Dual-Element-Modified Single-Crystal LiNi0.6Co0.2Mn0.2O2 as a Highly Stable Cathode for Lithium-Ion Batteries.

Single-crystalline LiNi0.6Co0.2Mn0.2O2 cathodes have received great attention due to their high discharge capacity and better electrochemical performance. However, the single-crystal materials are suffering from severe lattice distortion and electrode/electrolyte interface side reactions when cycling at high voltage. Herein, a unique single-crystal LiNi0.6Co0.2Mn0.2O2 with Al and Zr doping in the bulk and a self-formed coating layer of Li2ZrO3 in the surface has been constructed by a facile strategy. The optimized cathode material exhibits excellent structural stability and cycling performance at room/elevated temperatures after long-term cycling. Specifically, even after 100 cycles (1C, 3.0-4.4 V) at 50 °C, the capacity retention for the Al and Zr co-doped sample reaches 92.1%, which is much higher than those of the single Al-doped (85.4%), single Zr-doped (87.1%), and bare samples (76.3%). The characterization results and first-principles calculations reveal that the excellent electrochemical properties are attributed to the stable structure and interface, in which the Al and Zr co-doping hinders cation mixing and suppresses detrimental phase transformations to reduce internal stress and mitigate microcracks, and the coating layer of Li2ZrO3 can protect the surface and suppress interfacial parasitic reactions. Overall, this work provides important insights into how to simultaneously build a stable bulk structure and interface for the single-crystal NCM cathode via a facile preparation process.