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

Authors: Baodan Zhang, Yiming Zhang, Haichuan Wu, Linhui Zeng, Xiaotong Wang, Hui Liu, Xiaohong Wu, Jianken Chen, Haitang Zhang, Yawen Yan, Yonglin Tang, Huan Huang, Lirong Zheng, Qiaobao Zhang, Qingshui Xie, Dong-Liang Peng, Chao Li*, Yu Qiao*, Shi-Gang Sun

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.

Full-Link: https://www.sciencedirect.com/science/article/pii/S2405829723003045