Optimized 4‐V Spinel Cathode Material with High Energy Density for Li‐Ion Cells Operating at 60 °C

Spinel cathodes comprising 16‐μm, AlPO₄‐coated Li_1.09Mn_1.83Al_0.08O₄ with a high energy density of 1.2 W h cm^‐3 are synthesized via a conventional solid‐state reaction using MnO₂ and Li₂CO₃ at 770 °C for 10 h and using a solution‐based coating method in bulk scale (>20 kg). The cathodes are coated by aluminum phosphate at a thickness of <10 nm. The coated cathodes exhibit a first discharge capacity of 108 mA·h g^‐1 and a coulombic efficiency of >99.8%, and their capacity retention is 78% after 200 cycles at a 0.5C rate in a Li‐ion cell under 60 °C. More importantly, a Li‐ion cell containing the coated cathode does not exhibit a swelling problem after 200 cycles at 60 °C. Transmission and scanning electron microscopy suggest that the uniformly distributed AlPO₄ coating and the possible formation of a solid solution phase along the surface play key roles in enhancing the electrochemical performance of the LiMn₂O₄ spinel at 60 °C.