Understanding Gas Absorption in Multivalent Ionic Liquids via Solute-Solvent Interaction Analyses

Liu, Xiaoyang; Heath Turner, C.

doi:10.1016/j.cplett.2021.139204

Title: Understanding Gas Absorption in Multivalent Ionic Liquids via Solute-Solvent Interaction Analyses

Abstract

Solute-solvent interactions are often evaluated to understand and explain gas solubilities. This information is regularly used to interpret gas solubility and separation within ionic liquids (ILs). Here, we use several different quantum chemical and previous molecular dynamics simulation results to show that strong solute-solvent interactions neither lead to high solubility nor to high selectivity, with respect to other solutes. Instead, the solute-solvent interaction strength with different isolated IL ions is affected by the electrostatic extremes. Also, the solute-solvent interaction with different IL molecules is strongly correlated to the molecular volumes or polarizabilities (within a series of same-anion based ILs).

Authors:

^[1];

^[1]

Univ. of Alabama, Tuscaloosa, AL (United States)

Publication Date:: 2021-11-10

Research Org.:: Univ. of Alabama, Tuscaloosa, AL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1830673

Alternate Identifier(s):: OSTI ID: 1832646

Grant/Contract Number:: SC0018181

Resource Type:: Accepted Manuscript

Journal Name:: Chemical Physics Letters

Additional Journal Information:: Journal Volume: 786; Journal ID: ISSN 0009-2614

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ionic liquids; gas capture; interaction; solubility; affinity

Citation Formats


                    Liu, Xiaoyang, and Heath Turner, C. Understanding Gas Absorption in Multivalent Ionic Liquids via Solute-Solvent Interaction Analyses.  United States: N. p., 2021. 
Web.  doi:10.1016/j.cplett.2021.139204.

Copy to clipboard


                    Liu, Xiaoyang, & Heath Turner, C. Understanding Gas Absorption in Multivalent Ionic Liquids via Solute-Solvent Interaction Analyses.  United States.  https://doi.org/10.1016/j.cplett.2021.139204

Copy to clipboard


                    Liu, Xiaoyang, and Heath Turner, C. Wed .  
"Understanding Gas Absorption in Multivalent Ionic Liquids via Solute-Solvent Interaction Analyses".  United States.  https://doi.org/10.1016/j.cplett.2021.139204.  https://www.osti.gov/servlets/purl/1830673.

Copy to clipboard


                    
@article{osti_1830673,

  title        = {Understanding Gas Absorption in Multivalent Ionic Liquids via Solute-Solvent Interaction Analyses},

  author       = {Liu, Xiaoyang and Heath Turner, C.},

  abstractNote = {Solute-solvent interactions are often evaluated to understand and explain gas solubilities. This information is regularly used to interpret gas solubility and separation within ionic liquids (ILs). Here, we use several different quantum chemical and previous molecular dynamics simulation results to show that strong solute-solvent interactions neither lead to high solubility nor to high selectivity, with respect to other solutes. Instead, the solute-solvent interaction strength with different isolated IL ions is affected by the electrostatic extremes. Also, the solute-solvent interaction with different IL molecules is strongly correlated to the molecular volumes or polarizabilities (within a series of same-anion based ILs).},

  doi          = {10.1016/j.cplett.2021.139204},

  journal      = {Chemical Physics Letters},

  number       = ,

  volume       = 786,

  place        = {United States},

  year         = {2021},

  month        = {11}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (Publisher)

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1016/j.cplett.2021.139204

Other availability

Search WorldCat to find libraries that may hold this journal

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Breakdown of the Single-Exchange Approximation in Third-Order Symmetry-Adapted Perturbation Theory
journal, December 2011

Lao, Ka Un; Herbert, John M.
The Journal of Physical Chemistry A, Vol. 116, Issue 11
DOI: 10.1021/jp300109y

GFN2-xTB—An Accurate and Broadly Parametrized Self-Consistent Tight-Binding Quantum Chemical Method with Multipole Electrostatics and Density-Dependent Dispersion Contributions
journal, January 2019

Bannwarth, Christoph; Ehlert, Sebastian; Grimme, Stefan
Journal of Chemical Theory and Computation, Vol. 15, Issue 3
DOI: 10.1021/acs.jctc.8b01176

Psi4 1.1: An Open-Source Electronic Structure Program Emphasizing Automation, Advanced Libraries, and Interoperability
journal, June 2017

Parrish, Robert M.; Burns, Lori A.; Smith, Daniel G. A.
Journal of Chemical Theory and Computation, Vol. 13, Issue 7
DOI: 10.1021/acs.jctc.7b00174

