Novel Na+ Ion Diffusion Mechanism in Mixed Organic–Inorganic Ionic Liquid Electrolyte Leading to High Na+ Transference Number and Stable, High Rate Electrochemical Cycling of Sodium Cells.

Abstract

Ambient temperature sodium batteries hold the promise of a new generation of high energy density, low-cost energy storage technologies. Particularly challenging in sodium electrochemistry is achieving high stability at high charge/discharge rates. We report here mixtures of inorganic/organic cation fluorosulfonamide (FSI) ionic liquids that exhibit unexpectedly high Na+ transference numbers due to a structural diffusion mechanism not previously observed in this type of electrolyte. The electrolyte can therefore support high current density cycling of sodium. We investigate the effect of NaFSI salt concentration in methylpropylpyrrolidinium (C3mpyr) FSI ionic liquid (IL) on the reversible plating and dissolution of sodium metal, both on a copper electrode and in a symmetric Na/Na metal cell. NaFSI is highly soluble in the IL allowing the preparation of mixtures that contain very high Na contents, greater than 3.2 mol/kg (50 mol %) at room temperature. Despite the fact that overall ion diffusivity decreases...