Retarding the capacity fading and voltage decay of Li-rich Mn-based cathode materials via a compatible layer coating for high-performance lithium-ion batteries

Abstract

Li-rich Mn-based layered oxides have been considered as the most promising cathode candidate for high energy density lithium ion batteries. However, the practical application of Li-rich Mn-based layered oxides is hindered due to the capacity fading and voltage decay accompanied with structure transition from the layered structure to spinel phase during cycling. Herein, a facile surface structure repair via Ce modification is reported. The structural analysis of the bulk and coating layer was carried out using XRD, XPS, SEM and TEM, which confirmed the successful doping of Ce and formation of a Li₂CeO₃ coating on the surface. The modified sample LLO-2 delivers a discharge specific capacity of 263.5 mA h g⁻¹ at 0.1C and capacity retention rate with 88.1% at 0.2C after 100 cycles compared to 250.2 mA h g⁻¹ and 75.6% for the pristine sample. The enhanced performance could be because Ce doping enlarges the lattice parameter, which may contribute to accelerating the Li⁺ diffusion rate. Moreover, the newly formed Li₂CeO₃ coating with oxygen vacancies could inhibit the loss of lattice oxygen and protect the electrode surface by suppressing the attack from the electrolyte. This work provides an effective approach to design Li-rich Mn-based layered oxides with improved electrochemical performance.