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

doi:10.1016/j.actphy.2025.100087

物理化学学报 >> 2025, Vol. 41 >> Issue (8): 100087.doi: 10.1016/j.actphy.2025.100087

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

彭羽, 陈嘉威, 殷悦, 曹永杰, 廖莫愁, 王丛笑, 董晓丽*(), 夏永姚*()

复旦大学化学系, 上海市分子催化和创新材料重点实验室, 新能源研究院, 能源材料化学协同创新中心, 上海 200433

收稿日期:2025-02-19 修回日期:2025-03-18 录用日期:2025-04-02 发布日期:2025-06-07
通讯作者: Email: xldong@fudan.edu.cn (董晓丽)yyxia@fudan.edu.cn (夏永姚)
基金资助:
国家自然科学基金(21935003)

Tailored cathode electrolyte interphase via ethylene carbonate-free electrolytes enabling stable and wide-temperature operation of high-voltage LiCoO₂

Yu Peng, Jiawei Chen, Yue Yin, Yongjie Cao, Mochou Liao, Congxiao Wang, Xiaoli Dong*(), Yongyao Xia*()

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:2025-02-19 Revised:2025-03-18 Accepted:2025-04-02 Published:2025-06-07
Contact: Email: xldong@fudan.edu.cn (Xiaoli Dong)yyxia@fudan.edu.cn (Yongyao Xia)
Supported by:
the National Natural Science Foundation of China(21935003)

1. ACTPHY-2025.100087-SI-8p.pdf(4171KB)

摘要/Abstract

摘要：

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 ℃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。

关键词: 高电压电解液, 无碳酸乙烯酯电解液, 添加剂, 钴酸锂, 正极-电解质界面相

Abstract:

Raising the charge cut-off voltage of LiCoO₂ (LCO) cathodes provides a straightforward approach to increasing the energy density of lithium-ion batteries (LIBs). However, when the charge cut-off voltage exceeds 4.55 V (vs. Li/Li⁺), the cathode-electrolyte interphase (CEI) becomes unstable, failing to protect the LCO cathode from severe interfacial side reactions and structural instability. These issues accelerate battery degradation and severely hinder the practical application of high-energy-density LIBs. Moreover, ethylene carbonate (EC)-based electrolytes exhibit more pronounced parasitic reactions than EC-free electrolytes under high voltage, further exacerbating performance limitations. Therefore, optimizing the components and structure of the CEI with EC-free electrolytes remains a challenge. In this work, we aim to construct a robust and chemically stable F-/B-containing CEI on the surface of LCO cathodes using an EC-free electrolyte design. By replacing EC with more anti-oxidative propylene carbonate (PC) and fluoroethylene carbonate (FEC) co-solvents, the oxidative stability of the electrolyte is significantly improved. This promotes the formation of LiF within the CEI, thereby enhancing its mechanical strength. Meanwhile, the introduction of the sacrificial film-forming additive lithium bis(oxalato)borate (LiBOB) facilitates the generation of oxalates (Li₂C₂O₄) and B-containing crosslinked polymers (LiB_xO_y) within the CEI. These components exhibit high electrochemical stability and flexibility, compensating for the limitations of the LiF-rich CEI and further enhancing the overall structural stability of the CEI. This combination results in a rigid-flexible coupling architecture composed of inorganic-rich components (LiF and Li₂C₂O₄) embedded in B-containing crosslinked polymers (LiB_xO_y), ensuring both mechanical integrity and chemical stability of the CEI. Consequently, this tailored CEI effectively mitigates interfacial layer cracking and regeneration, reducing irreversible structural degradation and interfacial side reactions in high-voltage LCO cathodes. Based on these improvements, the EC-free PC-based electrolyte enables superior performance of LCO cathodes at 4.6 V, achieving 82% capacity retention at 0.5C over 200 cycles. Furthermore, graphite||LCO full cells demonstrate enhanced cycling stability at 4.5 V and enable operation across a wide temperature range (−40 to 80 ℃), highlighting the effectiveness of the rigid-flexible coupling CEI derived from the tailored electrolyte. By moving away from conventional EC-based electrolyte formulas, this work provides new insights into designing high-performance, wide-temperature, and sustainable PC-based electrolytes.

Key words: High-voltage electrolyte, Ethylene carbonate-free electrolyte, Additive, Lithium cobalt oxide, Cathode electrolyte interphase

彭羽, 陈嘉威, 殷悦, 曹永杰, 廖莫愁, 王丛笑, 董晓丽, 夏永姚. 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]. 物理化学学报, 2025, 41(8), 100087. doi: 10.1016/j.actphy.2025.100087

Yu Peng, Jiawei Chen, Yue Yin, Yongjie Cao, Mochou Liao, Congxiao Wang, Xiaoli Dong, Yongyao Xia. Tailored cathode electrolyte interphase via ethylene carbonate-free electrolytes enabling stable and wide-temperature operation of high-voltage LiCoO₂[J]. Acta Phys. -Chim. Sin. 2025, 41(8), 100087. doi: 10.1016/j.actphy.2025.100087

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100087

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I8/100087

图/表 6

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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

Tailored cathode electrolyte interphase via ethylene carbonate-free electrolytes enabling stable and wide-temperature operation of high-voltage LiCoO₂

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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

Tailored cathode electrolyte interphase via ethylene carbonate-free electrolytes enabling stable and wide-temperature operation of high-voltage LiCoO2

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Tailored cathode electrolyte interphase via ethylene carbonate-free electrolytes enabling stable and wide-temperature operation of high-voltage LiCoO₂