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Title: Solvents Polarity Governs Ion Interactions and Transport in a Solvated Room Temperature Ionic Liquid

We explore the influence of the solvent dipole moment on cation anion interactions and transport in 1-butyl-3-methyl-imidazolium bis-(trifluoromethylsulfonyl), [BMIM+][Tf2N ]. Free energy profiles derived from atomistic molecular dynamics (MD) simulations show a correlation of the cation anion separation and the equilibrium depth of the potential of mean force with the dipole moment of the solvent. Correlations of the ion diffusivity with the dipole moment and the concentration of the solvent were further demonstrated by classical MD simulations. Quasi-elastic neutron scattering experiments with deuterated solvents reveal a complex picture of nanophase separation into the ionic liquid-rich and solvent-rich phases. The experiment corroborates the trend of concentration- and dipole moment-dependent enhancement of ion mobility by the solvent, as suggested by the simulations. Despite the considerable structural complexity of ionic liquid solvent mixtures, we can rationalize and generalize the trends governing ionic transport in these complex electrolytes.
Authors:
 [1] ;  [2] ;  [3] ;  [3] ;  [4] ;  [3] ;  [2] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Drexel Univ., Philadelphia, PA (United States)
  3. Vanderbilt Univ., Nashville, TN (United States)
  4. Univ. of California, Riverside, CA (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
OSTI Identifier:
1337040

Osti, Naresh C, Van Aken, Katherine, Thompson, Matthew W, Tiet, Felix, Jiang, Dr. De-en, Cummings, Peter, Gogotsi, Yury G., and Mamontov, Eugene. Solvents Polarity Governs Ion Interactions and Transport in a Solvated Room Temperature Ionic Liquid. United States: N. p., Web. doi:10.1021/acs.jpclett.6b02587.
Osti, Naresh C, Van Aken, Katherine, Thompson, Matthew W, Tiet, Felix, Jiang, Dr. De-en, Cummings, Peter, Gogotsi, Yury G., & Mamontov, Eugene. Solvents Polarity Governs Ion Interactions and Transport in a Solvated Room Temperature Ionic Liquid. United States. doi:10.1021/acs.jpclett.6b02587.
Osti, Naresh C, Van Aken, Katherine, Thompson, Matthew W, Tiet, Felix, Jiang, Dr. De-en, Cummings, Peter, Gogotsi, Yury G., and Mamontov, Eugene. 2016. "Solvents Polarity Governs Ion Interactions and Transport in a Solvated Room Temperature Ionic Liquid". United States. doi:10.1021/acs.jpclett.6b02587. https://www.osti.gov/servlets/purl/1337040.
@article{osti_1337040,
title = {Solvents Polarity Governs Ion Interactions and Transport in a Solvated Room Temperature Ionic Liquid},
author = {Osti, Naresh C and Van Aken, Katherine and Thompson, Matthew W and Tiet, Felix and Jiang, Dr. De-en and Cummings, Peter and Gogotsi, Yury G. and Mamontov, Eugene},
abstractNote = {We explore the influence of the solvent dipole moment on cation anion interactions and transport in 1-butyl-3-methyl-imidazolium bis-(trifluoromethylsulfonyl), [BMIM+][Tf2N ]. Free energy profiles derived from atomistic molecular dynamics (MD) simulations show a correlation of the cation anion separation and the equilibrium depth of the potential of mean force with the dipole moment of the solvent. Correlations of the ion diffusivity with the dipole moment and the concentration of the solvent were further demonstrated by classical MD simulations. Quasi-elastic neutron scattering experiments with deuterated solvents reveal a complex picture of nanophase separation into the ionic liquid-rich and solvent-rich phases. The experiment corroborates the trend of concentration- and dipole moment-dependent enhancement of ion mobility by the solvent, as suggested by the simulations. Despite the considerable structural complexity of ionic liquid solvent mixtures, we can rationalize and generalize the trends governing ionic transport in these complex electrolytes.},
doi = {10.1021/acs.jpclett.6b02587},
journal = {Journal of Physical Chemistry Letters},
number = ,
volume = 8,
place = {United States},
year = {2016},
month = {12}
}