Quantitative analysis of molecular surface based on improved Marching Tetrahedra algorithm
journal, September 2012

Lu, Tian; Chen, Feiwu
Journal of Molecular Graphics and Modelling, Vol. 38
DOI: 10.1016/j.jmgm.2012.07.004

Low viscosity superbase protic ionic liquids for the highly efficient simultaneous removal of H2S and CO2 from CH4
journal, May 2021

Xiong, Wenjie; Shi, Mingzhen; Peng, Lingling
Separation and Purification Technology, Vol. 263
DOI: 10.1016/j.seppur.2021.118417

Wavefunction and reactivity study of benzo[a]pyrene diol epoxide and its enantiomeric forms
journal, April 2014

Lu, Tian; Manzetti, Sergio
Structural Chemistry, Vol. 25, Issue 5
DOI: 10.1007/s11224-014-0430-6

Highly selective absorption separation of H ₂ S and CO ₂ from CH ₄ by novel azole‐based protic ionic liquids
journal, February 2020

Zhang, Xiaomin; Xiong, Wenjie; Peng, Lingling
AIChE Journal, Vol. 66, Issue 6
DOI: 10.1002/aic.16936

van der Waals potential: an important complement to molecular electrostatic potential in studying intermolecular interactions
journal, October 2020

Lu, Tian; Chen, Qinxue
Journal of Molecular Modeling, Vol. 26, Issue 11
DOI: 10.1007/s00894-020-04577-0

Multiwfn: A multifunctional wavefunction analyzer
journal, December 2011

Lu, Tian; Chen, Feiwu
Journal of Computational Chemistry, Vol. 33, Issue 5
DOI: 10.1002/jcc.22885

Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density
journal, January 1988

Lee, Chengteh; Yang, Weitao; Parr, Robert G.
Physical Review B, Vol. 37, Issue 2
DOI: 10.1103/PhysRevB.37.785

UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations
journal, December 1992

Rappe, A. K.; Casewit, C. J.; Colwell, K. S.
Journal of the American Chemical Society, Vol. 114, Issue 25, p. 10024-10035
DOI: 10.1021/ja00051a040

B97-3c: A revised low-cost variant of the B97-D density functional method
journal, February 2018

Brandenburg, Jan Gerit; Bannwarth, Christoph; Hansen, Andreas
The Journal of Chemical Physics, Vol. 148, Issue 6
DOI: 10.1063/1.5012601

Screening Ionic Liquids Based on Ionic Volume and Electrostatic Potential Analyses
journal, April 2021

Liu, Xiaoyang; O’Harra, Kathryn E.; Bara, Jason E.
The Journal of Physical Chemistry B, Vol. 125, Issue 14
DOI: 10.1021/acs.jpcb.0c10259

A Robust and Accurate Tight-Binding Quantum Chemical Method for Structures, Vibrational Frequencies, and Noncovalent Interactions of Large Molecular Systems Parametrized for All spd-Block Elements ( Z = 1–86)
journal, April 2017

Grimme, Stefan; Bannwarth, Christoph; Shushkov, Philip
Journal of Chemical Theory and Computation, Vol. 13, Issue 5
DOI: 10.1021/acs.jctc.7b00118

Ionic-Liquid-Based CO ₂ Capture Systems: Structure, Interaction and Process
journal, May 2017

Zeng, Shaojuan; Zhang, Xiangping; Bai, Lu
Chemical Reviews, Vol. 117, Issue 14
DOI: 10.1021/acs.chemrev.7b00072

Physical Absorption Of CO ₂ in Protic and Aprotic Ionic Liquids: An Interaction Perspective
journal, August 2015

Izgorodina, Ekaterina I.; Hodgson, Jennifer L.; Weis, Derick C.
The Journal of Physical Chemistry B, Vol. 119, Issue 35
DOI: 10.1021/acs.jpcb.5b05115

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
DOI: 10.1021/acs.jpcb.5b03674

Polarizability and volume
journal, March 1993

Brinck, Tore; Murray, Jane S.; Politzer, Peter
The Journal of Chemical Physics, Vol. 98, Issue 5
DOI: 10.1063/1.465038

Understanding the High Solubility of CO ₂ in an Ionic Liquid with the Tetracyanoborate Anion
journal, August 2011

Babarao, Ravichandar; Dai, Sheng; Jiang, De-en
The Journal of Physical Chemistry B, Vol. 115, Issue 32
DOI: 10.1021/jp205399r

