Protective Spinel Coating for Li_1.17Ni_0.17Mn_0.50Co_0.17O₂ Cathode for Li-Ion Batteries through Single-Source Precursor...

The Li_1.17Ni_0.17Mn_0.50Co_0.17O₂ Li-rich NMC positive electrode (cathode) for lithium-ion batteries has been coated with nanocrystals of the LiMn_1.5Co_0.5O₄ high-voltage spinel cathode material. The coating was applied through a single-source precursor approach by a deposition of the molecular precursor LiMn_1.5Co_0.5(thd)₅ (thd = 2,2,6,6-tetramethyl-3,5-heptanedionate) dissolved in diethyl ether, followed by thermal decomposition at 400 °C inair resulting in a chemically homogeneous cubic spinel. The structure and chemical composition of the coatings, deposited on the model SiO₂ spheres and Li-rich NMC crystallites, were analyzed using powder X-ray diffraction, electron diffraction, high angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and energy-dispersive X-ray (EDX) mapping. The coated material containing 12 wt.% of spinel demonstrates a significantly improved first cycle Coulombic efficiency of 92% with a high first cycle discharge capacity of 290 mAhg^-1. The coating also improves the capacity and voltage retention monitored over 25 galvanostatic charge-discharge cycles, although a complete suppression of the capacity and voltage fade is not achieved.