Articles | Volume 22, issue 5
https://doi.org/10.5194/acp-22-3203-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-3203-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
A predictive viscosity model for aqueous electrolytes and mixed organic–inorganic aerosol phases
Joseph Lilek
Department of Atmospheric and Oceanic Sciences, McGill University, Montréal, Quebec, H3A 0B9, Canada
Department of Atmospheric and Oceanic Sciences, McGill University, Montréal, Quebec, H3A 0B9, Canada
Related authors
No articles found.
Dalrin Ampritta Amaladhasan, Dan Hassan-Barthaux, and Andreas Zuend
EGUsphere, https://doi.org/10.5194/egusphere-2025-4673, https://doi.org/10.5194/egusphere-2025-4673, 2026
Short summary
Short summary
A 2-dimensional polarity–volatility framework is introduced. It enables the automated characterization of thousands of organics and their systematic lumping into adjustable sets of surrogate components. A new polarity metric based on an activity coefficient ratio is presented for use in this framework. A related molecule substructure parsing tool for input file generation is introduced. This framework enables reduced-complexity representations of near-explicit organic aerosol systems.
Camilo Serrano Damha, Kyle Gorkowski, and Andreas Zuend
Atmos. Chem. Phys., 25, 5773–5792, https://doi.org/10.5194/acp-25-5773-2025, https://doi.org/10.5194/acp-25-5773-2025, 2025
Short summary
Short summary
We implemented the BAT-VBS (Binary Activity Thermodynamics volatility basis set) aerosol thermodynamics model in the GEOS-Chem chemical transport model to efficiently account for organic aerosol water uptake, nonideal mixing, and impacts on the gas–particle partitioning of semi-volatile organics. Compared to GEOS-Chem's complex (dry) scheme, we show that the BAT-VBS model can predict substantial enhancements in organic aerosol mass concentration at moderate-to-high relative humidity.
Ryan Schmedding and Andreas Zuend
Atmos. Chem. Phys., 25, 327–346, https://doi.org/10.5194/acp-25-327-2025, https://doi.org/10.5194/acp-25-327-2025, 2025
Short summary
Short summary
Four different approaches for computing the interfacial tension between liquid phases in aerosol particles were tested for particles with diameters from 10 nm to more than 5 μm. Antonov's rule led to the strongest reductions in the onset relative humidity of liquid–liquid phase separation and reproduced measured interfacial tensions for highly immiscible systems. A modified form of the Butler equation was able to best reproduce measured interfacial tensions in more miscible systems.
Liviana K. Klein, Allan K. Bertram, Andreas Zuend, Florence Gregson, and Ulrich K. Krieger
Atmos. Chem. Phys., 24, 13341–13359, https://doi.org/10.5194/acp-24-13341-2024, https://doi.org/10.5194/acp-24-13341-2024, 2024
Short summary
Short summary
The viscosity of ammonium nitrate–sucrose–H2O was quantified with three methods ranging from liquid to solid state depending on the relative humidity. Moreover, the corresponding estimated internal aerosol mixing times remained below 1 h for most tropospheric conditions, making equilibrium partitioning a reasonable assumption.
Ryan Schmedding and Andreas Zuend
Atmos. Chem. Phys., 23, 7741–7765, https://doi.org/10.5194/acp-23-7741-2023, https://doi.org/10.5194/acp-23-7741-2023, 2023
Short summary
Short summary
Aerosol particles below 100 nm in diameter have high surface-area-to-volume ratios. The enrichment of compounds in the surface of an aerosol particle may lead to depletion of that species in the interior bulk of the particle. We present a framework for modeling the equilibrium bulk–surface partitioning of mixed organic–inorganic particles, including cases of co-condensation of semivolatile organic compounds and species with extremely limited solubility in the bulk or surface of a particle.