Gas Solubility in Ionic Liquids
journal, November 2013

Lei, Zhigang; Dai, Chengna; Chen, Biaohua
Chemical Reviews, Vol. 114, Issue 2
DOI: 10.1021/cr300497a

Automated exploration of the low-energy chemical space with fast quantum chemical methods
journal, January 2020

Pracht, Philipp; Bohle, Fabian; Grimme, Stefan
Physical Chemistry Chemical Physics, Vol. 22, Issue 14
DOI: 10.1039/C9CP06869D

Solubility Behavior of CO ₂ in Ionic Liquids Based on Ionic Polarity Index Analyses
journal, April 2021

Liu, Xiaoyang; O’Harra, Kathryn E.; Bara, Jason E.
The Journal of Physical Chemistry B, Vol. 125, Issue 14
DOI: 10.1021/acs.jpcb.1c01508

A new mixing of Hartree–Fock and local density‐functional theories
journal, January 1993

Becke, Axel D.
The Journal of Chemical Physics, Vol. 98, Issue 2
DOI: 10.1063/1.464304

Computational study of the electrostatic potential and charges of multivalent ionic liquid molecules
journal, October 2021

Liu, Xiaoyang; Turner, C. Heath
Journal of Molecular Liquids, Vol. 340
DOI: 10.1016/j.molliq.2021.117190

Accurately extracting the signature of intermolecular interactions present in the NCI plot of the reduced density gradient versus electron density
journal, January 2017

Lefebvre, Corentin; Rubez, Gaëtan; Khartabil, Hassan
Physical Chemistry Chemical Physics, Vol. 19, Issue 27
DOI: 10.1039/C7CP02110K

Carbon capture with ionic liquids: overview and progress
journal, January 2012

Zhang, Xiangping; Zhang, Xiaochun; Dong, Haifeng
Energy & Environmental Science, Vol. 5, Issue 5
DOI: 10.1039/c2ee21152a

Understanding Gas Solubility of Pure Component and Binary Mixtures within Multivalent Ionic Liquids from Molecular Simulations
journal, July 2021

Liu, Xiaoyang; Bara, Jason E.; Turner, C. Heath
The Journal of Physical Chemistry B, Vol. 125, Issue 29
DOI: 10.1021/acs.jpcb.1c04212

The calculation of small molecular interactions by the differences of separate total energies. Some procedures with reduced errors
journal, October 1970

Boys, S.F.; Bernardi, F.
Molecular Physics, Vol. 19, Issue 4, p. 553-566
DOI: 10.1080/00268977000101561

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010

Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
The Journal of Chemical Physics, Vol. 132, Issue 15
DOI: 10.1063/1.3382344

VMD: Visual molecular dynamics
journal, February 1996

Humphrey, William; Dalke, Andrew; Schulten, Klaus
Journal of Molecular Graphics, Vol. 14, Issue 1
DOI: 10.1016/0263-7855(96)00018-5

Similar Records in DOE PAGES and OSTI.GOV collections:

Molecular insight into the anion effect and free volume effect of CO₂ solubility in multivalent ionic liquids

Journal Article Liu, Xiaoyang ; O’Harra, Kathryn E. ; Bara, Jason E. ; ... - Physical Chemistry Chemical Physics. PCCP

For many years, experimental and theoretical studies have investigated the solubility of CO₂ in a variety of ionic liquids (ILs), but the overarching absorption mechanism is still unclear. Currently, two different factors are believed to dominate the absorption performance: (a) the fractional free volume (FFV) accessible for absorption; and (b) the nature of the CO₂ interactions with the anion species. The FFV is often more influential than the specific choice of the anion, but neither mechanism provides a complete picture. Herein, we have attempted to decouple these mechanisms in order to provide a more definitive molecular-level perspective of CO₂ absorptionmore »« less
https://doi.org/10.1039/d0cp03424j

Full Text Available
Understanding Gas Solubility of Pure Component and Binary Mixtures within Multivalent Ionic Liquids from Molecular Simulations

Journal Article Liu, Xiaoyang ; Bara, Jason E. ; Turner, C. Heath - Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

Understanding the molecular-level solubility of CO₂ and its mixtures is essential to the progress of gas treating technologies. Herein, we use grand canonical Monte Carlo simulations to study the single component gas absorption of SO₂, N₂, CH₄, and H₂, and binary mixtures of CO₂/SO₂, CO₂/N₂, CO₂/CH₄, and CO₂/H₂ of varying mole fractions within multivalent ionic liquids (ILs). Our results highlight the importance of the free volume effect and the anion effect when interpreting the absorption behavior of these mixtures, similar to the behavior of CO₂ found in our previous study. The deviation of the gas solubility between the pure componentmore »« less
https://doi.org/10.1021/acs.jpcb.1c04212

