A joint theoretical/experimental study of the structure, dynamics, and Li+ transport in bis([tri]fluoro[methane]sulfonyl)imide [T]FSI-based ionic liquids

Abstract

The structure and dynamics of N-butyl-N-methyl pyrrolidinium+ bis([tri]fluoro[methane]sulfonyl)imide- (PYR14+-[T]FSI-) ionic liquids doped with Li(T)FSI are investigated by combining experimental measurements to molecular dynamics simulations. The polarizable force field calculations indicate that the lithium cations are coordinated by (T)FSI anion oxygens forming lithium adducts stabilized over a large temperature range by strong Li-O bonds. Lithium aggregation is found to be negligible at the doping level considered here (10% mole fraction), and Li+ diffusion occurs primarily by exchanging the (T)FSI anions in their first coordination shell. The resulting calculated transport properties are in good agreement with the corresponding nuclear magnetic resonance data. © 2013 AIP Publishing LLC.