Rani Jeong, Joseph Lilek, Andreas Zuend, Rongshuang Xu, Man Nin Chan, Dohyun Kim, Hi Gyu Moon, and Mijung Song
Atmos. Chem. Phys., 22, 8805–8817, https://doi.org/10.5194/acp-22-8805-2022, https://doi.org/10.5194/acp-22-8805-2022, 2022
Short summary
Short summary
In this study, the viscosities of particles of sucrose–H2O, AS–H2O, and sucrose–AS–H2O for OIRs of 4:1, 1:1, and 1:4 for decreasing RH, were quantified by poke-and-flow and bead-mobility techniques at 293 ± 1 K. Based on the viscosity results, the particles of binary and ternary systems ranged from liquid to semisolid, and even the solid state depending on the RH. Moreover, we compared the measured viscosities of ternary systems to the predicted viscosities with excellent agreement.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, https://doi.org/10.5194/acp-22-973-2022, 2022
Short summary
Short summary
Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
Short summary
Short summary
We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Young-Chul Song, Joseph Lilek, Jae Bong Lee, Man Nin Chan, Zhijun Wu, Andreas Zuend, and Mijung Song
Atmos. Chem. Phys., 21, 10215–10228, https://doi.org/10.5194/acp-21-10215-2021, https://doi.org/10.5194/acp-21-10215-2021, 2021
Short summary
Short summary
We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts/ H2O, over the atmospheric relative humidity (RH) range. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K.
Cited articles
Abdulagatov, I. M., Zeinalova, A. A., and Azizov, N. D.: Viscosity of the Aqueous Ca(NO3)2 Solutions at Temperatures from 298 to 573 K and at Pressures up to 40 MPa, J. Chem. Eng. Data, 49, 1444–1450, https://doi.org/10.1021/je049853n, 2004. a
Abrams, D. S. and Prausnitz, J. M.: Statistical thermodynamics of liquid mixtures: A new expression for the excess Gibbs energy of partly or completely miscible systems, AIChE J., 21, 116–128, https://doi.org/10.1002/aic.690210115, 1975. a
Ahn, K.-H., Kim, S.-M., Jung, H.-J., Lee, M.-J., Eom, H.-J., Maskey, S., and Ro, C.-U.: Combined Use of Optical and Electron Microscopic Techniques for the Measurement of Hygroscopic Property, Chemical Composition, and Morphology of Individual Aerosol Particles, Anal. Chem., 82, 7999–8009, https://doi.org/10.1021/ac101432y, 2010. a
Bajić, D. M., Šerbanović, S. P., Živković, E. M., Jovanović, J., and Kijevčanin, M. L.: Prediction and correlation of viscosity of binary mixtures of ionic liquids with organic solvents, J. Mol. Liq., 197, 1–6, https://doi.org/10.1016/j.molliq.2014.04.005, 2014. a
Baldelli, A., Power, R. M., Miles, R. E. H., Reid, J. P., and Vehring, R.: Effect of crystallization kinetics on the properties of spray dried microparticles, Aerosol Sci. Tech., 50, 693–704, https://doi.org/10.1080/02786826.2016.1177163, 2016. a, b, c, d
Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A., Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: Predicting the relative humidities of liquid-liquid phase separation, efflorescence, and deliquescence of mixed particles of ammonium sulfate, organic material, and water using the organic-to-sulfate mass ratio of the particle and the oxygen-to-carbon elemental ratio of the organic component, Atmos. Chem. Phys., 11, 10995–11006, https://doi.org/10.5194/acp-11-10995-2011, 2011. a, b
