Does single-crystallization a feasible direction for designing Li-rich layered cathodes?

Abstract

Although the synthesis technology of popular single-crystal electrode materials is mature, the large enough, greatly dispersed Li-rich single-crystal cathodes have been rarely reported. In this study, we overcome the challenge of elevated Mn-O breaking activation energy so that achieve micro-sized (∼3 μm) single-crystal Mn-Li-rich particles with extreme dispersity by regulating Li content and high temperature residence time step by step. However, the modified parameters during the sintering process severely intensify the Li/Ni mixing, leading to unavoidable dynamical hysteresis and structural damage. In addition, the long-range diffusion pathway in single-crystal Li-rich grains not only limits the effective Li⁺ transfer but also significantly weakens the kinetics of anionic redox. Hence, whether the single-crystal strategy is seriously applicable to Mn-based Li-rich cathodes remains a matter of debate, with promising outlets focusing on the enhancement of the dynamics in Li-rich cathodes.