Investigation of Dynamics in BMIM TFSA Ionic Liquid through Variable Temperature and Pressure NMR Relaxometry and Diffusometry

Pilar, Kartik; Rua, Armando; Suarez, Sophia N.; Mallia, Christopher; Lai, Shen; Jayakody, J. R. P.; Hatcher, Jasmine L.; Wishart, James F.; Greenbaum, Steve

doi:10.1149/2.0301708jes

Investigation of Dynamics in BMIM TFSA Ionic Liquid through Variable Temperature and Pressure NMR Relaxometry and Diffusometry

Journal Article · Thu May 11 00:00:00 EDT 2017 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/2.0301708jes· OSTI ID:1358032

Pilar, Kartik ^[1]; Rua, Armando ^[2]; Suarez, Sophia N. ^[3]; Mallia, Christopher ^[4]; Lai, Shen ^[1]; Jayakody, J. R. P. ^[5]; Hatcher, Jasmine L. ^[6]; Wishart, James F. ^[7]; Greenbaum, Steve ^[1]

Hunter College, New York, NY (United States). Dept. of Physics; CUNY Graduate School, New York, NY (United States)
Hunter College, New York, NY (United States). Dept. of Physics; CUNY Graduate School, New York, NY (United States); Univ. of Puerto Rico, Mayaguez, PR (United States). Dept. of Physics
CUNY Graduate School, New York, NY (United States); Brooklyn College, Brooklyn, NY (United States). Physics Dept.
Hunter College, New York, NY (United States). Dept. of Physics
Univ. of Kelaniya (Sri Lanka). Dept. of Physics
CUNY Graduate School, New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division

A comprehensive variable temperature, pressure and frequency multinuclear (¹H, ²H, and ¹⁹F) magnetic resonance study was undertaken on selectively deuterated 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)amide (BMIM TFSA) ionic liquid isotopologues. This study builds on our earlier investigation of the effects of increasing alkyl chain length on diffusion and dynamics in imidazolium-based TFSA ionic liquids. Fast field cycling ¹H T₁ data revealed multiple modes of motion. Through calculation of diffusion coefficient (D) values and activation energies, the low- and high-field regimes were assigned to the translational and reorientation dynamics respectively. Variable-pressure ²H T₁ measurements reveal site-dependent interactions in the cation with strengths in the order MD₃ > CD₃ > CD₂, indicating dissimilarities in the electric field gradients along the alkyl chain, with the CD₂ sites having the largest gradient. Additionally, the α saturation effect in T₁ vs. P was observed for all three sites, suggesting significant reduction of the short-range rapid reorientational dynamics. This reduction was also deduced from the variable pressure ¹H T₁ data, which showed an approach to saturation for both the methyl and butyl group terminal methyl sites. Pressure-dependent D measurements show independent motions for both cations and anions, with the cations having greater D values over the entire pressure range.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States); Brooklyn College, Brooklyn, NY (United States); Hunter College, New York, NY (United States)

Sponsoring Organization:: Office of Naval Research (ONR) (United States); Professional Staff Congress City Univ. of New York (PSC CUNY) (United States); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Contributing Organization:: CUNY Graduate School, New York, NY (United States); Univ. of Kelaniya (Sri Lanka); Univ. of Puerto Rico, Mayaguez, PR (United States)

Grant/Contract Number:: AC02-98CH10886; SC0012704

OSTI ID:: 1358032

Report Number(s):: BNL--113880-2017-JA; KC0301010

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 8 Vol. 164; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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