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.
- 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}
}
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/C9CP02725D
DOI: 10.1039/C9CP02725D
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Statistical thermodynamic model for viscosity of pure liquids and liquid mixtures
journal, November 1992
- Cao, Weihong; Fredenslund, Aage; Rasmussen, Peter
- Industrial & Engineering Chemistry Research, Vol. 31, Issue 11
Simultaneous correlation of viscosity and vapor-liquid equilibrium data
journal, September 1993
- Cao, Weihong; Knudsen, Kim; Fredenslund, Aage
- Industrial & Engineering Chemistry Research, Vol. 32, Issue 9
Statistical thermodynamics of liquid mixtures: A new expression for the excess Gibbs energy of partly or completely miscible systems
journal, January 1975
- Abrams, Denis S.; Prausnitz, John M.
- AIChE Journal, Vol. 21, Issue 1
Group-contribution estimation of activity coefficients in nonideal liquid mixtures
journal, November 1975
- Fredenslund, Aage; Jones, Russell L.; Prausnitz, John M.
- AIChE Journal, Vol. 21, Issue 6
Local compositions in thermodynamic excess functions for liquid mixtures
journal, January 1968
- Renon, Henri; Prausnitz, J. M.
- AIChE Journal, Vol. 14, Issue 1
Capturing the Solubility Behavior of CO 2 in Ionic Liquids by a Simple Model †
journal, November 2007
- Andreu, Jordi S.; Vega, Lourdes F.
- The Journal of Physical Chemistry C, Vol. 111, Issue 43
Modeling the Solubility Behavior of CO 2 , H 2 , and Xe in [C n -mim][Tf 2 N] Ionic Liquids
journal, December 2008
- Andreu, Jordi S.; Vega, Lourdes F.
- The Journal of Physical Chemistry B, Vol. 112, Issue 48
Equation of state modeling of the phase equilibria of ionic liquid mixtures at low and high pressure
journal, January 2008
- Karakatsani, Eirini K.; Economou, Ioannis G.; Kroon, Maaike C.
- Physical Chemistry Chemical Physics, Vol. 10, Issue 40
Modeling of the Carbon Dioxide Solubility in Imidazolium-Based Ionic Liquids with the tPC-PSAFT Equation of State
journal, May 2006
- Kroon, Maaike C.; Karakatsani, Eirini K.; Economou, Ioannis G.
- The Journal of Physical Chemistry B, Vol. 110, Issue 18
Solubility of Tetrafluoromethane in the Ionic Liquid [hmim][Tf 2 N]
journal, March 2008
- Kumełan, Jacek; Pérez-Salado Kamps, Álvaro; Tuma, Dirk
- The Journal of Physical Chemistry B, Vol. 112, Issue 10
Systems with ionic liquids: Measurement of VLE and γ∞ data and prediction of their thermodynamic behavior using original UNIFAC, mod. UNIFAC(Do) and COSMO-RS(Ol)
journal, June 2005
- Kato, Ryo; Gmehling, Jürgen
- The Journal of Chemical Thermodynamics, Vol. 37, Issue 6
Correlation of infinite dilution activity coefficient of solute in ionic liquid using UNIFAC model
journal, March 2008
- Wang, Junfeng; Sun, Wei; Li, Chunxi
- Fluid Phase Equilibria, Vol. 264, Issue 1-2
Measurement of vapor–liquid equilibria (VLE) and excess enthalpies (HE) of binary systems with 1-alkyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide and prediction of these properties and γ∞ using modified UNIFAC (Dortmund)
journal, September 2007
- Nebig, Silke; Bölts, Rainer; Gmehling, Jürgen
- Fluid Phase Equilibria, Vol. 258, Issue 2
COSMO-RS: a novel and efficient method for the a priori prediction of thermophysical data of liquids
journal, July 2000
- Klamt, Andreas; Eckert, Frank
- Fluid Phase Equilibria, Vol. 172, Issue 1
A Priori Phase Equilibrium Prediction from a Segment Contribution Solvation Model
journal, March 2002
- Lin, Shiang-Tai; Sandler, Stanley I.
- Industrial & Engineering Chemistry Research, Vol. 41, Issue 5
COSMO: a new approach to dielectric screening in solvents with explicit expressions for the screening energy and its gradient
journal, January 1993
- Klamt, A.; Schüürmann, G.
- J. Chem. Soc., Perkin Trans. 2, Issue 5
Gibbs-duhem-margules laws
journal, January 1996
- Gokcen, N. A.
