4.6 Article

Dynamics of Liquid-Liquid Phase Separation in Submicrometer Aerosol

Journal

JOURNAL OF PHYSICAL CHEMISTRY A
Volume 125, Issue 20, Pages 4446-4453

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.1c01985

Keywords

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Funding

  1. U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division [DE-SC0018032]

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Nanoscale materials exhibit unique properties compared to their bulk counterparts, with submicrometer particles showing shifts in phase transitions. Liquid-liquid phase separation (LLPS) has broad applications and is commonly observed in atmospheric aerosol particles. The lower SRH for submicrometer aerosol particles compared to micrometer-sized droplets suggests that current estimates of phase-separated aerosols may be overestimated.
Nanoscale materials, when compared to their bulk components, possess unique properties. In particular, shifts in phase transitions can occur for submicrometer particles. For instance, small particles do not undergo the process of liquid-liquid phase separation (LLPS). LLPS has applications in emulsions such as Janus particles, controllable morphology to create drug-rich phases during drug delivery, and is often observed in atmospheric aqueous aerosol particles. In atmospheric particles, LLPS is tracked as a function of particle water activity, which is equivalent to the relative humidity (RH) at equilibrium. We probed three organic/inorganic aerosol systems in the range of RH over which phase separation occurs (SRH). Our findings indicate that SRH for submicrometer aerosol particles is lower than for micrometer-sized droplets. These findings show that it may be necessary to update the representation of phase transitions in aerosol particles in climate models. The vast majority of organic/inorganic aerosol particles have submicrometer diameters, and a decrease in SRH for submicrometer particles indicates that the current estimation of phase-separated aerosols may be overestimated. Furthermore, understanding the properties of LLPS at the nanoscale can provide key parameters to describe these systems and may lead to better control of phase separation in submicrometer particles.

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