Super‐Reversible CuF₂ Cathodes Enabled by Cu²⁺‐Coordinated Alginate

Abstract

Copper fluoride (CuF₂ ) has the highest energy density among all metal fluoride cathodes owing to its high theoretical potential (3.55 V) and high capacity (528 mAh g^-1 ). However, CuF₂ can only survive for less than five cycles, mainly due to serious Cu-ion dissolution during charge/discharge cycles. Herein, copper dissolution is successfully suppressed by forming Cu²⁺ -coordinated sodium alginate (Cu-SA) on the surface of CuF₂ particles during the electrode fabrication process, by using water as a slurry solvent and sodium alginate (SA) as a binder. The trace dissolved Cu²⁺ in water from CuF₂ can in situ cross-link with SA binder forming a conformal Cu-SA layer on CuF₂ surface. After water evaporation during the electrode dry process, the Cu-SA layer is Li-ion conductor but Cu²⁺ insulator, which can effectively suppress the dissolution of Cu-ions in the organic 4 m LiClO₄ /ethylene carbonate/propylene carbonate electrolyte, enhancing the reversibility of CuF₂ . CuF₂ electrode with SA binder delivers a reversible capacity of 420.4 mAh g^-1 after 50 cycles at 0.05 C, reaching an energy density of 1009.1 Wh kg^-1 . Cu²⁺ cross-link polymer coating on CuF₂ opens the door for stabilizing the high-energy and low-cost CuF₂ cathode for next-generation Li-ion batteries.