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定制电子结构以实现快速的离子扩散和稳定的LiF-LiCl丰富的电极-电解质接口

Shan Su¹, Xuanyi Zhou¹, Weizhong Liang¹

¹Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education, School of Materials Science and Engineering, Xiangtan University Hunan 411105 China biaozhang@xtu.edu.cn.

Chemical science

|September 29, 2025

概括

一种新的功能性离子盐,DG-Cl,增强了金属电池 (LMB) 中固体电解质介相 (SEI) 的形成. 这促进了均的LiF-LiCl共同生长,使得超长周期稳定性和高容量保留用于先进的能量存储.

科学领域:

材料科学材料科学材料科学
电化学电化学电化学
电池技术电池技术

背景情况:

固体电解质间相 (SEI) 组成对于金属电池 (LMB) 的性能至关重要.
目前的SEI工程策略需要新的方法来增强稳定性和离子传输.
了解界面化学是释放金属阳极潜力的关键.

研究的目的:

设计一种功能性离子盐 (DG-Cl),以改善LMB中的SEI形成.
通过GD-Cl.调查Sei组件调节的分子层次机制.
为了评估金属电池的电化学性能提升,利用工程 SEI.

主要方法:

设计和合成具有 π 结合结构的功能性离子盐 (DG-Cl).
密度函数理论 (DFT) 计算来验证DG-Cl与Li+和TFSI-.的相互作用.
X射线光电子光谱 (XPS) 和飞行时间二次离子质谱 (TOF-SIMS) 用于SEI表征.
电化学测试对称和Li/LiFePO4全细胞,包括囊细胞.

主要成果:

DG-Cl通过空缺职位促进了Cl的定向释放,并通过TFSI结,促进了LiCl和LiF的形成.
据DFT的计算显示,DG-Cl在TFSI-中增强了C-F债券分拆,从而增加了LiF的产生.
XPS和TOF-SIMS证实了SEI上均的LiF-LiCl共同增长,改善了离子运输和调节沉积.
对称电池具有超长周期稳定性 (>4000小时在0.1 mA cm-2).
在2C的800个循环后,Li/LiFePO4全细胞显示82.04%的容量保留.
囊细胞表现出卓越的循环性能,在150个循环后保持96.6%.

结论:

功能性离子盐DG-Cl有效调节SEI的组成,并促进LiF-LiCl的形成.
这种分子层面对电子转移的控制导致LMB的循环稳定性和性能显著提高.
拟议的战略为开发高性能和稳定的金属电池提供了一个有希望的途径.

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