Improving the High-Voltage Li₂FeMn₃O₈ Cathode by Chlorine Doping

High-capacity and high-voltage cathode materials are desirable for high-energy-density lithium ion batteries. Among various cathode materials, Li2FeMn3O8 is attractive due to its high working voltage, low toxicity, and low cost. However, its superior electrochemical properties are significantly limited by the intrinsic defects in the Li2FeMn3O8 cathode, which makes the theoretical working voltage (4.9 V) and capacity (148 mAh/g) hard to reach. In this paper, we demonstrated that Cl doping can effectively increase the capacity and working voltage of the Li2FeMn3O8 cathode. X-ray photoelectron spectroscopy reveals that Cl doping reduced the valence state and increased the electron binding energy in cations and thus increased the voltage and enhanced the capacity of the Li2FeMn3O8 cathode. Our results also indicate that Cl doping can be a promising low-cost method to improve the electrochemical performance of various oxide cathode materials, including LiCoO2 and LiMn2O4.