Haiyan Luo, Xiangyu Ji, Baodan Zhang, Ming Chen, Xiaohong Wu, Yuanlong Zhu, Xiaoyu Yu, Junhao Wang, Haitang Zhang, Yuhao Hong, Yeguo Zou, Guang Feng, Yu Qiao, Haoshen Zhou, Shi-Gang Sun
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引用次数: 0
Abstract
Electrolyte engineering is crucial for improving cathode electrolyte interphase (CEI) to enhance the performance of lithium-ion batteries, especially at high charging cut-off voltages. However, typical electrolyte modification strategies always focus on the solvation structure in the bulk region, but consistently neglect the dynamic evolution of electrolyte solvation configuration at the cathode-electrolyte interface, which directly influences the CEI construction. Herein, we reveal an anti-synergy effect between Li+-solvation and interfacial electric field by visualizing the dynamic evolution of electrolyte solvation configuration at the cathode-electrolyte interface, which determines the concentration of interfacial solvated-Li+. The Li+ solvation in the charging process facilitates the construction of a concentrated (Li+-solvent/anion-rich) interface and anion-derived CEI, while the repulsive force derived from interfacial electric field induces the formation of a diluted (solvent-rich) interface and solvent-derived CEI. Modifying the electrochemical protocols and electrolyte formulation, we regulate the "inflection voltage" arising from the anti-synergy effect and prolong the lifetime of the concentrated interface, which further improves the functionality of CEI architecture.
电解质工程对于改善阴极电解质相间(CEI)以提高锂离子电池的性能至关重要,尤其是在高充电截止电压下。然而,典型的电解质改性策略总是侧重于体液区域的溶解结构,却始终忽视了阴极-电解质界面上电解质溶解构型的动态演化,而这直接影响到 CEI 的构建。在这里,我们通过可视化阴极-电解质界面上电解质溶解构型的动态演化,揭示了 Li+ 溶解与界面电场之间的反协同效应,而界面电场决定了界面溶解 Li+ 的浓度。充电过程中的 Li+ 溶解促进了浓缩(Li+ 溶剂/阴离子富集)界面和阴离子衍生 CEI 的形成,而界面电场产生的排斥力则诱导了稀释(溶剂富集)界面和溶剂衍生 CEI 的形成。通过修改电化学方案和电解质配方,我们调节了反协同效应产生的 "拐点电压",延长了浓缩界面的寿命,从而进一步提高了 CEI 结构的功能。
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.