Enhancing the Electrochemical Performance and Structural Stability of Ni-Rich Layered Cathode Materials via Dual-Site Doping.

Ni-rich layered cathode materials are considered as promising electrode materials for lithium ion batteries due to their high energy density and low cost. However, the low rate performance and poor electrochemical stability hinder the large-scale application of Ni-rich layered cathodes. In this work, both the rate performance and the structural stability of the Ni-rich layered cathode LiNiCoMnO are significantly improved via the dual-site doping of Nb on both lithium and transition-metal sites, as revealed by neutron diffraction results. The dual-site Nb-doped LiNiCoMnO delivers 202.8 mAh·g with a capacity retention of 81% after 200 electrochemical cycles, which is much higher than that of pristine LiNiCoMnO. Moreover, a discharge capacity of 176 mAh·g at 10C rate illustrates its remarkable rate capability. Through in situ X-ray diffraction and electronic transport property measurements, it was demonstrated that the achievement of dual-site doping in the Ni-rich layered cathode can not only suppress the Li/Ni disordering and facilitate the lithium ion transport process but also stabilize the layered structure against local collapse and structural distortion. This work adopts a dual-site-doping approach to enhance the electrochemical performance and structural stability of Ni-rich cathode materials, which could be extended as a universal modification strategy to improve the electrochemical performance of other cathode materials.