First-principle study on the structure and stability of LiNi1/3Co1/3Mn1/3O2 doped with metal cations of different valences

To minimize resource and energy consumption during the impurity removal process in industrial battery preparation and waste battery recycling, we conducted a preliminary study on the differential purification of impurity ions: Na+, Mg2+, Al3+. Utilizing the first-principle calculation, we assessed the impact of ions doping LiNi1/3Co1/3Mn1/3O2 on three factors that influence cycle stability: phase stability, structural changes during cycling, and oxygen vacancy formation. The results indicate that Na-doped exhibits a tendency for phase separation and increases structural changes during cycling, making it unsuitable for retention in the final products. On the other hand, Mg-doped and Al-doped demonstrate excellent phase stability, reduce structural changes during cycling due to the preferential oxidation of Co3+, and inhibit oxygen release. From a cycle stability perspective, they are suitable for inclusion in the final products.