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Title: Liquid–liquid phase separation in particles containing secondary organic material free of inorganic salts

Abstract

Particles containing secondary organic material (SOM) are ubiquitous in the atmosphere and play a role in climate and air quality. Recently, research has shown that liquid–liquid phase separation (LLPS) occurs at high relative humidity (RH) (greater than ~95 %) in α-pinene-derived SOM particles free of inorganic salts, while LLPS does not occur in isoprene-derived SOM particles free of inorganic salts. We expand on these findings by investigating LLPS at 290 ± 1 K in SOM particles free of inorganic salts produced from ozonolysis of β-caryophyllene, ozonolysis of limonene, and photo-oxidation of toluene. LLPS was observed at greater than ~95 % RH in the biogenic SOM particles derived from β-caryophyllene and limonene while LLPS was not observed in the anthropogenic SOM particles derived from toluene. This work combined with the earlier work on LLPS in SOM particles free of inorganic salts suggests that the occurrence of LLPS in SOM particles free of inorganic salts is related to the oxygen-to-carbon elemental ratio (O : C) of the organic material. These results help explain the difference between the hygroscopic parameter κ of SOM particles measured above and below water saturation in the laboratory and field, and have implications for predicting the cloud condensationmore » nucleation properties of SOM particles.« less

Authors:
 [1]; ORCiD logo [2];  [3]; ORCiD logo [4]
  1. Chonbuk National Univ., Jeollabuk-do (Korea, Republic of). Dept. of Earth and Environmental Sciences; Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Chemistry
  2. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences
  3. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences; Harvard Univ., Cambridge, MA (United States). Dept. of Earth and Planetary Sciences
  4. Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Chemistry
Publication Date:
Research Org.:
Harvard Univ., Cambridge, MA (United States)
Sponsoring Org.:
USDOE; Natural Sciences and Engineering Research Council of Canada (NSERC); National Science Foundation (NSF); National Research Foundation of Korea (NRF)
OSTI Identifier:
1425661
Grant/Contract Number:  
SC0012792
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Volume: 17; Journal Issue: 18; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Song, Mijung, Liu, Pengfei, Martin, Scot T., and Bertram, Allan K. Liquid–liquid phase separation in particles containing secondary organic material free of inorganic salts. United States: N. p., 2017. Web. doi:10.5194/acp-17-11261-2017.
Song, Mijung, Liu, Pengfei, Martin, Scot T., & Bertram, Allan K. Liquid–liquid phase separation in particles containing secondary organic material free of inorganic salts. United States. https://doi.org/10.5194/acp-17-11261-2017
Song, Mijung, Liu, Pengfei, Martin, Scot T., and Bertram, Allan K. 2017. "Liquid–liquid phase separation in particles containing secondary organic material free of inorganic salts". United States. https://doi.org/10.5194/acp-17-11261-2017. https://www.osti.gov/servlets/purl/1425661.
@article{osti_1425661,
title = {Liquid–liquid phase separation in particles containing secondary organic material free of inorganic salts},
author = {Song, Mijung and Liu, Pengfei and Martin, Scot T. and Bertram, Allan K.},
abstractNote = {Particles containing secondary organic material (SOM) are ubiquitous in the atmosphere and play a role in climate and air quality. Recently, research has shown that liquid–liquid phase separation (LLPS) occurs at high relative humidity (RH) (greater than ~95 %) in α-pinene-derived SOM particles free of inorganic salts, while LLPS does not occur in isoprene-derived SOM particles free of inorganic salts. We expand on these findings by investigating LLPS at 290 ± 1 K in SOM particles free of inorganic salts produced from ozonolysis of β-caryophyllene, ozonolysis of limonene, and photo-oxidation of toluene. LLPS was observed at greater than ~95 % RH in the biogenic SOM particles derived from β-caryophyllene and limonene while LLPS was not observed in the anthropogenic SOM particles derived from toluene. This work combined with the earlier work on LLPS in SOM particles free of inorganic salts suggests that the occurrence of LLPS in SOM particles free of inorganic salts is related to the oxygen-to-carbon elemental ratio (O : C) of the organic material. These results help explain the difference between the hygroscopic parameter κ of SOM particles measured above and below water saturation in the laboratory and field, and have implications for predicting the cloud condensation nucleation properties of SOM particles.},
doi = {10.5194/acp-17-11261-2017},
url = {https://www.osti.gov/biblio/1425661}, journal = {Atmospheric Chemistry and Physics (Online)},
issn = {1680-7324},
number = 18,
volume = 17,
place = {United States},
year = {Mon Sep 25 00:00:00 EDT 2017},
month = {Mon Sep 25 00:00:00 EDT 2017}
}

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Cited by: 38 works
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Works referencing / citing this record:

Multiphase reactivity of polycyclic aromatic hydrocarbons is driven by phase separation and diffusion limitations
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Liquid–liquid phase separation in organic particles containing one and two organic species: importance of the average O : C
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A review of experimental techniques for aerosol hygroscopicity studies
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Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter
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Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors
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A review of experimental techniques for aerosol hygroscopicity studies
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