Modeling solubility of CO 2 gas in room temperature ionic liquids using the COSMOSAC-LANL model: a first principles study
Abstract
In this paper we present a thermodynamic model for asymmetric solutions with a special emphasis on solute–solvent interactions. The new “COSMOSAC-LANL” activity coefficient model is rooted in first principles calculations based on the COSMO model where the microscopic information passes to the macroscopic world via a dielectric continuum solvation model followed by a post statistical thermodynamic treatment of self-consistent properties of the solute particle. To model the activity coefficient at infinite dilution for the binary mixtures, a 3-suffix Margules (3sM) function is introduced to model asymmetric interactions and, for the combinatorial term, the Staverman–Guggenheim (SG) form is used. The new “COSMOSAC-LANL” activity coefficient model has been used to calculate the solubility of CO2 in room temperature ionic liquids and to model the selectivity between CO2 and CH4 gases. We have shown improved solubility and selectivity prediction of CO2 and CH4 gas in room temperature ionic liquids using the ADF-COSMOSAC-2013 model with the new “LANL” activity coefficient model. The calculated values have been compared with experimental results where they are available.
- Authors:
-
- Theoretical Division (T-1), Los Alamos National Laboratory, Los Alamos 87545, USA
- MPA-11 Division, Los Alamos National Laboratory, Los Alamos 87545, USA
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1561377
- Alternate Identifier(s):
- OSTI ID: 1570644
- Report Number(s):
- LA-UR-19-22863
Journal ID: ISSN 1463-9076; PPCPFQ
- Grant/Contract Number:
- 20170046DR; 89233218CNA000001
- Resource Type:
- Journal Article: Published Article
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Volume: 21 Journal Issue: 35; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 gas capture; Ionic Liquids; COSMOSAC
Citation Formats
Karmakar, Anwesa, and Mukundan, Rangachary. Modeling solubility of CO 2 gas in room temperature ionic liquids using the COSMOSAC-LANL model: a first principles study. United Kingdom: N. p., 2019.
Web. doi:10.1039/C9CP02725D.
Karmakar, Anwesa, & Mukundan, Rangachary. Modeling solubility of CO 2 gas in room temperature ionic liquids using the COSMOSAC-LANL model: a first principles study. United Kingdom. https://doi.org/10.1039/C9CP02725D
Karmakar, Anwesa, and Mukundan, Rangachary. 2019.
"Modeling solubility of CO 2 gas in room temperature ionic liquids using the COSMOSAC-LANL model: a first principles study". United Kingdom. https://doi.org/10.1039/C9CP02725D.
@article{osti_1561377,
title = {Modeling solubility of CO 2 gas in room temperature ionic liquids using the COSMOSAC-LANL model: a first principles study},
author = {Karmakar, Anwesa and Mukundan, Rangachary},
abstractNote = {In this paper we present a thermodynamic model for asymmetric solutions with a special emphasis on solute–solvent interactions. The new “COSMOSAC-LANL” activity coefficient model is rooted in first principles calculations based on the COSMO model where the microscopic information passes to the macroscopic world via a dielectric continuum solvation model followed by a post statistical thermodynamic treatment of self-consistent properties of the solute particle. To model the activity coefficient at infinite dilution for the binary mixtures, a 3-suffix Margules (3sM) function is introduced to model asymmetric interactions and, for the combinatorial term, the Staverman–Guggenheim (SG) form is used. The new “COSMOSAC-LANL” activity coefficient model has been used to calculate the solubility of CO2 in room temperature ionic liquids and to model the selectivity between CO2 and CH4 gases. We have shown improved solubility and selectivity prediction of CO2 and CH4 gas in room temperature ionic liquids using the ADF-COSMOSAC-2013 model with the new “LANL” activity coefficient model. The calculated values have been compared with experimental results where they are available.},
doi = {10.1039/C9CP02725D},
url = {https://www.osti.gov/biblio/1561377},
journal = {Physical Chemistry Chemical Physics. PCCP},
issn = {1463-9076},
number = 35,
volume = 21,
place = {United Kingdom},
year = {Wed Sep 11 00:00:00 EDT 2019},
month = {Wed Sep 11 00:00:00 EDT 2019}
}
Web of Science
Figures / Tables:
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