A new model on cation distribution in cation-disordered Li1+xTM1-xO2 cathodes

The search for new materials that could improve the energy density of Li-ion batteries (LIB) is one of today's most challenging issues. Recently, cation-disordered lithium-excess metal oxides have emerged as a promising new class of cathode materials for LIB, due to their high reversible capacities and nice structural stability. However, a full structural model of the Li-transition metal (TM) sharing sublattice and the origin of short range ordering (SRO) of cations requires further investigation. In this work, we put forward a Monte Carlo strategy of building cation-disordered rocksalt material supercell models. The cations of Li1.0Ti0.5Ni0.5O2 (LTNO) are placed at the FCC sublattice sites with the constraint of Pauling's electroneutrality rule, instead of a random way. This constraint causes the Li-Ti and Ni-Ni clustering. Based on this model, we discussed the relationship between the SRO, the local distorting, the theoretical capacity and the order-disorder strengths. A unified understanding of these factors in cation-disordered materials may enable a better design of disordered-electrode materials with high capacity and high energy density.