Publication date: 10th April 2024
The development of high-energy-density batteries with lithium (de-)intercalation reaction is one of the most promising solutions to realize electric vehicles and power storage system applications with long-term stability. In this study, anti-fluorite structured Li5+xFe1-xMnxO4 was synthesized by a solid-state reaction, and lithium intercalation properties were characterized by electrochemical and structural investigations.
A mixed phase of the Li5FeO4-type and Li6MnO4-type structure was obtained for x < 0.6 composition. A new phase with the Li6MnO4-type structure was formed at x = 0.4, and a single phase with Li6MnO4-type structure was obtained in the range between 0.6 and 1.0 composition. The particle size of the synthesized samples was about 50 µm, which is quite large compared with conventional cathode materials for lithium batteries. The as-prepared Li5.6Fe0.4Mn0.6O4 exhibited first charge and discharge capacities of 680 and 300 mAh/g, respectively, with a large irreversible capacity of 380 mAh/g (coulombic efficiency = 44%). This indicates that the new iron-manganese composition with antifluorite-type structure is lithium insertion/extraction-active although a large irreversible electrode reaction was observed.
To improve the charge-discharge performance of the prepared sample, the electrode fabrication process was changed as shown in the experimental section. The ball milling process was introduced to decrease the particle size and compensate for homogeneous electronic conductivity in the composite electrode. Charge-discharge measurements showed that the first discharge capacity of the Li5.6Fe0.4Mn0.6O4 (x = 0.6) electrode treated by ball-milling was 450 mAh/g. The coulombic efficiency was 60%. A reversible reaction continued to proceed with ca. 200 mAh/g after the following cycles. A new iron-manganese system with an anti-fluorite structure could become a potential for high-capacity cathode material.
This work was financially supported by Tokuyama Science Foundation and Nippon Sheet Glass Foundation for Materials Science and Engineering.
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