Rui Xu, Xue Liu, Yi Wang, Jean-Jacques Gaumet, Chaojiang Niu, Wen Luo
Layered cathodes (LiNixCoyMnzO2, NCM) have emerged as critical materials for batteries and energy storage fields by virtue of their high energy density. However, NCM materials undergo rapid performance degradation and severe capacity fading under harsh conditions of long-term cycling and high voltage. Currently, research regarding spent NCM materials mainly concentrates on failure analysis and modification processes at the macroscopic scale. Nevertheless, the failure mechanisms of NCM, the intrinsic processes during repair and modification, and the fundamental origins of performance improvement are generally embedded in structural evolution at the nanoscale or even atomic scale. This review first discusses the failure mechanisms of NCM. Particularly, the main content focuses on lattice distortion and layered structural instability at the lattice level, migration of nanoscale species together with performance degradation induced by side reactions at the interface level, and generation of nanocracks at the particle level. Moreover, this paper reviews the characterization methods applied at the nanometer scale, and two modification strategies are summarized, namely nanoscale coating and elemental doping. It is expected to provide theoretical references and technical insights for constructing efficient and controllable targeted modification strategies of layered NCM cathodes and developing high-performance ternary cathode materials.