Insights into Capacity Fading Mechanism and Coating Modification of High-Nickel Cathodes in Lithium-Ion Batteries

Developments in electric vehicles and mobile electronic devices are promoting the demand for lithium-ion batteries with higher capacity and longer lifetime. The performances of lithium-ion batteries are crucially affected by cathode materials, among which ternary cathode materials are the most competitive option with the advantages of high capacity, safety, and cost-effectiveness. However, although high-nickel ternary cathode materials can achieve relatively high specific capacity, they generally have unsatisfactory stability during long-term cycling. In this study, the microscopic mechanisms of the cathode failure and the principle of coating modification in lithium-ion batteries have been comprehensively examined. It has been revealed that the irreversible capacity fading is mainly attributed to the interface chemical reaction, which reduces the transition-metal valence states and generates undesired disordered rock-salt phases. This structural phase transformation at the interface induces the dissolution of transition metals and results in irreversible capacity loss of the cathode. To restrain the occurrence of this process, a LiNbO3 coating-modified single-crystal LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode material has been prepared. The electrochemical properties as well as the microstructural evolution of the cathode–electrolyte interface during cycling of both the uncoated and coated samples have been comprehensively characterized and compared through impedance spectroscopy testing, SEM-EDX, STEM, and EELS characterization. Additionally, molecular dynamics simulation results confirmed that LiNbO3 coating can effectively inhibit the dissolution of transition metals while providing stable lithium-ion channels. The experimental results also indicate that the coating modification can effectively improve the cycling stability of the NCM811, with the capacity retention rate for 500 cycles increasing from 19% to 70%. This study is helpful to deepen the understanding of the capacity fading mechanisms, and the coating method is effective at maintaining the structural stability and improving the cycle life of lithium-ion batteries.