Mitigating Surface Irreversible Layer‐To‐Spinel Phase Transition for Stable and Ultrahigh‐Capacity LiCoO <sub>2</sub> Cathodes
Currently, the surface structure collapse issues have long hindered the utilization of ultrahigh-capacity LiCoO<sub>2</sub> (LCO) cathodes. Herein, a dual-optimized LCO (D-LCO) is proposed with a surface rocksalt (RS) phase (10 nm) and a subsurface layered phase reinforced by Al/F doping (>50 nm). Unlike solely surface modifications, subsurface Al/F doping drastically suppresses lattice O<sup>n-</sup> (0<n<2) migration at high states of charge (SOC), preventing the irreversible layer-to-spinel transitions and RS-phase thickening in the near-surface region. Consequently, D-LCO achieves an ultrahigh capacity of 236 mAh g<sup>-1</sup> at 4.6 V versus Li<sup>+</sup>/Li, with 90.3% capacity retention after 200 cycles at 1 C and 81.2% after 1000 cycles at 4 C. This work demonstrates that coordinated subsurface/surface stabilization is essential for unlocking the ultrahigh capacity of layered oxide cathodes.
Authors
- Zirui Lou (ORCID: https://orcid.org/0000-0002-5299-9771)
- Chengkai Yang (ORCID: https://orcid.org/0000-0001-9868-4831)
- Hengyu Ren
- Feng Pan (ORCID: https://orcid.org/0000-0002-1362-4336)
- Qinghe Zhao (ORCID: https://orcid.org/0000-0002-8580-0634)
- Zijian Li (ORCID: https://orcid.org/0000-0002-8212-5282)
- Shengyu Wu
- Wenguang Zhao (ORCID: https://orcid.org/0009-0008-1552-0259)
- Xiaohu Wang (ORCID: https://orcid.org/0000-0001-9062-5415)
- Yutong Lin (ORCID: https://orcid.org/0000-0001-8038-4064)
- Yuhao Du
- Haocong Yi
Institutions
- Fujian Normal University (CN)
- Hong Kong Polytechnic University (HK)
- Peking University (CN)
- Peking University Shenzhen Hospital (CN)
- Fuzhou University (CN)
Publication Details
- Journal
- Small
- Published
- 2025-10-31
- DOI
- https://doi.org/10.1002/smll.202508900
- Citations
- 2
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 1.46