preprints.org > doi: 10.20944/preprints201909.0254.v1

Preprint Article Version 1 This version is not peer-reviewed

Version 1 : Received: 21 September 2019 / Approved: 22 September 2019 / Online: 22 September 2019 (15:32:13 CEST)

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 cation ions requires further investigation. In this work, we put forward a Monte Carlo strategy of building a cation-disordered rocksalt material supercell model. The cation ions of Li_1.0Ti_0.5Ni_0.5O₂ (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 (the cation short range ordering). Based on this model, we discussed the relationship between the short range ordering, the local distorting, the theoretic 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.

cation-disordered Li-excess cathodes; short range ordering; local distorting; theoretic capacity; order-disorder strength