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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 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:
ORCiD logo [1];  [2]
  1. Theoretical Division (T-1), Los Alamos National Laboratory, Los Alamos 87545, USA
  2. 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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1039/C9CP02725D

Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: A cartoon representation of asymmetric interaction in a binary mixture at infinite dilution.

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Works referenced in this record:

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