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Title: 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 CO 2 in room temperature ionic liquids and to model the selectivity between CO 2 and CH 4 gases. We have shown improved solubility and selectivity prediction of CO 2 and CH 4 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:
ORCiD logo [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (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:  
89233218CNA000001; 20170046DR
Resource Type:
Published Article
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 21; Journal Issue: 35; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
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 CO2 gas in room temperature ionic liquids using the COSMOSAC-LANL model: a first principles study. United States: N. p., 2019. Web. doi:10.1039/C9CP02725D.
Karmakar, Anwesa, & Mukundan, Rangachary. Modeling solubility of CO2 gas in room temperature ionic liquids using the COSMOSAC-LANL model: a first principles study. United States. doi:10.1039/C9CP02725D.
Karmakar, Anwesa, and Mukundan, Rangachary. Fri . "Modeling solubility of CO2 gas in room temperature ionic liquids using the COSMOSAC-LANL model: a first principles study". United States. doi:10.1039/C9CP02725D.
@article{osti_1561377,
title = {Modeling solubility of CO2 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},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 35,
volume = 21,
place = {United States},
year = {2019},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/C9CP02725D

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