Pure ionic liquid electrolytes compatible with a graphitized carbon negative electrode in rechargeable lithium-ion batteries

Ambient temperature ionic liquids composed of bis(fluorosulfonyl)imide (FSI) as an anion and 1-ethyl-3-methylimidazolium (EMI) or N-methyl-N-propylpyrrolidinium (P-13) as a cation have the following desirable physicochemical properties, particularly for a battery electrolyte: a high ionic conductivity, low viscosity, and a low melting point. While an irreversible cationic intercalation into graphene interlayers at ca. 0.5 V versus Li/Li+ has been a significant and common problem with usual ionic liquids, we found that ionic liquids containing FSI with the Li cation can prevent such an irreversible reaction and provide reversible Li intercalation into graphene interlayers. Our experimental results found the reversible capacity of a graphite negative electrode, in a half-cell with EMI-FSI containing the Li cation as an electrolyte, to be a stable value of approximately 360 mAh g−1 during 30 cycles at a charge/discharge rate of 0.2 C, The present paper may be the first report that a “pure” ionic liquid can provide a stable, reversible capacity for a graphitized negative electrode at an ambient temperature without any additives or solvents when an appropriate counter anion, e.g., FSI, is selected.