Using High-Entropy Configuration Strategy to Design Spinel Lithium Manganate Cathodes with Remarkable Electrochemical...

Owing to its abundant manganese source, high operating voltage, and good ionic diffusivity attributed to its 3D Li-ion diffusion channels. Spinel LiMn₂O₄ is considered a promising low-cost positive electrode material in the context of reducing scarce elements such as cobalt and nickel from advanced lithium-ion batteries. However, the rapid capacity degradation and inadequate rate capabilities induced by the Jahn-Teller distortion and the manganese dissolution have limited the large-scale adoption of spinel LiMn₂O₄ for decades. In this study, LiMn_1.98Mg_0.005Ti_0.005Sb_0.005Ce_0.005O₄ spinel positive electrode material (HE-LMO) with remarkable interfacial structural and cycling stability is developed based on a complex concentrated doping strategy. The initial discharge capacity and capacity retention of the electrode of HE-LMO are 111.51 mAh g^-1 and 90.55% after 500 cycles at 1 C. The as-prepared HE-LMO displays favorable cycling stability, significantly surpassing the pristine sample. Furthermore, theoretical calculations strongly support the above finding. HE-LMO has a higher and more continuous density of states at the Fermi energy level and more robust bonded states of the electrons among the Mn─O atom pairs. This research contributes to the field of high-entropy doping modification and establishes a facile strategy for designing advanced spinel manganese-based lithium-ion batteries (LIBs).