Full Text Available
Computational study of the electrostatic potential and charges of multivalent ionic liquid molecules

Journal Article Liu, Xiaoyang ; Turner, C. Heath - Journal of Molecular Liquids

The electrostatic interactions in ionic liquids (ILs) can be difficult to quantify, but this information is very valuable for improving intermolecular potentials for performing molecular-level simulations. Although polarizable forcefields can provide improved accuracy, the computational efficiency of fixed charge molecular models is often preferred for larger systems. Here, we propose a multi-scale screening approach for analyzing the charge scaling behavior and other electrostatic properties of ILs, which is more attainable than previous analysis methods that rely on the IL crystalline structures. Based on isolated molecules and small clusters, we study the electrostatic potential properties and charges of multivalent IL moleculesmore »« less
https://doi.org/10.1016/j.molliq.2021.117190

Full Text Available
Solubility Behavior of CO₂ in Ionic Liquids Based on Ionic Polarity Index Analyses

Journal Article Liu, Xiaoyang ; O’Harra, Kathryn E. ; Bara, Jason E. ; ... - Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

Ionic liquids (ILs) can serve as effective CO2 solvents with an appropriate selection of different anions and cations. However, due to the large library of potential IL compositions, rapid screening methods are needed for characterizing and ranking the expected properties. We have recently proposed the ionic polarity index (IPI) parameter, effectively connecting volume-based approaches and electrostatic potential analyses and providing a single metric that can potentially be used to rapidly screen for desirable IL properties. In this work, the corresponding anion and cation IPIs are used to generate correlations with respect to the CO2 volumetric solubility in ILs. The relationshipsmore »« less
https://doi.org/10.1021/acs.jpcb.1c01508

Full Text Available
Quantifying the anion effect of gas solubility within ionic liquids using the solvation affinity index

Journal Article Liu, Xiaoyang ; Turner, C. Heath - Chemical Engineering Science

The solubility of gas molecules within ionic liquids (ILs) is strongly dictated by the anion effect and the free volume effect, and of these two influences, the anion effect can be challenging to predict. We evaluate a wide range of different gas solutes (O₂, NH₃, CH₄, H₂S, SO₂, Ar, H₂, N₂, CO₂) in different ILs, and we find that the solubility is strongly correlated to one of three different IL properties, which can be directly calculated from the anion electrostatic potential (ESP) surfaces. Thus, the solutes can be grouped into three fundamental types, leading to a general descriptor, the solvationmore »« less
https://doi.org/10.1016/j.ces.2022.117851

Similar Records

Title: Understanding Gas Absorption in Multivalent Ionic Liquids via Solute-Solvent Interaction Analyses

Abstract

Citation Formats

Breakdown of the Single-Exchange Approximation in Third-Order Symmetry-Adapted Perturbation Theory journal, December 2011

GFN2-xTB—An Accurate and Broadly Parametrized Self-Consistent Tight-Binding Quantum Chemical Method with Multipole Electrostatics and Density-Dependent Dispersion Contributions journal, January 2019

Psi4 1.1: An Open-Source Electronic Structure Program Emphasizing Automation, Advanced Libraries, and Interoperability journal, June 2017

Quantitative analysis of molecular surface based on improved Marching Tetrahedra algorithm journal, September 2012

Low viscosity superbase protic ionic liquids for the highly efficient simultaneous removal of H2S and CO2 from CH4 journal, May 2021

Wavefunction and reactivity study of benzo[a]pyrene diol epoxide and its enantiomeric forms journal, April 2014

Highly selective absorption separation of H 2 S and CO 2 from CH 4 by novel azole‐based protic ionic liquids journal, February 2020

van der Waals potential: an important complement to molecular electrostatic potential in studying intermolecular interactions journal, October 2020

Multiwfn: A multifunctional wavefunction analyzer journal, December 2011

Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density journal, January 1988

UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations journal, December 1992

B97-3c: A revised low-cost variant of the B97-D density functional method journal, February 2018

Screening Ionic Liquids Based on Ionic Volume and Electrostatic Potential Analyses journal, April 2021

A Robust and Accurate Tight-Binding Quantum Chemical Method for Structures, Vibrational Frequencies, and Noncovalent Interactions of Large Molecular Systems Parametrized for All spd-Block Elements ( Z = 1–86) journal, April 2017

Ionic-Liquid-Based CO 2 Capture Systems: Structure, Interaction and Process journal, May 2017

