High energy density and durable pouch-cell graphite-based dual ion battery using concentrated hybrid electrolytes

Abstract

Graphite-based dual-ion batteries (GDIBs) represent a promising battery concept for large-scale energy storage on account of low cost, high working voltage, and sustainability. The electrolyte concentration plays a critical role in determining the energy density and cycle life of GDIBs. However, the concentrated electrolytes show low Lithium ions (Li+) transport kinetics, reducing their intercalation and solid electrolyte interface (SEI) formation abilities. Moreover, the GDIBs in the high cut-off voltage suffer from electrolyte degradation, and corrosion of the current collector. Herein, we report a highly concentrated electrolyte formulation based on hybrid lithium hexafluorophosphate (LiPF6) and lithium bis(fluorosulfonyl)imide (LiFSI) salts with a super-wide electrochemical stability window (6 V) and the ability to form SEI and passivation layer on graphite anode and current collector, respectively. By regulating the concentrated LiFSI electrolyte with LiPF6 and solvent additive, the coulombic efficiency of the graphite cathode can be further improved to ∼98%. As a result, GDIB pouch cell exhibits a capacity of 21 mAh g−1 (cell level) at 50 mA g−1, and 98.2% capacity retention after 300 cycles. The resultant battery offers an energy density of 90.3 Wh kg−1, along with a high energy efficiency of 87% and average discharge voltage of 4.3 V.