A lithium carbonate-based additive for the interfacial stabilization of LiCoO2 cathode at 4.6 V

A Li2CO3-based additive was synthesized using the solid-phase sand-milling method, providing active Li+ and rapidly forming a uniform and stable cathode electrolyte interphase (CEI) layer, stabilizing the interface of the LCO cathode. [Display omitted] Extending the charging voltage of LiCoO2 (LCO)...

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Bibliographic Details
Published in:Journal of energy chemistry 2025-05, Vol.104, p.404-413
Main Authors: Wang, Zhen, Liu, Jun-Ke, Deng, Li, Liu, Jian, Jin, Zhi-Liang, Luo, Yu-Xi, Bai, Guo-Dong, Sun, Wen-Jing, Bai, Gao-Yang, Lin, Jing-Yi, Yin, Zu-Wei, Zhou, Yao, Li, Jun-Tao
Format: Article
Language:English
Subjects:
Cathode additive
High-voltage LiCoO2
Interfacial stability
Lithium carbonate
Lithium-ion batteries
Sand-milling
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Summary:A Li2CO3-based additive was synthesized using the solid-phase sand-milling method, providing active Li+ and rapidly forming a uniform and stable cathode electrolyte interphase (CEI) layer, stabilizing the interface of the LCO cathode. [Display omitted] Extending the charging voltage of LiCoO2 (LCO) is anongoing and promising approach to increase its energy density. However, the main challenge of the approach lies in the insuperable cathodic interfacial processes at high voltage, which leads to rapid failure both in the performance and structure of the LCO cathode. Herein, a Li2CO3-based additive was prepared by a simple sand-milling method, enabling a low electrochemical decomposition voltage 4.8 V, stabilizing the interface of the LCO cathode at 4.6 V. The decomposition of Li2CO3 provides extra Li+ and CO2 to supplement the Li consumption required in the initial irreversible interfacial reactions and rapidly form a uniform and stable cathode electrolyte interphase layer (less organic and more inorganic components) on the LCO cathode by reducing CO2. Thus, the phase transformation and the emergence of high-valent Co ions on the surface of LCO at 4.6 V high voltage were inhibited. Thanks to this, with 2% Li2CO3-based additive, the capacity retention of commercial LCO at a high voltage of 4.6 V at 0.5 C for 100 cycles was improved from 59.3% to 79.3%. This work improves the high-voltage stability of LCO and provides a new idea for realizing the high-voltage operation of batteries.
ISSN:2095-4956
DOI:10.1016/j.jechem.2024.12.046