Xu Zhixin, Zhang Xiyue, Yang Jun, Cui Xuzixu, Nuli Yanna, Wang Jiulin
Shanghai Electrochemical Energy Devices Research Center, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, 20742, USA.
Nat Commun. 2024 Nov 14;15(1):9856. doi: 10.1038/s41467-024-51958-7.
Current electrolytes of mixing different functional solvents inherit both merits and weaknesses of each solvent, thus cannot simultaneously meet all the requirements of high energy, long cycle life, and high safety for Li metal batteries (LMBs). Here, we design a high voltage and safe electrolyte (VSE) by integrating different functional groups into one molecule. The VSE electrolyte has a wide electrochemical stability window of ~5.6 V enabling a Li anode to achieve high Coulombic efficiency of >99.3%, Li | |LiNiCoMnO coin cell to maintain capacity retention of 92% after 500 cycles, and the 3.5-Ah-grade Li | |LiNiCoMnO pouch cell to deliver a high energy density of 531 Wh kg without any flame and expansion after cycled under extreme conditions. The VSE electrolyte even enables 5.0 V Li | |LiNiMnO cells to charge/discharge for 200 cycles without capacity decay. This work provides a promising direction for the rational design of high-voltage and intrinsically safe electrolytes for LMBs.
目前混合不同功能溶剂的电解质继承了每种溶剂的优点和缺点,因此不能同时满足锂金属电池(LMBs)对高能量、长循环寿命和高安全性的所有要求。在此,我们通过将不同的官能团整合到一个分子中,设计了一种高电压且安全的电解质(VSE)。VSE电解质具有约5.6 V的宽电化学稳定窗口,使得锂金属阳极能够实现>99.3%的高库仑效率,Li||LiNiCoMnO扣式电池在500次循环后保持92%的容量保持率,3.5 Ah级Li||LiNiCoMnO软包电池在极端条件下循环后可提供531 Wh kg的高能量密度,且无任何起火和膨胀现象。VSE电解质甚至能使5.0 V Li||LiNiMnO电池充放电200次而无容量衰减。这项工作为合理设计用于LMBs的高电压和本质安全电解质提供了一个有前景的方向。