Preprints
https://doi.org/10.5194/acp-2021-836
https://doi.org/10.5194/acp-2021-836

  25 Oct 2021

25 Oct 2021

Review status: this preprint is currently under review for the journal ACP.

A predictive viscosity model for aqueous electrolytes and mixed organic-inorganic aerosol phases

Joseph Lilek and Andreas Zuend Joseph Lilek and Andreas Zuend
  • Department of Atmospheric and Oceanic Sciences, McGill University, Montréal, Quebec, Canada

Abstract. Aerosol viscosity is determined by mixture composition and temperature, with a key influence from relative humidity (RH) in modulating aerosol water content. Aerosol particles frequently contain mixtures of water, organic compounds and inorganic ions, so we have extended the thermodynamics-based group-contribution model AIOMFAC-VISC to predict viscosity for aqueous electrolyte solutions and aqueous organic-inorganic mixtures. For aqueous electrolyte solutions, our new, semi-empirical approach uses a physical expression based on Eyring's absolute rate theory, and we define activation energy for viscous flow as a function of temperature, ion activities, and ionic strength. The AIOMFAC-VISC electrolyte model's ion-specific expressions were simultaneously fitted, which arguably makes this approach more predictive than that of other models. This also enables viscosity calculations for aqueous solutions containing an arbitrary number of cation and anion species, including mixtures that have never been studied experimentally. These predictions achieve an excellent level of accuracy while also providing physically meaningful extrapolations to extremely high electrolyte concentrations, which is essential in the context of microscopic aqueous atmospheric aerosols. For organic-inorganic mixtures, multiple mixing approaches were tested to couple the AIOMFAC-VISC electrolyte model with its existing aqueous organic model. We discuss the best performing mixing models implemented in AIOMFAC-VISC for reproducing viscosity measurements of aerosol surrogate systems. We present advantages and drawbacks of different model design choices and associated computational costs of these methods, of importance for use of AIOMFAC-VISC in dynamic simulations. Finally, we demonstrate the capabilities of AIOMFAC-VISC predictions for phase-separated organic-inorganic particles equilibrated to observed temperature and relative humidity conditions from atmospheric balloon soundings. The predictions for the studied cases suggest liquid-like viscosities for an aqueous electrolyte-rich particle phase throughout the troposphere, yet a highly viscous or glassy organic-rich phase in the middle and upper troposphere.

Joseph Lilek and Andreas Zuend

Status: open (until 06 Dec 2021)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-836', Anonymous Referee #1, 15 Nov 2021 reply
  • RC2: 'Comment on acp-2021-836', Anonymous Referee #2, 17 Nov 2021 reply
  • RC3: 'Comment on acp-2021-836', Anonymous Referee #3, 17 Nov 2021 reply

Joseph Lilek and Andreas Zuend

Joseph Lilek and Andreas Zuend

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Short summary
Depending on temperature and chemical makeup, certain aerosols can be highly viscous or glassy, with atmospheric implications. Here, we implement two major upgrades to the viscosity prediction model AIOMFAC-VISC. First, we created a new viscosity model for aqueous electrolyte solutions containing an arbitrary number of ion species. Second, we integrated the electrolyte model within the existing AIOMFAC-VISC framework to enable viscosity predictions for organic-inorganic mixtures.
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