Combining Surface Holistic Ge Coating and Subsurface Mg Doping to Enhance the Electrochemical Performance of LiNiCoMnO Cathodes.

Nickel-rich layered cathode LiNiCoMnO (NCM811) is the most promising cathode material due to its high specific capacity and lower cost than lithium cobalt oxides. However, NCM811 suffers from structural instability and capacity degradation during charge-discharge cycles. Herein, we report a strategy to construct a conductive network by employing a holistic Ge coating, which interconnects Mg-doped NCM811 particles. Dopant Mg ions, serving as a "pillar" in the Li slab of NCM811, substantially enhance the structural reversibility. The Ge particles are not only coated on the electrode surface but also enter into the electrode pores to form a multidimensional conductive structure, which improves the conductivity of the electrode and slows down the interface side reaction, thus minimizing the irreversible loss of NCM811 upon long cycling. The modified NCM811 electrode delivers a high discharge capacity (∼204 mAh g at 0.1C), excellent rate performance (∼155 mAh g at 10C), and high capacity retention (83% after 200 cycles) even at 4.4 V. Additionally, a cylindrical full battery with graphite/modified NCM811 undergoes 1000 cycles with 86% capacity retention at 2C.