Boender, C. G. E., Rinnooy Kan, A. H. G., Timmer, G. T., and Stougie, L.: A stochastic method for global optimization, Math. Program., 22, 125–140, https://doi.org/10.1007/BF01581033, 1982. a
Cai, C., Tan, S., Chen, H., Ma, J., Wang, Y., Reid, J. P., and Zhang, Y.: Slow water transport in MgSO4 aerosol droplets at gel-forming relative humidities, Phys. Chem. Chem. Phys., 17, 29753–29763, https://doi.org/10.1039/C5CP05181A, 2015. a, b
Charnawskas, J. C., Alpert, P. A., Lambe, A. T., Berkemeier, T., O'Brien, R. E., Massoli, P., Onasch, T. B., Shiraiwa, M., Moffet, R. C., Gilles, M. K., Davidovits, P., Worsnop, D. R., and Knopf, D. A.: Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation, Faraday Discuss., 200, 165–194, https://doi.org/10.1039/C7FD00010C, 2017. a, b
Ciobanu, V. G., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Efflorescence of Ammonium Sulfate and Coated Ammonium Sulfate Particles: Evidence for Surface Nucleation, J. Phys. Chem. A, 114, 9486–9495, https://doi.org/10.1021/jp103541w, 2010. a
Cox, W. M., Wolfenden, J. H., and Hartley, H. B.: The viscosity of strong electrolytes measured by a differential method, P. R. Soc. Lond. A-Conta., 145, 475–488, https://doi.org/10.1098/rspa.1934.0113, 1934. a
Csendes, T.: Nonlinear parameter estimation by global optimization-efficiency and reliability, Acta Cybernetica, 8, 361–370, 1988. a
Dehaoui, A., Issenmann, B., and Caupin, F.: Viscosity of deeply supercooled water and its coupling to molecular diffusion, P. Natl. Acad. Sci. USA, 112, 12020–12025, https://doi.org/10.1073/pnas.1508996112, 2015. a
Esteves, M. J. C., Cardoso, M. J. E. d. M., and Barcia, O. E.: A Debye–Hückel Model for Calculating the Viscosity of Binary Strong Electrolyte Solutions, Ind. Eng. Chem. Res., 40, 5021–5028, https://doi.org/10.1021/ie010392y, 2001. a
Evoy, E., Maclean, A. M., Rovelli, G., Li, Y., Tsimpidi, A. P., Karydis, V. A., Kamal, S., Lelieveld, J., Shiraiwa, M., Reid, J. P., and Bertram, A. K.: Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes–Einstein and fractional Stokes–Einstein relations, Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, 2019. a
Fabuss, B. M., Korosi, A., and Othmer, D. F.: Viscosities of aqueous solutions of several electrolytes present in sea water, J. Chem. Eng. Data, 14, 192–197, https://doi.org/10.1021/je60041a025, 1969. a, b
Fard, M. M., Krieger, U. K., and Peter, T.: Kinetic Limitation to Inorganic Ion Diffusivity and to Coalescence of Inorganic Inclusions in Viscous Liquid–Liquid Phase-Separated Particles, J. Phys. Chem. A, 121, 9284–9296, https://doi.org/10.1021/acs.jpca.7b05242, 2017. a
Fredenslund, A., Jones, R. L., and Prausnitz, J. M.: Group-contribution estimation of activity coefficients in nonideal liquid mixtures, AIChE J., 21, 1086–1099, https://doi.org/10.1002/aic.690210607, 1975. a
Fu, H., Zhang, M., Li, W., Chen, J., Wang, L., Quan, X., and Wang, W.: Morphology, composition and mixing state of individual carbonaceous aerosol in urban Shanghai, Atmos. Chem. Phys., 12, 693–707, https://doi.org/10.5194/acp-12-693-2012, 2012. a
Glasstone, S., Laidler, K., and Eyring, H.: The theory of rate processes: the kinetics of chemical reactions, viscosity, diffusion and electrochemical phenomena, McGraw-Hill, 1st edn., ISBN-13 9780070233607, 1941. a
Goldsack, D. E. and Franchetto, A. A.: The viscosity of concentrated electrolyte solutions–III. A mixture law, Electrochim. Acta, 22, 1287–1294, https://doi.org/10.1016/0013-4686(77)87012-6, 1977a. a, b
