Stabilizing Surface Lattice O<i><sup>n</sup></i><sup>−</sup> (0 &lt; <i>n</i> &lt; 2) for Long‐Term Durability of LiCoO<sub>2</sub>

The instability of surface lattice O<sup>n</sup> <sup>-</sup> (0 < n < 2) in charged LiCoO₂ (LCO) limits its long-term cycling stability beyond 4.55 V versus Li/Li⁺. Herein, the spinel and rock-salt (RS) phases are constructed on LCO surface to stabilize lattice O<sup>n</sup> <sup>-</sup>, namely S-LCO and R-LCO, respectively. Upon long-term cycling at 4.6 V, the loss of lattice O<sup>n</sup> <sup>-</sup> leads to a progressive deterioration of surface spinel phase, which ultimately transforms into a strong Li<sup>+</sup>-blocking phase. In contrast, for R-LCO, the surface lattice O<sup>n</sup> <sup>-</sup> in the RS phase remains stable in long-term cycles. Theoretical calculations reveal that the migration barriers of lattice O<sup>n</sup> <sup>-</sup> are significantly higher in the RS phase than in the spinel phase. Due to the stabilized surface lattice O<sup>n</sup> <sup>-</sup>, the R-LCO||Li cell shows an impressive capacity retention of 78.6% after 1000 cycles at 4.6 V (at 1C rate) and superior floating charge durability at 45 °C. This study highlights the importance of surface structure tailoring in developing advanced LCO cathodes.

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Publication Details

Journal
Angewandte Chemie International Edition
Published
2025-03-28
DOI
https://doi.org/10.1002/anie.202503100
Citations
10
Primary Topic
Advancements in Battery Materials
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article
Field-Weighted Citation Impact
7.30
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article

Stabilizing Surface Lattice On− (0 < n < 2) for Long‐Term Durability of LiCoO2

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10 citations
Angewandte Chemie International Edition
Advancements in Battery Materials
7.30
article

Stabilizing Surface Lattice On− (0 < n < 2) for Long‐Term Durability of LiCoO2

Bin Fei, Shunning Li, Xingxing Yin, Hengyu Ren, Dong Zhou, Feng Pan, Mingyang Li, Guojie Chen, Hai Lin, Lin Zhou, Wangyang Ding, Zijian Li, Wenguang Zhao, Xiaohu Wang, Qinghe Zhao, Shiming Chen, Haocong Yi, Jun Wang
article en
10 citations

Abstract

The instability of surface lattice O<sup>n</sup> <sup>-</sup> (0 < n < 2) in charged LiCoO₂ (LCO) limits its long-term cycling stability beyond 4.55 V versus Li/Li⁺. Herein, the spinel and rock-salt (RS) phases are constructed on LCO surface to stabilize lattice O<sup>n</sup> <sup>-</sup>, namely S-LCO and R-LCO, respectively. Upon long-term cycling at 4.6 V, the loss of lattice O<sup>n</sup> <sup>-</sup> leads to a progressive deterioration of surface spinel phase, which ultimately transforms into a strong Li<sup>+</sup>-blocking phase. In contrast, for R-LCO, the surface lattice O<sup>n</sup> <sup>-</sup> in the RS phase remains stable in long-term cycles. Theoretical calculations reveal that the migration barriers of lattice O<sup>n</sup> <sup>-</sup> are significantly higher in the RS phase than in the spinel phase. Due to the stabilized surface lattice O<sup>n</sup> <sup>-</sup>, the R-LCO||Li cell shows an impressive capacity retention of 78.6% after 1000 cycles at 4.6 V (at 1C rate) and superior floating charge durability at 45 °C. This study highlights the importance of surface structure tailoring in developing advanced LCO cathodes.

Angewandte Chemie International EditionVol. 64(23)
King University (US), Hong Kong Polytechnic University (HK), Sun Yat-sen University (CN), Shenzhen University (CN), Peking University (CN), Southern University of Science and Technology (CN), University of Malaya (MY), Advanced Energy (United States) (US), Peking University Shenzhen Hospital (CN)
Openalex Percentile: Top 3%
Advancements in Battery Materials
7.30
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