Revisiting OPLS Force Field Parameters for Ionic Liquid Simulations

Brian Doherty, Xiang Zhong, Symon Gathiaka, Bin Li, Orlando Acevedo

Research output: Contribution to journalArticle

18 Citations (Scopus)

Abstract

Our OPLS-2009IL force field parameters (J. Chem. Theory Comput. 2009, 5, 1038-1050) were originally developed and tested on 68 unique ionic liquids featuring the 1-alkyl-3-methylimidazolium [RMIM], N-alkylpyridinium [RPyr], and choline cations. Experimental validation was limited to densities and a few, largely conflicting, heat of vaporization (ΔHvap) values reported in the literature at the time. Owing to the use of Monte Carlo as our sampling technique, it was also not possible to investigate the reproduction of dynamics. The [RMIM] OPLS-2009IL parameters have been revisited in this work and adapted for use in molecular dynamics (MD) simulations. In addition, new OPLS-AA parameters have been developed for multiple anions, i.e., AlCl4-, BF4-, Br-, Cl-, NO3-, PF6-, acetate, benzoate bis(pentafluoroethylsulfonyl)amide, bis(trifluoroethylsulfonyl)amide, dicyanamide, formate, methylsulfate, perchlorate, propanoate, thiocyanate, tricyanomethanide, and trifluoromethanesulfonate. The computed solvent densities, heats of vaporization, viscosities, diffusion coefficients, heat capacities, surface tensions, and other relevant solvent data compared favorably with experiment. A charge scaling of ±0.8 e was also investigated as a means to mimic polarization and charge transfer effects. The 0.8-scaling led to significant improvements for ΔHvap, surface tension, and self-diffusivity; however, a concern when scaling charges is the potential degradation of local intermolecular interactions at short ranges. Radial distribution functions (RDFs) were used to examine cation-anion interactions when employing 0.8∗OPLS-2009IL and the scaled force field accurately reproduced RDFs from ab initio MD simulations.

Original languageEnglish (US)
Pages (from-to)6131-6135
Number of pages5
JournalJournal of Chemical Theory and Computation
Volume13
Issue number12
DOIs
StatePublished - Dec 12 2017

Fingerprint

heat of vaporization
Ionic Liquids
Vaporization
Ionic liquids
field theory (physics)
formic acid
Amides
scaling
radial distribution
amides
Distribution functions
Anions
Surface tension
Molecular dynamics
Cations
interfacial tension
Negative ions
liquids
Positive ions
distribution functions

ASJC Scopus subject areas

  • Computer Science Applications
  • Physical and Theoretical Chemistry

Cite this

Revisiting OPLS Force Field Parameters for Ionic Liquid Simulations. / Doherty, Brian; Zhong, Xiang; Gathiaka, Symon; Li, Bin; Acevedo, Orlando.

In: Journal of Chemical Theory and Computation, Vol. 13, No. 12, 12.12.2017, p. 6131-6135.

Research output: Contribution to journalArticle

Doherty, Brian ; Zhong, Xiang ; Gathiaka, Symon ; Li, Bin ; Acevedo, Orlando. / Revisiting OPLS Force Field Parameters for Ionic Liquid Simulations. In: Journal of Chemical Theory and Computation. 2017 ; Vol. 13, No. 12. pp. 6131-6135.
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AB - Our OPLS-2009IL force field parameters (J. Chem. Theory Comput. 2009, 5, 1038-1050) were originally developed and tested on 68 unique ionic liquids featuring the 1-alkyl-3-methylimidazolium [RMIM], N-alkylpyridinium [RPyr], and choline cations. Experimental validation was limited to densities and a few, largely conflicting, heat of vaporization (ΔHvap) values reported in the literature at the time. Owing to the use of Monte Carlo as our sampling technique, it was also not possible to investigate the reproduction of dynamics. The [RMIM] OPLS-2009IL parameters have been revisited in this work and adapted for use in molecular dynamics (MD) simulations. In addition, new OPLS-AA parameters have been developed for multiple anions, i.e., AlCl4-, BF4-, Br-, Cl-, NO3-, PF6-, acetate, benzoate bis(pentafluoroethylsulfonyl)amide, bis(trifluoroethylsulfonyl)amide, dicyanamide, formate, methylsulfate, perchlorate, propanoate, thiocyanate, tricyanomethanide, and trifluoromethanesulfonate. The computed solvent densities, heats of vaporization, viscosities, diffusion coefficients, heat capacities, surface tensions, and other relevant solvent data compared favorably with experiment. A charge scaling of ±0.8 e was also investigated as a means to mimic polarization and charge transfer effects. The 0.8-scaling led to significant improvements for ΔHvap, surface tension, and self-diffusivity; however, a concern when scaling charges is the potential degradation of local intermolecular interactions at short ranges. Radial distribution functions (RDFs) were used to examine cation-anion interactions when employing 0.8∗OPLS-2009IL and the scaled force field accurately reproduced RDFs from ab initio MD simulations.

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