The significant growth rate of the electric vehicles (EVs) market, powered by rechargeable lithium-ion batteries (LIBs), in favor over of the internal combustion engine (ICE), represents an opportunity to massively reduce CO₂ emissions and help limit global warming issues. EVs should have a similar performance to that of ICE-powered vehicles in terms of fulfilling driving range as well as lifetime of the battery to appeal the potential consumers. However, the driving range of EV’s is limited by the battery performance, which is related to the properties of the cathode material. Therefore, the development of advanced cathodes is needed.

Current state-of-the-art, Li-ion cathodes for EV batteries are derived from layered LiNiO₂ (LNO) by substitution of Ni with other elements such as Mn, Co, and Al – so called LiNi_xMn_yCo_zAl_1-x-y-zO₂ (NMCA). Substitutions are used to offset the inferior structural stability and poor cycle-life performance of typically-produced, high-capacity NMCAs. In this regard, pure LNO has been reported as a baseline material for gauging the improvements, via doping/coating strategies, for the NMCA-class of cathodes. However, for the purposes of a fully understanding the roles of Mn, Co, Al, and other dopants in NMCAs, the development of a truly state-of-the-art, LNO cathode should be accomplished. This presentation will discuss the various parameters affecting the synthesis and performance of LNO and LNO-based oxides, from precursors to final products, and the strategies that have been pursued at Argonne National Laboratory towards the realization of high-performance LNO baselines and derivatives thereof. Their potential applicability to battery applications will be also reviewed.