High-entropy layered cathode structures and their properties based on first-principles calculations

Based on first principles calculations and high-throughput screening methods, three novel layered high entropy oxide structures, namely LiTMuniformO2, LiTMnon-uniform-2O2, and LiTMnon-uniform-1O2 are screened by the doping of Fe, Mn, and Ni elements at the Co site in the cathode LiCoO2. The crystal structure, electronic structure and structural stability of the three structures are calculated. The impact of Li+ deintercalation on the crystal structureand electronic structure during the delithiation process is analyzed. Finally, using the Climbing Image Nudged Elastic Band (CI-NEB) method, the migration energy barriers of Li+ in the three high entropy oxides are calculated. The results show that all three high entropy oxide structures exhibit good electrical conductivity, facilitating electron conduction in the system. Additionally, compared with the LiTMnon-uniform-2O2 and LiTMnon-uniform-1O2, the LiTMuniformO2 exhibits stronger stability and faster ion transport properties. This work provides theoretical guidance for studying cathode materials with high stability and high energy density.