Citation: Yu Peng, Jiawei Chen, Yue Yin, Yongjie Cao, Mochou Liao, Congxiao Wang, Xiaoli Dong, Yongyao Xia. 无碳酸乙烯酯电解液定向构筑正极电解质界面相实现高电压钴酸锂的宽温域稳定运行[J]. Acta Physico-Chimica Sinica, ;2025, 41(8): 100087. doi: 10.1016/j.actphy.2025.100087 shu

无碳酸乙烯酯电解液定向构筑正极电解质界面相实现高电压钴酸锂的宽温域稳定运行

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai 200433, China

Received Date: 19 February 2025
Revised Date: 18 March 2025
Accepted Date: 2 April 2025

Fund Project: The project was supported by the National Natural Science Foundation of China (21935003).

提升钴酸锂(LCO)正极的充电截止电压是提高锂离子电池(LIBs)能量密度的直接策略。然而，高电压下正极-电解质界面相(CEI)的不稳定性严重制约了高能量密度LIBs的发展。因此，本研究利用无碳酸乙烯酯(EC)的电解液设计，通过构建兼具化学稳定性与机械强度的氟/硼复合CEI以提升界面稳定性。采用碳酸丙烯酯(PC)及氟代碳酸乙烯酯(FEC)作为溶剂，增强电解液的抗氧化稳定性，促进CEI中氟化锂(LiF)组分的生成，提升其机械强度。同时，引入双草酸硼酸锂(LiBOB)添加剂，在CEI中形成含硼交联聚合物(LiB_xO_y)组分，以其柔性结构特征弥补LiF层的不足之处。最终，构建出具有富无机相(LiF和Li₂C₂O₄)嵌入含硼类聚合物(LiB_xO_y)基体结构的刚柔并济CEI。这种CEI其兼具结构致密性、良好的机械稳定性与电化学稳定性等优点，有效抑制高电压下LCO的界面副反应及不可逆结构退化。实验结果表明，无EC的PC基电解液使LCO正极在4.6 V高截止电压下展现出优异的电化学性能，0.5C倍率循环200次后容量保持率达82%。此外，石墨||LCO全电池在4.5 V截止电压下表现出显著提升的循环稳定性，并实现-40 - 80 °C宽温域范围内的稳定运行，验证了该优化电解液衍生的刚柔并济CEI的有效性。本研究突破传统EC基电解液设计范式，为开发高性能、宽温域及可持续PC基电解液提供了新思路。
- High-voltage electrolyte,
- Ethylene carbonate-free electrolyte,
- Additive,
- Lithium cobalt oxide,
- Cathode electrolyte interphase
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