- Journal of Phase Equilibria, Vol. 17, Issue 1
Liquid—liquid phase splitting—I analytical models for critical mixing and azeotropy
journal, January 1983
- Wisniak, Jaime
- Chemical Engineering Science, Vol. 38, Issue 6
The entropy of high polymer solutions. Generalization of formulae
journal, January 1950
- Staverman, A. J.
- Recueil des Travaux Chimiques des Pays-Bas, Vol. 69, Issue 2
An Improvement to COSMO-SAC for Predicting Thermodynamic Properties
journal, April 2014
- Xiong, Ruichang; Sandler, Stanley I.; Burnett, Russell I.
- Industrial & Engineering Chemistry Research, Vol. 53, Issue 19
Solubility model of metal complex in ionic liquids from first principle calculations
journal, January 2019
- Karmakar, Anwesa; Mukundan, Rangachary; Yang, Ping
- RSC Advances, Vol. 9, Issue 32
COSMOSPACE: Alternative to conventional activity-coefficient models
journal, October 2002
- Klamt, Andreas; Krooshof, Gerard J. P.; Taylor, Ross
- AIChE Journal, Vol. 48, Issue 10
Screening of ionic liquids for CO2 capture using the COSMO-SAC model
journal, January 2015
- Lee, Bong-Seop; Lin, Shiang-Tai
- Chemical Engineering Science, Vol. 121
On the origin of ionicity in ionic liquids. Ion pairing versus charge transfer
journal, January 2014
- Hollóczki, Oldamur; Malberg, Friedrich; Welton, Tom
- Phys. Chem. Chem. Phys., Vol. 16, Issue 32
Refinement and Parametrization of COSMO-RS
journal, June 1998
- Klamt, Andreas; Jonas, Volker; Bürger, Thorsten
- The Journal of Physical Chemistry A, Vol. 102, Issue 26
Solubility of carbon dioxide, nitrous oxide, ethane, and nitrogen in 1-butyl-1-methylpyrrolidinium and trihexyl(tetradecyl)phosphonium tris(pentafluoroethyl)trifluorophosphate (eFAP) ionic liquids
journal, April 2013
- Stevanovic, S.; Costa Gomes, M. F.
- The Journal of Chemical Thermodynamics, Vol. 59
Improvements of COSMO-SAC for vapor–liquid and liquid–liquid equilibrium predictions
journal, October 2010
- Hsieh, Chieh-Ming; Sandler, Stanley I.; Lin, Shiang-Tai
- Fluid Phase Equilibria, Vol. 297, Issue 1
What Determines CO 2 Solubility in Ionic Liquids? A Molecular Simulation Study
journal, July 2015
- Klähn, Marco; Seduraman, Abirami
- The Journal of Physical Chemistry B, Vol. 119, Issue 31
Enthalpic Driving Force for the Selective Absorption of CO 2 by an Ionic Liquid
journal, February 2018
- Daly, Clyde A.; Brinzer, Thomas; Allison, Cecelia
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 6
Molecular Origins of the Apparent Ideal CO 2 Solubilities in Binary Ionic Liquid Mixtures
journal, September 2018
- Kapoor, Utkarsh; Shah, Jindal K.
- The Journal of Physical Chemistry B, Vol. 122, Issue 42
State-of-the-Art of CO 2 Capture with Ionic Liquids
journal, June 2012
- Ramdin, Mahinder; de Loos, Theo W.; Vlugt, Thijs J. H.
- Industrial & Engineering Chemistry Research, Vol. 51, Issue 24
Thermodynamic description of the solvophobic effect in ionic liquids
journal, October 2016
- Sedov, I. A.; Solomonov, B. N.
- Fluid Phase Equilibria, Vol. 425
Ionic liquids as amphiphile self-assembly media
journal, January 2008
- Greaves, Tamar L.; Drummond, Calum J.
- Chemical Society Reviews, Vol. 37, Issue 8
ILThermo: A Free-Access Web Database for Thermodynamic Properties of Ionic Liquids †
journal, July 2007
- Dong, Qian; Muzny, Chris D.; Kazakov, Andrei
- Journal of Chemical & Engineering Data, Vol. 52, Issue 4
Solvation quantities from a COSMO-RS equation of state
journal, November 2015
- Panayiotou, C.; Tsivintzelis, I.; Aslanidou, D.
- The Journal of Chemical Thermodynamics, Vol. 90