Synergistic bulk and surface engineering via rapid quenching for high-performance Li-rich layered manganese oxide cathodes

doi:10.1088/1674-1056/adc673

中国物理B ›› 2025, Vol. 34 ›› Issue (5): 58201-058201.doi: 10.1088/1674-1056/adc673

Synergistic bulk and surface engineering via rapid quenching for high-performance Li-rich layered manganese oxide cathodes

Xinyun Xiong(熊馨筠)^1,3, Sichen Jiao(焦思晨)^2,4, Qinghua Zhang(张庆华)¹, Luyao Wang(王璐瑶)^1,4, Kun Zhou(周坤)^1,3, Bowei Cao(曹博维)^1,3, Xilin Xu(徐熙林)^2,4, Xiqian Yu(禹习谦)^1,2,4,†, and Hong Li(李泓)^1,2,4,‡

1 National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China;
2 Beijing Frontier Research Center on Clean Energy, Huairou Division, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China;
3 School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China;
4 Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

收稿日期:2025-03-04 修回日期:2025-03-19 接受日期:2025-03-28 出版日期:2025-04-18 发布日期:2025-05-06
通讯作者: Xiqian Yu, Hong Li E-mail:xyu@iphy.ac.cn;hli@iphy.ac.cn
基金资助:
Project supported by the National Key Research and Development Program of China (Grant No. 2022YFB2502200) and the National Natural Science Foundation of China (Grant Nos. 52325207, 22239003, and 22393904).

Synergistic bulk and surface engineering via rapid quenching for high-performance Li-rich layered manganese oxide cathodes

1 National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China;
2 Beijing Frontier Research Center on Clean Energy, Huairou Division, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China;
3 School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China;
4 Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Received:2025-03-04 Revised:2025-03-19 Accepted:2025-03-28 Online:2025-04-18 Published:2025-05-06
Contact: Xiqian Yu, Hong Li E-mail:xyu@iphy.ac.cn;hli@iphy.ac.cn
Supported by:
Project supported by the National Key Research and Development Program of China (Grant No. 2022YFB2502200) and the National Natural Science Foundation of China (Grant Nos. 52325207, 22239003, and 22393904).

1. 2025-058201-SI.pdf(696KB)

摘要/Abstract

摘要： Lithium-rich manganese-based cathodes (LRMs) have garnered significant attention as promising candidates for high-energy-density batteries due to their exceptional specific capacity exceeding 300 mAh/g, achieved through synergistic anionic and cationic redox reactions. However, these materials face challenges including oxygen release-induced structural degradation and consequent capacity fading. To address these issues, strategies such as surface modification and bulk phase engineering have been explored. In this study, we developed a facile and cost-effective quenching approach that simultaneously modifies both surface and bulk characteristics. Multi-scale characterization and computational analysis reveal that rapid cooling partially preserves the high-temperature disordered phase in the bulk structure, thereby enhancing the structural stability. Concurrently, Li$^{+}$/H$^{+}$ exchange at the surface forms a robust rock-salt/spinel passivation layer, effectively suppressing oxygen evolution and mitigating interfacial side reactions. This dual modification strategy demonstrates a synergistic stabilization effect. The enhanced oxygen redox activity coexists with the improved structural integrity, leading to superior electrochemical performance. The optimized cathode delivers an initial discharge capacity approaching 307.14 mAh/g at 0.1 C and remarkable cycling stability with 94.12% capacity retention after 200 cycles at 1 C. This study presents a straightforward and economical strategy for concurrent surface-bulk modification, offering valuable insights for designing high-capacity LRM cathodes with extended cycle life.

关键词: lithium-rich manganese-based cathodes, surface-bulk engineering, oxygen redox activity, high-capacity cathodes, long-cycle stability

Abstract: Lithium-rich manganese-based cathodes (LRMs) have garnered significant attention as promising candidates for high-energy-density batteries due to their exceptional specific capacity exceeding 300 mAh/g, achieved through synergistic anionic and cationic redox reactions. However, these materials face challenges including oxygen release-induced structural degradation and consequent capacity fading. To address these issues, strategies such as surface modification and bulk phase engineering have been explored. In this study, we developed a facile and cost-effective quenching approach that simultaneously modifies both surface and bulk characteristics. Multi-scale characterization and computational analysis reveal that rapid cooling partially preserves the high-temperature disordered phase in the bulk structure, thereby enhancing the structural stability. Concurrently, Li$^{+}$/H$^{+}$ exchange at the surface forms a robust rock-salt/spinel passivation layer, effectively suppressing oxygen evolution and mitigating interfacial side reactions. This dual modification strategy demonstrates a synergistic stabilization effect. The enhanced oxygen redox activity coexists with the improved structural integrity, leading to superior electrochemical performance. The optimized cathode delivers an initial discharge capacity approaching 307.14 mAh/g at 0.1 C and remarkable cycling stability with 94.12% capacity retention after 200 cycles at 1 C. This study presents a straightforward and economical strategy for concurrent surface-bulk modification, offering valuable insights for designing high-capacity LRM cathodes with extended cycle life.

Key words: lithium-rich manganese-based cathodes, surface-bulk engineering, oxygen redox activity, high-capacity cathodes, long-cycle stability

中图分类号: (Lithium-ion batteries)

82.47.Aa

82.45.Fk (Electrodes)

Xinyun Xiong(熊馨筠), Sichen Jiao(焦思晨), Qinghua Zhang(张庆华), Luyao Wang(王璐瑶), Kun Zhou(周坤), Bowei Cao(曹博维), Xilin Xu(徐熙林), Xiqian Yu(禹习谦), and Hong Li(李泓). Synergistic bulk and surface engineering via rapid quenching for high-performance Li-rich layered manganese oxide cathodes[J]. 中国物理B, 2025, 34(5): 58201-058201.

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