Unraveling and Suppression of Multi‐Directional Planar Slipping and Microcracking in Single‐Crystal Co‐Free, Ni‐Rich Cathodes
Abstract High‐capacity Co‐free Ni‐rich layered oxides are promising cathode materials for lithium‐based batteries, but they suffer from chemo–electro–mechanical instabilities. While single‐crystal morphologies reduce these issues, slipping, and microcracking persist during extended cycling, and the degradation mechanisms remain inadequately understood. Herein, we report on multi‐directional planar slipping and microcracking along the (003) and (100) planes in a single‐crystal LiNi 0.75 Mn 0.25 O 2 (LNM) cathode. According to the Darken–Gurry theory and formation energy in LNM, magnesium (Mg 2+ ) has been selected as the best pillaring element to strengthen the structural integrity and improve cycling stability. Notably, Li 0.99 Mg 0.01 Ni 0.75 Mn 0.25 O 2 (LMNM) achieves a capacity retention of 91% after 1000 cycles at 4.3 V operation against graphite by alleviating instability issues. We systematically unravel the pillaring effect, for the first time, from the quantum scale to the lattice level and from the microscale to the macroscopic level of the cathode particles, providing an in‐depth understanding of chemo–electro–mechanical degradation.
Authors
- Wengao Zhao (ORCID: https://orcid.org/0000-0003-0868-8404)
- Xinming Fan (ORCID: https://orcid.org/0000-0002-4168-6366)
- Zhongdong Peng (ORCID: https://orcid.org/0000-0002-9531-0305)
- Xiaobo Ji (ORCID: https://orcid.org/0000-0002-5405-7913)
- Torsten Brezesinski (ORCID: https://orcid.org/0000-0002-4336-263X)
- Xueyi Guo (ORCID: https://orcid.org/0000-0003-0660-3024)
- Qiuming Yan
- Fucheng Ren (ORCID: https://orcid.org/0000-0001-7078-6238)
- Ke Du (ORCID: https://orcid.org/0000-0002-2216-1046)
- Yuming Shu
- Di Chen (ORCID: https://orcid.org/0000-0002-2187-9240)
- Yong Yang (ORCID: https://orcid.org/0000-0002-9928-7165)
- Hongyi Chen (ORCID: https://orcid.org/0000-0001-5529-2942)
- Jing Lin (ORCID: https://orcid.org/0000-0002-6403-4803)
- Huinan Yu
- Guorong Hu
- Jiangnan Huang
- Hanghang Lei
- Yanbing Cao (ORCID: https://orcid.org/0000-0001-5984-6973)
Institutions
- Karlsruhe Institute of Technology (DE)
- Central South University (CN)
- Xiamen University (CN)
- Institute of Nanotechnology (GB)
- Lanzhou City University (CN)
- Lanzhou University (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- Angewandte Chemie
- Published
- 2025-08-18
- DOI
- https://doi.org/10.1002/ange.202512232
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- National Natural Science Foundation of China
- National Key Research and Development Program of China