Unique insights into the design of low-strain single-crystalline Ni-rich cathodes with superior cycling stability.

ABSTRACT: Micro-sized single-crystalline Ni-rich cathodes are emerging as prominent candidates owing to their larger compact density and higher safety compared with poly-crystalline counterparts, yet the uneven stress distribution and lattice oxygen loss result in the intragranular crack generation and planar gliding. Herein, taking LiNi_0.83Co_0.12Mn_0.05O₂ as an example, an optimal particle size of 3.7 µm is predicted by simulating the stress distributions at various states of charge and their relationship with fracture free-energy, and then, the fitted curves of particle size with calcination temperature and time are further built, which guides the successful synthesis of target-sized particles (m-NCM83) with highly ordered layered structure by a unique high-temperature short-duration pulse lithiation strategy. The m-NCM83 significantly reduces strain energy, Li/O loss, and cationic mixing, thereby inhibiting crack formation, planar gliding, and surface degradation. Accordingly, the m-NCM83 exhibits superior cycling stability with highly structural integrity and dual-doped m-NCM83 further shows excellent 88.1% capacity retention.

SUBMITTER: Han Q 

PROVIDER: S-EPMC10927491 | biostudies-literature | 2024 Mar

REPOSITORIES: biostudies-literature