Correlating the Viscosity and Rate of Water Diffusion in Semisolid Gel-Forming Aerosol Particles

Sheldon, Craig S.; Salazar, Jorge; Diaz, Teresa Palacios; Morton, Katie; Davis, Ryan D.; Davies, James F.

doi:10.1021/acsearthspacechem.3c00241

Title: Correlating the Viscosity and Rate of Water Diffusion in Semisolid Gel-Forming Aerosol Particles

Journal Article · 18 October 2023 · ACS Earth and Space Chemistry

DOI: https://doi.org/10.1021/acsearthspacechem.3c00241 · OSTI ID:2311328

Sheldon, Craig S. ^[1]; Salazar, Jorge ^[1]; Diaz, Teresa Palacios ^[2]; Morton, Katie ^[2];

^[3];

^[1]

Univ. of California, Riverside, CA (United States)
Trinity Univ., San Antonio, TX (United States)
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States)

Aerosol particles are known to exist in highly viscous amorphous states at a low relative humidity and temperature. The slow diffusion of molecules in viscous particles impacts the uptake and loss of volatile and semivolatile species and the rate of heterogeneous chemistry. Recent work has demonstrated that in particles containing organic molecules and salts, the formation of two-phase gel states is possible, leading to observations of rigid particles that resist coalescence. The way that molecules diffuse and transport in gel systems is not well-characterized. In this work, we use an electrodynamic balance to levitate sample particles containing a range of organic compounds in mixtures with calcium chloride and measure the rate of water diffusion. Particles of the pure organics have been shown to form viscous amorphous states, while in mixtures with divalent salts, coalescence measurements have revealed the apparent solidification of particles, consistent with the formation of a gel state facilitated by ion–molecule interactions. We report in several cases that water transport can actually be increased in the rigid gel state relative to the pure compound that forms a viscous state under similar conditions. These measurements reveal the limitations of using viscosity as a metric for predicting molecular diffusion and that the gel structure that forms is a much stronger controlling factor in the rate of diffusion. In conclusion, this underscores the need for diffusion measurements as well as a deeper understanding of noncovalent molecular assembly that leads to supramolecular structures in aerosol particles.

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Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)

Grant/Contract Number:: NA0003525

OSTI ID:: 2311328

Report Number(s):: SAND--2023-14358J

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 11 Vol. 7; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
water diffusion
particle phase
viscosity
gel formation
ion-molecule interactions
organic-inorganic mixtures

Title: Correlating the Viscosity and Rate of Water Diffusion in Semisolid Gel-Forming Aerosol Particles

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