Surface Engineering via Rare Earth Oxide Composite Coating to Enhance the High-Voltage Stability of the LiCoO2 Cathode.

Abstract

The commercial application of high-voltage LiCoO₂ (LCO) faces significant challenges due to rapid capacity decay, primarily attributed to an unstable interface and structure at deeply delithiated states. Herein, a unique rare earth oxide composite coating comprising La₂O₃, Y₂O₃, and LaYO₃ has been prepared to stabilize LCO at high voltage. The synergistic effect between these rare earth oxides significantly reinforces the protective capabilities of the coating, effectively enhancing the interfacial/structural stability of LCO. When tested at 4.6 V, the coated LCO exhibits an excellent capacity retention of 94.4% after 300 cycles at 1 C. Even after an ultralong charge/discharge test of 700 cycles at 2 C, the coated LCO retains 85.2% of its initial specific capacity, which significantly outperforms the uncoated LCO (6.3%). Moreover, the coated LCO shows enhanced cycling performance at a high temperature of 45 °C, owing to the outstanding thermal stability of the La-Y-O composite. Additionally, the superior cycling stability of the coated LCO at 4.7 V, compared to the uncoated LCO, demonstrated the promising potential of the La-Y-O composite coating in improving electrochemical performance of LCO at higher cutoff voltages. These findings highlight an efficacious strategy to enhance the interfacial/structural stability of high-voltage LCO using rare earth oxides.