Wang Yuankun, Ni Youxuan, Xu Shuo, Lu Yong, Shang Long, Yang Zhuo, Zhang Kai, Yan Zhenhua, Xie Weiwei, Chen Jun
Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin 300071, China.
J Am Chem Soc. 2025 Mar 26;147(12):10772-10783. doi: 10.1021/jacs.5c02140. Epub 2025 Mar 14.
Developing solvents with balanced physicochemical properties for high-voltage cathodes and lithium metal anodes is crucial for a sustainable and intelligent future. Herein, we report fully methylated tetramethyl-1,3-dimethoxydisiloxane (TMMS) as a single solvent for lithium metal batteries. We demonstrate that the fully methylated structure and Si-O bonds within TMMS can effectively elevate the dehydrogenation energy barrier, migrating the oxidation decomposition of the electrolyte. Additionally, the weak solvating power of TMMS favors the formation of an anion-rich solvation structure that induces the generation of an inorganic-rich electrode/electrolyte interphase layer at both the cathode and anode. Accordingly, the formulated electrolyte exhibits remarkable stability against high-voltage cathodes and lithium metal anodes. Notably, LiNiCoMnO||Li (NCM811||Li) full cells with TMMS-based electrolytes realize a significant improvement in capacity retention compared with a dimethoxyethane-based electrolyte at both room temperature and 50 °C. This work provides insight into full methylation and the Si-O bond strategy and paves the way for the development of high-voltage lithium metal batteries.
开发具有平衡物理化学性质的溶剂用于高压阴极和锂金属阳极对于可持续和智能的未来至关重要。在此，我们报告了全甲基化的四甲基-1,3-二甲氧基二硅氧烷（TMMS）作为锂金属电池的单一溶剂。我们证明，TMMS内的全甲基化结构和Si-O键可以有效提高脱氢能垒，迁移电解质的氧化分解。此外，TMMS的弱溶剂化能力有利于形成富阴离子的溶剂化结构，从而在阴极和阳极诱导生成富含无机的电极/电解质界面层。因此，所配制的电解质对高压阴极和锂金属阳极表现出显著的稳定性。值得注意的是，与基于二甲氧基乙烷的电解质相比，具有基于TMMS电解质的LiNiCoMnO||Li（NCM811||Li）全电池在室温和50°C下的容量保持率都有显著提高。这项工作为全甲基化和Si-O键策略提供了见解，并为高压锂金属电池的开发铺平了道路。