Goldsack, D. E. and Franchetto, R.: The viscosity of concentrated electrolyte solutions. I. Concentration dependence at fixed temperature, Can. J. Chem., 55, 1062–1072, https://doi.org/10.1139/v77-148, 1977b. a, b, c, d
Goldsack, D. E. and Franchetto, R. C.: The viscosity of concentrated electrolyte solutions. II. Temperature dependence, Can. J. Chem., 56, 1442–1450, https://doi.org/10.1139/v78-236, 1978. a
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009. a
Heald, C. L. and Kroll, J. H.: The fuel of atmospheric chemistry: Toward a complete description of reactive organic carbon, Science Advances, 6, eaay8967, https://doi.org/10.1126/sciadv.aay8967, 2020. a
Hu, Y.-F. and Lee, H.: Prediction of viscosity of mixed electrolyte solutions based on the Eyring's absolute rate theory and the semi-ideal hydration model, Electrochim. Acta, 48, 1789–1796, https://doi.org/10.1016/S0013-4686(03)00226-3, 2003. a
Huang, Y., Mahrt, F., Xu, S., Shiraiwa, M., Zuend, A., and Bertram, A. K.: Coexistence of three liquid phases in individual atmospheric aerosol particles, P. Natl. Acad. Sci. USA, 118, e2102512118, https://doi.org/10.1073/pnas.2102512118, 2021. a
Iyoki, S., Iwasaki, S., Kuriyama, Y., and Uemura, T.: Densities, viscosities, and surface tensions for the two ternary systems water + lithium bromide + lithium iodide + lithium chloride + lithium nitrate, J. Chem. Eng. Data, 38, 302–305, https://doi.org/10.1021/je00010a031, 1993. a
Jacobson, M. Z.: Air pollution and global warming: history, science, and solutions, Cambridge University Press, ISBN-13 9780521010443, 2002. a
Jenkins, H. D. B. and Marcus, Y.: Viscosity B-Coefficients of Ions in Solution, Chem. Rev., 95, 2695–2724, https://doi.org/10.1021/cr00040a004, 1995. a
Jones, G. and Dole, M.: The viscosity of aqueous solutions of strong electrolytes with special reference to barium chloride, J. Am. Chem. Soc., 51, 2950–2964, https://doi.org/10.1021/ja01385a012, 1929. a
Kaminsky, M.: Untersuchungen über die Wechselwirkung Ion-Lösungsmittel, insbesondere auf Grund von Viskositätsmessungen, Z. Naturforsch. A, 12, 424–433, https://doi.org/10.1515/zna-1957-0511, 1957. a, b
Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere, Phys. Chem. Chem. Phys., 13, 19238–19255, https://doi.org/10.1039/C1CP22617G, 2011. a, b, c, d
Kumar, R., Saunders, R. W., Mahajan, A. S., Plane, J. M. C., and Murray, B. J.: Physical properties of iodate solutions and the deliquescence of crystalline I2O5 and HIO3, Atmos. Chem. Phys., 10, 12251–12260, https://doi.org/10.5194/acp-10-12251-2010, 2010. a
Laliberté, M.: A Model for Calculating the Heat Capacity of Aqueous Solutions, with Updated Density and Viscosity Data, J. Chem. Eng. Data, 54, 1725–1760, https://doi.org/10.1021/je8008123, 2009. a, b, c
Lencka, M. M., Anderko, A., Sanders, S. J., and Young, R. D.: Modeling Viscosity of Multicomponent Electrolyte Solutions, Int. J. Thermophys., 19, 367–378, https://doi.org/10.1023/A:1022501108317, 1998. a, b
Li, Y.-J., Liu, P.-F., Bergoend, C., Bateman, A. P., and Martin, S. T.: Rebounding hygroscopic inorganic aerosol particles: Liquids, gels, and hydrates, Aerosol Sci. Tech., 51, 388–396, https://doi.org/10.1080/02786826.2016.1263384, 2017. a, b, c
Marcus, Y.: Effect of ions on the structure of water: structure making and breaking, Chem. Rev., 109, 1346–1370, 2009. a
