Improved Capacity Retention for a Disordered Rocksalt Cathode via Solvate Ionic Liquid Electrolytes

Abstract

Lithium-rich disordered rocksalts (DRX) are a promising class of cathode materials for high-energy lithium ion batteries (LIBs) and lithium metal batteries (LMBs) due to the high initial specific capacities (>200 mAh g−1) as well as flexible chemical composition. However, challenges concerning severe capacity fade and voltage decay upon cycling at high cut-off voltages are still to be overcome. Moreover, state-of-the-art carbonate-based electrolytes can be decomposed by reactive oxygen species released by DRX materials during cycling. In this work, the electrochemical performance of Li1.25Fe0.5Nb0.25O2 (LFNO) || Li LMB and LFNO || graphite LIB cells is compared for a conventional, carbonate-based electrolyte and the solvate ionic liquid (SIL) [Li(G3)][TFSI] (G3: triethyleneglycoldimethylether). Cycle life is notably improved by the chemically more stable ionic liquid electrolyte, as the anionic redox activity of LFNO is prolonged compared to the carbonate-based cells. This work represents an important step toward an improved cycle life of DRX cathodes.