Study on electrochemical performance of Al-substitution for different cations in Li-rich Mn-based materials

Abstract Layered Li-rich Mn-based cathode materials have attracted immense interest for using in lithium-ion batteries, owing to their high energy density. However, the severe degradation of cycle and rate performances has impeded the actual commercial application. Herein, Al was selected as doping element to substitute for the metal elements of Li, Ni, Co and Mn in Li1.2Mn0.54Ni0.13Co0.13O2 material to promote electrochemical performances and optimize element proportion. Results indicate that when replacing Li with Al, it displays outstanding initial coulombic efficiency of 80.06%. Besides, Al-substitution for Co shows excellent rate performance of 147.3 mAh g−1 at 5.0 C. Particularly, the replacement of Mn not only shows the highest capacity and voltage retention within the potential range from 2.0 to 4.8 V, but also presents superior capacity retention up to the potential of 5.0 V. Unfortunately, the substitution of Ni displays the worst balanced electrochemical performance among Al-doped materials, which shows lower voltage retention than that of pristine. The reasons why Al-substitution for various cations displays difference on electrochemical performance were discussed from the perspective of migration, dissolution and valence reduction of transition metal ions to the structure evolution in detail. The proposed method and detected action mechanisms can provide guidance on how to optimize materials structure and composition for cathode materials in lithium-ion batteries to obtain electrode materials with excellent comprehensive electrochemical performance.