On the Mechanistic Understanding of First‐Cycle Capacity Loss in Polycrystalline and Single‐Crystal Layered Ni‐Rich Oxide Cathodes for Li‐Ion Batteries

Layered Ni‐rich oxide cathode materials deliver high specific capacities at moderate cutoff potentials and thus are highly sought after for e‐mobility applications. However, considerable discrepancies exist between the charge and discharge capacities that can be achieved in the initial cycle, as well as to the theoretical specific capacity. This article aims to summarize and consolidate recent hypotheses into the underlying mechanisms of first‐cycle capacity loss in Ni‐rich cathodes. We differentiate between losses due to limited lithium diffusivity and those caused by material instabilities and describe their interdependence. Correlations with advanced tailoring strategies (particle size, coating, doping) are discussed. In addition, several strategies are proposed on how to keep first‐cycle irreversibilities at a minimum.