Mutual and Self-Diffusivities in Binary Mixtures of [EMIM][B(CN)4] with Dissolved Gases by Using Dynamic Light Scattering and Molecular Dynamics Simulations

Thomas M. Koller, Andreas Heller, Michael H. Rausch, Peter Wasserscheid, Ioannis Economou, Andreas P. Fröba

Research output: Contribution to journalArticle

12 Citations (Scopus)

Abstract

Ionic liquids (ILs) are possible working fluids for the separation of carbon dioxide (CO2) from flue gases. For evaluating their performance in such processes, reliable mutual-diffusivity data are required for mixtures of ILs with relevant flue gas components. In the present study, dynamic light scattering (DLS) and molecular dynamics (MD) simulations were used for the investigation of the molecular diffusion in binary mixtures of the IL 1-ethyl-3-methylimidazolium tetracyanoborate ([EMIM][B(CN)4]) with the dissolved gases carbon dioxide, nitrogen, carbon monoxide, hydrogen, methane, oxygen, and hydrogen sulfide at temperatures from 298.15 to 363.15 K and pressures up to 63 bar. At conditions approaching infinite dilution of a gas, the Fick mutual diffusivity of the mixture measured by DLS and the self-diffusivity of the corresponding gas calculated by MD simulations match, which could be generally found within combined uncertainties. The obtained diffusivities are in agreement with literature data for the same or comparable systems as well as with the general trend of increasing diffusivities for decreasing IL viscosities. The DLS and MD results reveal distinctly larger molecular diffusivities for [EMIM][B(CN)4]-hydrogen mixtures compared to mixtures with all other gases. This behavior results in the failure of an empirical correlation with the molar volumes of the gases at their normal boiling points. The DLS experiments also showed that there is no noticeable influence of the dissolved gas and temperature on the thermal diffusivity of the studied systems. (Figure Presented).

Original languageEnglish
Pages (from-to)8583-8592
Number of pages10
JournalJournal of Physical Chemistry B
Volume119
Issue number27
DOIs
Publication statusPublished - 9 Jul 2015

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dissolved gases
Dynamic light scattering
Molecular Dynamics Simulation
Binary mixtures
binary mixtures
diffusivity
Molecular dynamics
light scattering
Gases
Ionic Liquids
molecular dynamics
Ionic liquids
Computer simulation
flue gases
simulation
liquids
gases
carbon dioxide
sulfides
Flue gases

ASJC Scopus subject areas

  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry
  • Materials Chemistry

Cite this

Mutual and Self-Diffusivities in Binary Mixtures of [EMIM][B(CN)4] with Dissolved Gases by Using Dynamic Light Scattering and Molecular Dynamics Simulations. / Koller, Thomas M.; Heller, Andreas; Rausch, Michael H.; Wasserscheid, Peter; Economou, Ioannis; Fröba, Andreas P.

In: Journal of Physical Chemistry B, Vol. 119, No. 27, 09.07.2015, p. 8583-8592.

Research output: Contribution to journalArticle

Koller, Thomas M. ; Heller, Andreas ; Rausch, Michael H. ; Wasserscheid, Peter ; Economou, Ioannis ; Fröba, Andreas P. / Mutual and Self-Diffusivities in Binary Mixtures of [EMIM][B(CN)4] with Dissolved Gases by Using Dynamic Light Scattering and Molecular Dynamics Simulations. In: Journal of Physical Chemistry B. 2015 ; Vol. 119, No. 27. pp. 8583-8592.
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abstract = "Ionic liquids (ILs) are possible working fluids for the separation of carbon dioxide (CO2) from flue gases. For evaluating their performance in such processes, reliable mutual-diffusivity data are required for mixtures of ILs with relevant flue gas components. In the present study, dynamic light scattering (DLS) and molecular dynamics (MD) simulations were used for the investigation of the molecular diffusion in binary mixtures of the IL 1-ethyl-3-methylimidazolium tetracyanoborate ([EMIM][B(CN)4]) with the dissolved gases carbon dioxide, nitrogen, carbon monoxide, hydrogen, methane, oxygen, and hydrogen sulfide at temperatures from 298.15 to 363.15 K and pressures up to 63 bar. At conditions approaching infinite dilution of a gas, the Fick mutual diffusivity of the mixture measured by DLS and the self-diffusivity of the corresponding gas calculated by MD simulations match, which could be generally found within combined uncertainties. The obtained diffusivities are in agreement with literature data for the same or comparable systems as well as with the general trend of increasing diffusivities for decreasing IL viscosities. The DLS and MD results reveal distinctly larger molecular diffusivities for [EMIM][B(CN)4]-hydrogen mixtures compared to mixtures with all other gases. This behavior results in the failure of an empirical correlation with the molar volumes of the gases at their normal boiling points. The DLS experiments also showed that there is no noticeable influence of the dissolved gas and temperature on the thermal diffusivity of the studied systems. (Figure Presented).",
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AB - Ionic liquids (ILs) are possible working fluids for the separation of carbon dioxide (CO2) from flue gases. For evaluating their performance in such processes, reliable mutual-diffusivity data are required for mixtures of ILs with relevant flue gas components. In the present study, dynamic light scattering (DLS) and molecular dynamics (MD) simulations were used for the investigation of the molecular diffusion in binary mixtures of the IL 1-ethyl-3-methylimidazolium tetracyanoborate ([EMIM][B(CN)4]) with the dissolved gases carbon dioxide, nitrogen, carbon monoxide, hydrogen, methane, oxygen, and hydrogen sulfide at temperatures from 298.15 to 363.15 K and pressures up to 63 bar. At conditions approaching infinite dilution of a gas, the Fick mutual diffusivity of the mixture measured by DLS and the self-diffusivity of the corresponding gas calculated by MD simulations match, which could be generally found within combined uncertainties. The obtained diffusivities are in agreement with literature data for the same or comparable systems as well as with the general trend of increasing diffusivities for decreasing IL viscosities. The DLS and MD results reveal distinctly larger molecular diffusivities for [EMIM][B(CN)4]-hydrogen mixtures compared to mixtures with all other gases. This behavior results in the failure of an empirical correlation with the molar volumes of the gases at their normal boiling points. The DLS experiments also showed that there is no noticeable influence of the dissolved gas and temperature on the thermal diffusivity of the studied systems. (Figure Presented).

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