Physical Absorption Of CO 2 in Protic and Aprotic Ionic Liquids: An Interaction Perspective journal, August 2015

What Determines CO 2 Solubility in Ionic Liquids? A Molecular Simulation Study journal, July 2015

Polarizability and volume journal, March 1993

Understanding the High Solubility of CO 2 in an Ionic Liquid with the Tetracyanoborate Anion journal, August 2011

Gas Solubility in Ionic Liquids journal, November 2013

Automated exploration of the low-energy chemical space with fast quantum chemical methods journal, January 2020

Solubility Behavior of CO 2 in Ionic Liquids Based on Ionic Polarity Index Analyses journal, April 2021

A new mixing of Hartree–Fock and local density‐functional theories journal, January 1993

Computational study of the electrostatic potential and charges of multivalent ionic liquid molecules journal, October 2021

Accurately extracting the signature of intermolecular interactions present in the NCI plot of the reduced density gradient versus electron density journal, January 2017

Carbon capture with ionic liquids: overview and progress journal, January 2012

Understanding Gas Solubility of Pure Component and Binary Mixtures within Multivalent Ionic Liquids from Molecular Simulations journal, July 2021

The calculation of small molecular interactions by the differences of separate total energies. Some procedures with reduced errors journal, October 1970

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal, April 2010

VMD: Visual molecular dynamics journal, February 1996

Breakdown of the Single-Exchange Approximation in Third-Order Symmetry-Adapted Perturbation Theory
journal, December 2011

GFN2-xTB—An Accurate and Broadly Parametrized Self-Consistent Tight-Binding Quantum Chemical Method with Multipole Electrostatics and Density-Dependent Dispersion Contributions
journal, January 2019

Psi4 1.1: An Open-Source Electronic Structure Program Emphasizing Automation, Advanced Libraries, and Interoperability
journal, June 2017

Quantitative analysis of molecular surface based on improved Marching Tetrahedra algorithm
journal, September 2012

Low viscosity superbase protic ionic liquids for the highly efficient simultaneous removal of H2S and CO2 from CH4
journal, May 2021

Wavefunction and reactivity study of benzo[a]pyrene diol epoxide and its enantiomeric forms
journal, April 2014

Highly selective absorption separation of H ₂ S and CO ₂ from CH ₄ by novel azole‐based protic ionic liquids
journal, February 2020

van der Waals potential: an important complement to molecular electrostatic potential in studying intermolecular interactions
journal, October 2020

Multiwfn: A multifunctional wavefunction analyzer
journal, December 2011

Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density
journal, January 1988

UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations
journal, December 1992

B97-3c: A revised low-cost variant of the B97-D density functional method
journal, February 2018

Screening Ionic Liquids Based on Ionic Volume and Electrostatic Potential Analyses
journal, April 2021

A Robust and Accurate Tight-Binding Quantum Chemical Method for Structures, Vibrational Frequencies, and Noncovalent Interactions of Large Molecular Systems Parametrized for All spd-Block Elements ( Z = 1–86)
journal, April 2017

Ionic-Liquid-Based CO ₂ Capture Systems: Structure, Interaction and Process
journal, May 2017

Physical Absorption Of CO ₂ in Protic and Aprotic Ionic Liquids: An Interaction Perspective
journal, August 2015

What Determines CO ₂ Solubility in Ionic Liquids? A Molecular Simulation Study
journal, July 2015

Polarizability and volume
journal, March 1993

Understanding the High Solubility of CO ₂ in an Ionic Liquid with the Tetracyanoborate Anion
journal, August 2011

Gas Solubility in Ionic Liquids
journal, November 2013

Automated exploration of the low-energy chemical space with fast quantum chemical methods
journal, January 2020

Solubility Behavior of CO ₂ in Ionic Liquids Based on Ionic Polarity Index Analyses
journal, April 2021

A new mixing of Hartree–Fock and local density‐functional theories
journal, January 1993

Computational study of the electrostatic potential and charges of multivalent ionic liquid molecules
journal, October 2021

Accurately extracting the signature of intermolecular interactions present in the NCI plot of the reduced density gradient versus electron density
journal, January 2017

Carbon capture with ionic liquids: overview and progress
journal, January 2012

Understanding Gas Solubility of Pure Component and Binary Mixtures within Multivalent Ionic Liquids from Molecular Simulations
journal, July 2021

The calculation of small molecular interactions by the differences of separate total energies. Some procedures with reduced errors
journal, October 1970

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010

VMD: Visual molecular dynamics
journal, February 1996