High-Entropy Rock-Salt Surface Layer Stabilizes the Ultrahigh-Ni Single-Crystal CathodeClick to copy article linkArticle link copied!
- Zhongxing XuZhongxing XuSchool of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaSchool of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. ChinaMore by Zhongxing Xu
- Xinghan ChenXinghan ChenSchool of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaSchool of Materials, Sun Yat-sen University, Shenzhen 518107, P. R. ChinaMore by Xinghan Chen
- Wenguang FanWenguang FanSchool of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaMore by Wenguang Fan
- Minzhi ZhanMinzhi ZhanSchool of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaMore by Minzhi Zhan
- Xulin MuXulin MuShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, P. R. ChinaMore by Xulin Mu
- Hongbin CaoHongbin CaoSchool of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaMore by Hongbin Cao
- Xiaohu WangXiaohu WangSchool of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaMore by Xiaohu Wang
- Haoyu XueHaoyu XueSchool of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaMore by Haoyu Xue
- Zhihai GaoZhihai GaoSchool of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaMore by Zhihai Gao
- Yongzhi LiangYongzhi LiangSchool of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaMore by Yongzhi Liang
- Jiajie Liu*Jiajie Liu*Email: [email protected]School of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaMore by Jiajie Liu
- Xinghua Tan*Xinghua Tan*Email: [email protected]School of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, P. R. ChinaMore by Xinghua Tan
- Feng Pan*Feng Pan*Email: [email protected]School of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, P. R. ChinaMore by Feng Pan
Abstract

Single-crystalline Ni-rich layered oxides are one of the most promising cathode materials for lithium-ion batteries due to their superior structural stability. However, sluggish lithium-ion diffusion kinetics and interfacial issues hinder their practical applications. These issues intensify with increasing Ni content in the ultrahigh-Ni regime (≥90%), significantly threatening the practical viability of the single-crystalline strategy for ultrahigh-Ni layered oxide cathodes. Herein, by developing a high-entropy coating strategy, we successfully constructed an epitaxial lattice-coherent high-entropy rock-salt layer (∼3 nm) via Zr and Al doping on the surface of the single-crystalline cathode LiNi0.92Co0.05Mn0.03O2 through an in situ modification process. The surface high-entropy rock-salt layer with tailored Ni valence and lattice coherence not only greatly improves lithium-ion diffusion kinetics but also suppresses interface parasitic reactions and surface structural degradations. The high-entropy surface layer-stabilized ultrahigh-Ni single-crystalline cathode (SC-Ni92-ZA) demonstrates significantly improved rate and cycling performances (127.5 mAh g–1 at 20C, capacity retention of 74.9% after 500 cycles at 1C) in a half-cell. The SC-Ni92-ZA exhibits a capacity retention of 87.1% after 600 cycles at 1C in a full-cell. This epitaxial lattice-coherent high-entropy coating strategy develops a promising avenue for developing high-capacity, long-life cathode materials.
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