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Thermal, Mutual, and Self-Diffusivities of Binary Liquid Mixtures Consisting of Gases Dissolved in n-Alkanes at Infinite Dilution

  • Cédric Giraudet*
    Cédric Giraudet
    Institute of Advanced Optical Technologies - Thermophysical Properties (AOT-TP), Department of Chemical and Biological Engineering (CBI) and Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-University Erlangen-Nürnberg (FAU), Paul-Gordan-Straße 6, 91052 Erlangen, Germany
    *Phone: +49-9131-85-23022. Fax: +49-9131-85-25851. E-mail: [email protected]
  • Tobias Klein
    Tobias Klein
    Institute of Advanced Optical Technologies - Thermophysical Properties (AOT-TP), Department of Chemical and Biological Engineering (CBI) and Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-University Erlangen-Nürnberg (FAU), Paul-Gordan-Straße 6, 91052 Erlangen, Germany
    More by Tobias Klein
  • Guanjia Zhao
    Guanjia Zhao
    Institute of Advanced Optical Technologies - Thermophysical Properties (AOT-TP), Department of Chemical and Biological Engineering (CBI) and Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-University Erlangen-Nürnberg (FAU), Paul-Gordan-Straße 6, 91052 Erlangen, Germany
    Thermal Engineering, College of Electrical and Power Engineering, Taiyuan University of Technology, Taiyuan, Shanxi CN 030024, China
    More by Guanjia Zhao
  • Michael H. Rausch
    Michael H. Rausch
    Institute of Advanced Optical Technologies - Thermophysical Properties (AOT-TP), Department of Chemical and Biological Engineering (CBI) and Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-University Erlangen-Nürnberg (FAU), Paul-Gordan-Straße 6, 91052 Erlangen, Germany
  • Thomas M. Koller
    Thomas M. Koller
    Institute of Advanced Optical Technologies - Thermophysical Properties (AOT-TP), Department of Chemical and Biological Engineering (CBI) and Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-University Erlangen-Nürnberg (FAU), Paul-Gordan-Straße 6, 91052 Erlangen, Germany
  • , and 
  • Andreas P. Fröba
    Andreas P. Fröba
    Institute of Advanced Optical Technologies - Thermophysical Properties (AOT-TP), Department of Chemical and Biological Engineering (CBI) and Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-University Erlangen-Nürnberg (FAU), Paul-Gordan-Straße 6, 91052 Erlangen, Germany
Cite this: J. Phys. Chem. B 2018, 122, 12, 3163–3175
Publication Date (Web):February 27, 2018
https://doi.org/10.1021/acs.jpcb.8b00733
Copyright © 2018 American Chemical Society

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    Abstract

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    In the present study, dynamic light scattering (DLS) experiments and molecular dynamics (MD) simulations were used for the investigation of the molecular diffusion in binary mixtures of liquids with dissolved gases at macroscopic thermodynamic equilibrium. Model systems based on the n-alkane n-hexane or n-decane with dissolved hydrogen, helium, nitrogen, or carbon monoxide were studied at temperatures between 303 and 423 K and at gas mole fractions below 0.06. With DLS, the relaxation behavior of microscopic equilibrium fluctuations in concentration and temperature is analyzed to determine simultaneously mutual and thermal diffusivity in an absolute way. The present measurements document that even for mole gas fractions of 0.007 and Lewis numbers close to 1, reliable mutual diffusivities with an average expanded uncertainty (k = 2) of 13% can be obtained. By use of suitable molecular models for the mixture components, the self-diffusion coefficient of the gases was determined by MD simulations with an averaged expanded uncertainty (k = 2) of 7%. The DLS experiments showed that the thermal diffusivity of the studied systems is not affected by the dissolved gas and agrees with the reference data for the pure n-alkanes. In agreement with theory, mutual diffusivities and self-diffusivities were found to be equal mostly within combined uncertainties at conditions approaching infinite dilution of the gas. Our DLS and MD results, representing the first available data for the present systems, reveal distinctly larger mass diffusivities for mixtures containing hydrogen or helium compared to mixtures containing nitrogen or carbon monoxide. On the basis of the broad range of mass diffusivities of the studied gas–liquid systems covering about 2 orders of magnitude from about 10–9 to 10–7 m2·s–1, effects of the solvent and solute properties on the temperature-dependent mass diffusivities are discussed. This contributed to the development of a simple semiempirical correlation for the mass diffusivity of the studied gases dissolved in n-alkanes of varying chain length at infinite dilution as a function of temperature. The generalized expression requiring only information on the kinematic viscosity and molar mass of the pure solvent as well as the molar mass and acentric factor of the solute represents the database from this work and further literature with an absolute average deviation of about 11%.

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    . The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcb.8b00733.

    • Details on the model for the estimation of the solubility of the gases H2, He, CO, and N2 dissolved in n-C6H14 or n-C10H22, on the influence of the incident laser power on the DLS experiments, and on the computational procedure as well as the data evaluation of the self-diffusivity of the dissolved gases by MD simulations (PDF)

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