Miller, A.: Global optimization using the Boender-Timmer-Rinnoy Kan algorithm, https://www.mat.univie.ac.at/~neum/glopt/contrib/global.f90 (last access: 7 March 2022), 2003. a
Moré, J. J., Garbow, B. S., and Hillstrom, K. E.: User guide for MINPACK-1, Tech. rep., CM-P00068642, https://doi.org/10.2172/6997568, 1980. a
Moré, J. J., Sorensen, D. C., Hillstrom, K., and Garbow, B.: The MINPACK project, Sources and Development of Mathematical Software, 25, 88–111, 1984. a
Murray, B. J., Haddrell, A. E., Peppe, S., Davies, J. F., Reid, J. P., O'Sullivan, D., Price, H. C., Kumar, R., Saunders, R. W., Plane, J. M. C., Umo, N. S., and Wilson, T. W.: Glass formation and unusual hygroscopic growth of iodic acid solution droplets with relevance for iodine mediated particle formation in the marine boundary layer, Atmos. Chem. Phys., 12, 8575–8587, https://doi.org/10.5194/acp-12-8575-2012, 2012. a
Nishikata, E., Ishii, T., and Ohta, T.: Viscosities of aqueous hydrochloric acid solutions, and densities and viscosities of aqueous hydroiodic acid solutions, J. Chem. Eng. Data, 26, 254–256, https://doi.org/10.1021/je00025a008, 1981. a
Nowlan, M.-F., Doan, T. H., and Sangster, J.: Prediction of the viscosity of mixed electrolyte solutions from single-salt data, Can. J. Chem. Eng., 58, 637–642, https://doi.org/10.1002/cjce.5450580514, 1980. a
Power, R., Simpson, S., Reid, J., and Hudson, A.: The transition from liquid to solid-like behaviour in ultrahigh viscosity aerosol particles, Chem. Sci., 4, 2597–2604, 2013. a
Prather, K. A., Bertram, T. H., Grassian, V. H., Deane, G. B., Stokes, M. D., DeMott, P. J., Aluwihare, L. I., Palenik, B. P., Azam, F., Seinfeld, J. H., Moffet, R. C., Molina, M. J., Cappa, C. D., Geiger, F. M., Roberts, G. C., Russell, L. M., Ault, A. P., Baltrusaitis, J., Collins, D. B., Corrigan, C. E., Cuadra-Rodriguez, L. A., Ebben, C. J., Forestieri, S. D., Guasco, T. L., Hersey, S. P., Kim, M. J., Lambert, W. F., Modini, R. L., Mui, W., Pedler, B. E., Ruppel, M. J., Ryder, O. S., Schoepp, N. G., Sullivan, R. C., and Zhao, D.: Bringing the ocean into the laboratory to probe the chemical complexity of sea spray aerosol, P. Natl. Acad. Sci. USA, 110, 7550–7555, https://doi.org/10.1073/pnas.1300262110, 2013. a
Pye, H. O. T., Zuend, A., Fry, J. L., Isaacman-VanWertz, G., Capps, S. L., Appel, K. W., Foroutan, H., Xu, L., Ng, N. L., and Goldstein, A. H.: Coupling of organic and inorganic aerosol systems and the effect on gas–particle partitioning in the southeastern US, Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, 2018. a
Pye, H. O. T., Nenes, A., Alexander, B., Ault, A. P., Barth, M. C., Clegg, S. L., Collett Jr., J. L., Fahey, K. M., Hennigan, C. J., Herrmann, H., Kanakidou, M., Kelly, J. T., Ku, I.-T., McNeill, V. F., Riemer, N., Schaefer, T., Shi, G., Tilgner, A., Walker, J. T., Wang, T., Weber, R., Xing, J., Zaveri, R. A., and Zuend, A.: The acidity of atmospheric particles and clouds, Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, 2020. a
Reid, J. P., Bertram, A. K., Topping, D. O., Laskin, A., Martin, S. T., Petters, M. D., Pope, F. D., and Rovelli, G.: The viscosity of atmospherically relevant organic particles, Nat. Commun., 9, 956, https://doi.org/10.1038/s41467-018-03027-z, 2018. a, b, c
