Exploiting anion and cation redox chemistry in lithium-rich perovskite oxalate: a novel next-generation Li/Na-ion battery electrode

Abstract

The fundamental understanding of electrochemical reaction kinetics for lithium/sodium-ion batteries (LIBs & NIBs) is a significant criterion for advancing new-generation electrode materials. Herein, we demonstrate a novel lithium-rich perovskite oxalate KLi₃Fe(C₂O₄)₃ (KLFC) cathode with the combination of cation and anion redox delivering discharge capacities of 86 and 99 mA h g⁻¹ after 100 cycles for a LIB and NIB, respectively, with good cyclability. Experimental Raman spectroscopy analysis combined with DFT calculations of charged/discharged samples illustrate the oxalate anion redox activity. Further, first-principles calculations of the partial density of states and Bader charges analysis have also characterised the redox behaviour and charge transfer during the potassium extraction processes.