Characterization of molecular diffusion in liquids with dissolved gases
Final Report Abstract
Molecular mass diffusion was characterized in binary mixtures of a liquid with a dissolved gas over a wide range of thermodynamic states by applying dynamic light scattering (DLS) and equilibrium molecular dynamics (EMD) simulations for the determination and prediction of the Fick diffusion coefficient D11. DLS contributed to a reliable database where results were used as validation for EMD simulations, which, in turn, provide insight into the fluid structure and support the interpretation of D11 values. D11 predicted with EMD simulations close to infinite dilution of the gas or over a wide composition range agreed well with the DLS results in nearly all cases. Correct modelling of the interactions between solute and solvent represented by the thermodynamic factor was shown to be crucial for the accurate prediction of D11. In the second funding period, the chosen systems included extended ranges of molecular characteristics like molar mass, size, and polarity of gases as well as chain length, branching, oxygenation, and degree of hydrogenation of liquids. The 89 mixtures studied provided a sound database for developing an improved prediction model for D11 close to infinite dilution of the dissolved gas, where newly identified relations between fluid properties and diffusivities were considered. For 765 D11 data from this work and literature spanning seven orders of magnitude, the average absolute relative deviation of predicted from experimental data is 21%.
Publications
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Diffusivities in Binary Mixtures of [AMIM][NTf2] Ionic Liquids with the Dissolved Gases H2, He, N2, CO, CO2, or Kr Close to Infinite Dilution. Journal of Chemical & Engineering Data, 65(8), 4116-4129.
Klein, Tobias; Piszko, Maximilian; Lang, Maren; Mehler, Julian; Schulz, Peter S.; Rausch, Michael H.; Giraudet, Cédric; Koller, Thomas M. & Fröba, Andreas P.
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Diffusivities in Binary Mixtures of n-Hexane or 1-Hexanol with Dissolved CH4, Ne, Kr, R143a, SF6, or R236fa Close to Infinite Dilution. Journal of Chemical & Engineering Data, 66(5), 2218-2232.
Piszko, Maximilian; Lenahan, Frances D.; Hahn, Simon; Rausch, Michael H.; Koller, Thomas M.; Klein, Tobias & Fröba, Andreas P.
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Diffusivities in Binary Mixtures of n-Decane, n-Hexadecane, n-Octacosane, 2-Methylpentane, 2,2-Dimethylbutane, Cyclohexane, Benzene, Ethanol, 1-Decanol, Ethyl Butanoate, or n-Hexanoic Acid with Dissolved He or Kr Close to Infinite Dilution. Journal of Chemical & Engineering Data, 67(3), 622-635.
Lenahan, Frances D.; Piszko, Maximilian; Klein, Tobias & Fröba, Andreas P.
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Mutual and Thermal Diffusivities in Mixtures of Cyclohexane, n-Hexadecane, n-Octacosane, or n-Hexanoic Acid with Carbon Dioxide Obtained by Dynamic Light Scattering and Molecular Dynamics Simulations. Journal of Chemical & Engineering Data, 67(10), 3059-3076.
Piszko, Maximilian; Lenahan, Frances D.; Friedl, Lukas; Klein, Tobias & Fröba, Andreas P.
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Diffusivities in Binary Mixtures of Cyclohexane or Ethyl Butanoate with Dissolved CH4 or R143a Close to Infinite Dilution. Journal of Chemical & Engineering Data, 68(2), 339-348.
Piszko, Maximilian; Lenahan, Frances D.; Klein, Tobias & Fröba, Andreas P.
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Molecular dynamics simulations of liquid ethane up to 298.15 K. Molecular Physics, 121(14).
Lenahan, Frances D.; Piszko, Maximilian; Klein, Tobias & Fröba, Andreas P.
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Mutual and Thermal Diffusivities in Binary Mixtures of n-Hexane or 1-Hexanol with Krypton, R143a, or Sulfur Hexafluoride by Using Dynamic Light Scattering and Molecular Dynamics Simulations. Journal of Chemical & Engineering Data, 68(6), 1343-1357.
Piszko, Maximilian; Lenahan, Frances D.; Dennstädt, Claudio; Klein, Tobias & Fröba, Andreas P.
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Solubility and Liquid Density of Binary Mixtures of n-Hexane or 1-Hexanol with Krypton, Sulfur Hexafluoride, or R143a. Journal of Chemical & Engineering Data, 68(4), 813-834.
Jander, Julius H.; Piszko, Maximilian; Kühl, Julius V. W.; Rausch, Michael H. & Fröba, Andreas P.
