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Lithium cobalt oxide (LiCoO 2 ), which has been successfully applied in commercial lithium-ion batteries for portable devices, possesses a theoretical specific capacity of 274 mAh g −1 . However, its actual capacity is only half of the theoretical specific capacity, because the charging voltage is restricted below 4.2 V. If a higher charging voltage is applied, an irreversible phase transition of LiCoO 2  during delithiation would occur, resulting in severe capacity fading. Therefore, it is essential to investigate the electrochemically driven phase transition of LiCoO 2  cathode material to approach its theoretical capacity. In this work, it was observed that LiCoO 2  partially degraded to Co 3 O 4  after 150 charging-discharging cycles. From the perspective of crystallography, the conventional cell of LiCoO 2  was rebuilt to an orthonormal coordinate, and the transition path from layered LiCoO 2  to cubic Co 3 O 4  proposed. The theoretical analysis indicated that the electrochemically driven phase transition from LiCoO 2  to Co 3 O 4  underwent several stages. Based on this, an experimental verification was made by doping LiCoO 2  with Al, In, Mg, and Zr, respectively. The doped samples theoretically predicted behavior. The findings in this study provide insights into the electrochemically driven phase transition in LiCoO 2 , and the phase transition can be eliminated to improve the capacity of LiCoO 2  to its theoretical value.

Electrochemically Driven Phase Transition in LiCoO2 Cathode