1i-Lab, CAS Center for Excellence in Nanoscience, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences (CAS), Suzhou 215123, China 2In Situ Center for Physical Sciences, School of Chemistry and Chemical Engineering, Shanghai Jiaotong University, Shanghai 200240, China
Abstract:Ni-rich layered oxide cathode materials, such as LiNi$_{0.83}$Co$_{0.12}$Mn$_{0.05}$O$_{2}$ (NCM811), exhibit high specific capacity and low cost, and become cathode material preference of high-energy-density Li-ion batteries. However, these cathode materials are not stable and will form Li-poor reconstructed layers and alkaline compounds (Li$_{2}$CO$_{3}$, LiOH) on the surface during the storage and processing in humid air, resulting in serious deterioration of electrochemical properties. During the past two decades, the consensus on the surface instability mechanism during humid air storage has not been reached. The main controversy focuses on the unstable octahedron mechanism and the Li/H exchange mechanism. Herein, we investigate the instability mechanism in the humid air by conducting scanning electronic microscopy, scanning transmission electron microscopy, and x-ray photoelectron spectroscopy analysis on NCM811 samples stored in designed atmospheres, etc., and realize that the surface instability of the NCM811 during storage should be mainly originated from Li/H exchange when it contacts with moisture.