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Title: Size-Dependent Liquid–Liquid Phase Separation in Atmospherically Relevant Complex Systems

Abstract

Physical properties of aerosol particles, such as liquid-liquid phase separation (LLPS), have the potential to impact the climate system. Model systems have been shown to have size-dependent LLPS in the submicron regime, yet, these systems are an extreme simplification of ambient aerosol, which can include myriad organic compounds. In our research, we expand the studies of LLPS in particles consisting of ammonium sulfate and more complex organic mixtures from multiple organic compounds to α-pinene secondary organic matter (SOM). All systems display a size-dependent morphology, with small particles remaining homogeneous while large particles phase separate. Surprisingly, three-phase particles were also observed in some of the systems in addition to a new phase state that we have termed channel morphology, which can arise upon efflorescence. The existence of size-dependent LLPS in complex organic mixtures and SOM provides evidence that this is a relevant phenomenon for ambient aerosol and should be considered when modeling atmospheric aerosol.

Authors:
 [1];  [1]; ORCiD logo [1]
  1. Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1604445
Grant/Contract Number:  
SC0018032
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 21; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kucinski, Theresa M., Dawson, Joseph Nelson, and Freedman, Miriam Arak. Size-Dependent Liquid–Liquid Phase Separation in Atmospherically Relevant Complex Systems. United States: N. p., 2019. Web. doi:10.1021/acs.jpclett.9b02532.
Kucinski, Theresa M., Dawson, Joseph Nelson, & Freedman, Miriam Arak. Size-Dependent Liquid–Liquid Phase Separation in Atmospherically Relevant Complex Systems. United States. https://doi.org/10.1021/acs.jpclett.9b02532
Kucinski, Theresa M., Dawson, Joseph Nelson, and Freedman, Miriam Arak. Tue . "Size-Dependent Liquid–Liquid Phase Separation in Atmospherically Relevant Complex Systems". United States. https://doi.org/10.1021/acs.jpclett.9b02532. https://www.osti.gov/servlets/purl/1604445.
@article{osti_1604445,
title = {Size-Dependent Liquid–Liquid Phase Separation in Atmospherically Relevant Complex Systems},
author = {Kucinski, Theresa M. and Dawson, Joseph Nelson and Freedman, Miriam Arak},
abstractNote = {Physical properties of aerosol particles, such as liquid-liquid phase separation (LLPS), have the potential to impact the climate system. Model systems have been shown to have size-dependent LLPS in the submicron regime, yet, these systems are an extreme simplification of ambient aerosol, which can include myriad organic compounds. In our research, we expand the studies of LLPS in particles consisting of ammonium sulfate and more complex organic mixtures from multiple organic compounds to α-pinene secondary organic matter (SOM). All systems display a size-dependent morphology, with small particles remaining homogeneous while large particles phase separate. Surprisingly, three-phase particles were also observed in some of the systems in addition to a new phase state that we have termed channel morphology, which can arise upon efflorescence. The existence of size-dependent LLPS in complex organic mixtures and SOM provides evidence that this is a relevant phenomenon for ambient aerosol and should be considered when modeling atmospheric aerosol.},
doi = {10.1021/acs.jpclett.9b02532},
journal = {Journal of Physical Chemistry Letters},
number = 21,
volume = 10,
place = {United States},
year = {2019},
month = {10}
}

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Cited by: 29 works
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Figures / Tables:

Figure 1 Figure 1: Particle morphology for submicron particles observed using cryo-transmission electron microscopy (cryo-TEM) for dry particles composed of 60:40 ammonium sulfate/complex organic mixture-succinic acid (COM-SA) and 80:20 ammonium sulfate/$α$-pinene secondary organic matter (SOM). Smaller particles are homogeneous (a & c) whereas larger particles phase separate (b & d). A fastmore » drying rate, at ~99.7% RH/s, was used. The white outline is due to under focusing the electron beam to have optimal contrast to see the phase state. Black line indicates scale bar for each particle.« less

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