Impact of Ni Content on the Electrochemical Performance of the Co-Free, Li and Mn-Rich Layered Cathode Materials

Li and Mn-rich layered cathode (LLC) materials show great potential as the next generation cathode materials because of their high, practical and achievable specific capacity of ~250 mAh/g, thermal stability and lower raw material cost. However, LLC materials suffer from degradation of specific capacity, voltage fading due to phase transformation upon cycling and transition-metal dissolution, which presents a significant barrier for commercialization. Here, we report the effects of Ni content on the electrochemical performance, structural and thermal stability of a series of Co-free, LLC materials (Li1.2NixMn0.8-xO2, x = 0.12, 0.18, 0.24, 0.30 and 0.36) synthesized via a sol-gel method. Our study shows that the structure of the material as well as the electrochemical and thermal stability properties of the LLC materials are strongly dependent on the Ni or Mn content. An increase in the Ni to Mn ratio results in an increase in the average discharge voltage and capacity, as well as improved structural stability but decreased thermal stability.