Ultrafast Li/Fluorinated Graphene Primary Batteries with High Energy Density and Power Density

Lithium/fluorinated carbon (Li/CFx) primary batteries have essential applications in consumer electronics and medical and high-power military devices. However, their application is limited due to the difficulty in achieving simultaneous high power density and high energy density in the CFx cathode. The tradeoff between conductivity and fluorine content is the decisive factor. Herein, by rational design, 3D porous fluorinated graphene microspheres (FGS-x) with both high conductivity and a high F/C ratio are successfully synthesized for the first time. FGS-x possesses an F/C ratio as high as 1.03, a nanosheet structure with hierarchical pores, abundant C═C bonds, few inactive C–F2 bonds, and electrochemically active C–F bonds. The beneficial features that can increase discharge capacity, shorten the diffusion length for both ions and electrons, enhance the Li+ intercalation kinetics, and accommodate the volume change are demonstrated. The Li/FGS-1.03 coin cell delivers an unprecedented power density of 71,180.9 W/kg at an ultrahigh rate of 50 C (43.25 A/g), coupled with a high energy density of 830.7 Wh/kg. Remarkably, the Li/FGS-1.03 pouch cell exhibits a record cell-level power density of 12,451.2 W/kg at 20 C. The in-depth investigation by the ex situ method on structural evolution at different discharge depths reveals that the excellent performance benefits from the structural stability and the uniform formation of LiF. The FGS-1.03 cathode also has excellent performance in extreme operating temperatures (0 to 100 °C) and high active material mass loading (4.3 mg/cm2). These results indicate that the engineered fluorinated graphene developed here has great potential in applications requiring both high power density and high energy density.