An oxalate cathode for lithium ion batteries with combined cationic and polyanionic redox

The growing demand for advanced lithium-ion batteries calls for the continued development of high-performance positive electrode materials. Polyoxyanion compounds are receiving considerable interest as alternative cathodes to conventional oxides due to their advantages in cost, safety and environmental friendliness. However, polyanionic cathodes reported so far rely heavily upon transition-metal redox reactions for lithium transfer. Here we show a polyanionic insertion material, Li2Fe(C2O4)(2), in which in addition to iron redox activity, the oxalate group itself also shows redox behavior enabling reversible charge/discharge and high capacity without gas evolution. The current study gives oxalate a role as a family of cathode materials and suggests a direction for the identification and design of electrode materials with polyanionic frameworks.