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

• 成果类型: Article
• 署名作者: Han, Qiang; Yu, Haifeng; Cai, Lele; Chen, Ling; Li, Chunzhong; Jiang, Hao
• 署名单位: East China University of Science & Technology; East China University of Science & Technology
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-10053
• DOI: 10.1073/pnas.2317282121
• 发表日期: 2024-03-05
• 关键词: layered oxide cathodes; origin

摘要

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 LiNi0.83Co0.12Mn0.05O2 as an example, an optimal particle size of 3.7 mu m 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.