Ternary metal fluorides as high-energy cathodes with low cycling hysteresis

Abstract

Transition metal fluorides are an appealing alternative to conventional intercalation compounds for use as cathodes in next-generation lithium batteries due to their extremely high capacity (3–4 times greater than the current state-of-the-art). However, issues related to reversibility, energy efficiency and kinetics prevent their practical application. Here we report on the synthesis, structural and electrochemical properties of ternary metal fluorides (M 1yM 21-yFx: M 1, M 2=Fe, Cu), which may overcome these issues. By substituting Cu into the Fe lattice, forming the solid–solution CuyFe 1-yF 2, reversible Cu and Fe redox reactions are achieved with surprisingly small hysteresis (<150 mV). This finding indicates that cation substitution may provide a new avenue for tailoring key electrochemical properties of conversion electrodes. Although the reversible capacity of Cu conversion fades rapidly, likely due to Cu+ dissolution, the low hysteresis and high energy suggest that a Cu-based fluoride cathode remains an intriguing candidate for rechargeable lithium batteries.