Richards, D. S., Trobaugh, K. L., Hajek-Herrera, J., and Davis, R. D.: Dual-Balance Electrodynamic Trap as a Microanalytical Tool for Identifying Gel Transitions and Viscous Properties of Levitated Aerosol Particles, Anal. Chem., 92, 3086–3094, https://doi.org/10.1021/acs.analchem.9b04487, 2020a. a, b, c, d, e
Richards, D. S., Trobaugh, K. L., Hajek-Herrera, J., Price, C. L., Sheldon, C. S., Davies, J. F., and Davis, R. D.: Ion-molecule interactions enable unexpected phase transitions in organic-inorganic aerosol, Science Advances, 6, eabb5643, https://doi.org/10.1126/sciadv.abb5643, 2020b. a, b, c, d, e, f, g
Roy, M. N., Jha, A., and Choudhury, A.: Densities, Viscosities and Adiabatic Compressibilities of Some Mineral Salts in Water at Different Temperatures, J. Chem. Eng. Data, 49, 291–296, https://doi.org/10.1021/je030205y, 2004. a
Shiraiwa, M. and Seinfeld, J. H.: Equilibration timescale of atmospheric secondary organic aerosol partitioning, Geophys. Res. Lett., 39, L24801, https://doi.org/10.1029/2012GL054008, 2012. a
Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gas–particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441, https://doi.org/10.1039/c3cp51595h, 2013. a
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Liquid-liquid phase separation in aerosol particles: Dependence on O:C, organic functionalities, and compositional complexity, Geophys. Res. Lett., 39, L19801, https://doi.org/10.1029/2012GL052807, 2012. a
Stokes, R. H. and Robinson, R. A.: Interactions in aqueous nonelectrolyte solutions. i. Solute-solvent equilibria, J. Phys. Chem., 70, 2126–2130, 1966. a
Storn, R. and Price, K.: Differential Evolution – A Simple and Efficient Heuristic for global Optimization over Continuous Spaces, J. Global Optim., 11, 341–359, https://doi.org/10.1023/A:1008202821328, 1997. a
Wahab, A. and Mahiuddin, S.: Isentropic Compressibility and Viscosity of Aqueous and Methanolic Calcium Chloride Solutions, J. Chem. Eng. Data, 46, 1457–1463, https://doi.org/10.1021/je010072l, 2001. a
Wallace, B. J. and Preston, T. C.: Water Uptake and Loss in Viscous Aerosol Particles with Concentration-Dependent Diffusivities, J. Phys. Chem. A, 123, 3374–3382, https://doi.org/10.1021/acs.jpca.9b00907, 2019. a
Wang, P., Anderko, A., and Young, R. D.: Modeling viscosity of concentrated and mixed-solvent electrolyte systems, Fluid Phase Equilibr., 226, 71–82, https://doi.org/10.1016/j.fluid.2004.09.008, 2004. a
Wimby, J. M. and Berntsson, T. S.: Viscosity and density of aqueous solutions of lithium bromide, lithium chloride, zinc bromide, calcium chloride and lithium nitrate. 1. Single salt solutions, J. Chem. Eng. Data, 39, 68–72, https://doi.org/10.1021/je00013a019, 1994. a
Wolf, M. J., Zhang, Y., Zawadowicz, M. A., Goodell, M., Froyd, K., Freney, E., Sellegri, K., Rösch, M., Cui, T., Winter, M., Lacher, L., Axisa, D., DeMott, P. J., Levin, E. J. T., Gute, E., Abbatt, J., Koss, A., Kroll, J. H., Surratt, J. D., and Cziczo, D. J.: A biogenic secondary organic aerosol source of cirrus ice nucleating particles, Nat. Commun., 11, 4834, https://doi.org/10.1038/s41467-020-18424-6, 2020. a
Yan, W., Topphoff, M., Rose, C., and Gmehling, J.: Prediction of vapor–liquid equilibria in mixed-solvent electrolyte systems using the group contribution concept, Fluid Phase Equilibr., 162, 97–113, https://doi.org/10.1016/S0378-3812(99)00201-0, 1999. a
Yin, H., Dou, J., Klein,
L., Krieger, U. K., Bain, A., Wallace, B. J., Preston, T. C., and
