Single-crystal layered oxides as cathode materials for next-generation lithium-ion batteries

The review addresses potential applications of layered LiNi_<i>x</i>Co_<i>y</i>Mn_<i>z</i>O₂ (<i>x</i> + <i>y</i> + <i>z</i> = 1) oxides in the form of non-agglomerated large-crystalline (single-crystal) particles as cathode materials for lithium-ion batteries (LIBs). A unique feature of this review is integration of fundamental aspects into a unified material design strategy. Correlations between the thermodynamics of crystal facet surface energy, the chemical potentials of lithium and oxygen, and crystal growth kinetics were established for the first time. This enables targeted control of particle morphology depending on the surface composition and synthesis conditions. The chemistry and thermodynamic conditions of defect formation are described in detail, and existing gaps in their crystallographic description are highlighted. In comparison with other studies, the patterns of mechanical degradation of single crystals during long-term cycling were identified, which made it possible to formulate strategies for effective control of the defect structure to fabricate cathodes with high specific capacity and extended cycle life. Methods for investigating the mechanical properties of particles and methodological limitations of these methods are analyzed for the first time. <br> The bibliography includes 308 references.