Stabilisation of lithiated graphite in an electrolyte based on ionic liquids: an electrochemical and scanning electron microscopy study

• Published in: Carbon (New York) 2005-06, Vol.43 (7), p.1488-1498
• Main Authors: Holzapfel, M., Jost, C., Prodi-Schwab, A., Krumeich, F., Würsig, A., Buqa, H., Novák, P.
• Format: Article
• Language: English
• Subjects: Battery carbon; Cross-disciplinary physics: materials science; rheology; Electrochemical properties; Electrodes; Exact sciences and technology; Fullerenes and related materials; diamonds, graphite; Graphite; Intercalation; Materials science; Physics; Specific materials
• ISSN: 0008-6223; 1873-3891
• DOI: 10.1016/j.carbon.2005.01.030

1-Ethyl-3-methylimidazolium-bis(trifluoromethylsulfonyl)imide (EMI-TFSI) is shown to reversibly permit lithium intercalation into standard TIMREX ® SFG44 graphite when vinylene carbonate (VC) is used in small amounts as additive. The best performance was obtained when 5% of VC was added to a 1 M solution of LiPF 6 in EMI-TFSI. Intercalation of lithium in the SFG44 graphite host was demonstrated over 100 cycles without noticeable capacity fading. The reversible charge capacity was around 350 mA h g −1 and an only small irreversible capacity loss per cycle could be observed. Li 4Ti 5O 12 was used as counter electrode material. Scanning electron microscopy indicates the reduction of the electrolyte without graphite exfoliation in the neat electrolyte and the formation of a passivation film in the case of a VC-containing electrolyte. Other additives that were tested comprise ethylene sulphite and acrylonitrile which show also a positive effect, but a smaller one than vinylene carbonate. LiCoO 2 positive electrodes were cycled in a 1 M solution of LiPF 6 in EMI-TFSI with good charge capacity retention over more than 300 cycles, when Li 4Ti 5O 12 was used as counter electrode. The formation of a passivation film is proven on the LiCoO 2-electrodes, when the electrolyte contained VC, but not in the neat ionic liquid. Finally, the stable cycling of a full cell configuration is proven in this electrolyte system. An ammonium-containing ionic liquid (methyltrioctylammonium-bis(trifluoromethylsulfonyl)-imide, MTO-TFSI) is shown to permit the cycling of both, graphite and lithium cobalt oxide when VC is used as additive in small amounts, but at slightly elevated temperatures.