Zuend, A.: Extension of the AIOMFAC model by iodine and carbonate
species: applications for aerosol acidity and cloud droplet
activation, Atmos. Chem. Phys., 22, 973–1013,
https://doi.org/10.5194/acp-22-973-2022, 2022. a, b, c
You, Y., Smith, M. L., Song, M., Martin, S. T., and Bertram, A. K.: Liquid–liquid phase separation in atmospherically relevant particles consisting of organic species and inorganic salts, Int. Rev. Phys. Chem., 33, 43–77, https://doi.org/10.1080/0144235X.2014.890786, 2014. a
Zdanovskii, A. B.: Regularities in the property variations of mixed solutions, Tr. Solyanoi Lab. Akad. Nauk SSSR, 5–70, 1936. a
Zdanovskii, A. B.: New methods of calculating solubilities of electrolytes in multicomponent systems, Zh. Fiz. Khim., 22, 1478–1485, 1948. a
Zhang, H.-L. and Han, S.-J.: Viscosity and Density of Water + Sodium Chloride + Potassium Chloride Solutions at 298.15 K, J. Chem. Eng. Data, 41, 516–520, https://doi.org/10.1021/je9501402, 1996. a
Zhang, H.-L., Chen, G.-H., and Han, S.-J.: Viscosity and Density of H2O + NaCl + CaCl2 and H2O + KCl + CaCl2 at 298.15 K, J. Chem. Eng. Data, 42, 526–530, https://doi.org/10.1021/je9602733, 1997. a
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J., Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes, Geophys. Res. Lett., 34, L13801, https://doi.org/10.1029/2007GL029979, 2007. a
Zhou, S., Hwang, B. C. H., Lakey, P. S. J., Zuend, A., Abbatt, J. P. D., and Shiraiwa, M.: Multiphase reactivity of polycyclic aromatic hydrocarbons is driven by phase separation and diffusion limitations, P. Natl. Acad. Sci. USA, 116, 11658–11663, https://doi.org/10.1073/pnas.1902517116, 2019. a, b
Zobrist, B., Marcolli, C., Pedernera, D. A., and Koop, T.: Do atmospheric aerosols form glasses?, Atmos. Chem. Phys., 8, 5221–5244, https://doi.org/10.5194/acp-8-5221-2008, 2008. a, b
Zuend, A.: andizuend/AIOMFAC: AIOMFAC-web v3.03 (v3.03), Zenodo [code], https://doi.org/10.5281/zenodo.6049217, 2022. a
Zuend, A. and Seinfeld, J. H.: Modeling the gas-particle partitioning of secondary organic aerosol: the importance of liquid-liquid phase separation, Atmos. Chem. Phys., 12, 3857–3882, https://doi.org/10.5194/acp-12-3857-2012, 2012. a, b
Zuend, A., Marcolli, C., Peter, T., and Seinfeld, J. H.: Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols, Atmos. Chem. Phys., 10, 7795–7820, https://doi.org/10.5194/acp-10-7795-2010, 2010. a, b, c
Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V., Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J. H.: New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups, Atmos. Chem. Phys., 11, 9155–9206, https://doi.org/10.5194/acp-11-9155-2011, 2011. a
Zuend, A., Levac, N., and Seinfeld, J.: AIOMFAC-web website and online model, https://aiomfac.lab.mcgill.ca (last access: 6 December 2021), 2012. a
Zuend, A., Yin, H., and Lilek, J.: AIOMFAC-web v3.00 – Public model code repository, https://github.com/andizuend/AIOMFAC (last access: 6 December 2021), 2021. a
Short summary
Depending on temperature and chemical makeup, certain aerosols can be highly viscous or glassy, with atmospheric implications. We have therefore implemented two major upgrades to the predictive viscosity 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.
Depending on temperature and chemical makeup, certain aerosols can be highly viscous or glassy,...
Altmetrics
Final-revised paper
Preprint