI: 10.5194/acp-19-2933-2019

Evolution of Organic Aerosols in the Atmosphere
journal, December 2009

Size Dependence of the Structure of Organic Aerosol
journal, October 2013

  • Veghte, Daniel P.; Altaf, Muhammad Bilal; Freedman, Miriam Arak
  • Journal of the American Chemical Society, Vol. 135, Issue 43
  • DOI: 10.1021/ja408903g

Relative humidity-dependent viscosities of isoprene-derived secondary organic material and atmospheric implications for isoprene-dominant forests
journal, January 2015

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
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 3
  • DOI: 10.5194/acp-17-2423-2017

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
  • DOI: 10.5194/acp-17-13037-2017

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
  • DOI: 10.1021/jp508521c

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
  • DOI: 10.5194/acp-7-1961-2007

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
  • Journal of Aerosol Medicine, Vol. 0, Issue 0
  • DOI: 10.1089/jam.2007.0655

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
  • DOI: 10.5194/acp-17-8453-2017

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
  • DOI: 10.1021/jp0556759

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
  • DOI: 10.5194/acp-9-7325-2009

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
  • DOI: 10.1073/pnas.1603138113

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
  • DOI: 10.1039/C5SC03223G

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
  • DOI: 10.5194/acp-10-11415-2010

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
  • Journal of Geophysical Research: Atmospheres, Vol. 111, Issue D10
  • DOI: 10.1029/2005JD006139

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
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 2
  • DOI: 10.5194/acp-19-1241-2019
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