Pan Haoyu, Yang Zhanlin, Chen Jianhui, Li Hengyi, Wen Cuilian, Sa Baisheng
Multiscale Computational Materials Facility & Materials Genome Institute, School of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, China.
Fujian Applied Technology Engineering Center of Power Battery Materials, Fujian College of Water Conservancy and Electric Power, Yong'an 366000, China.
Molecules. 2024 Jun 21;29(13):2955. doi: 10.3390/molecules29132955.
Currently, lithium-ion batteries have an increasingly urgent need for high-performance electrolytes, and additives are highly valued for their convenience and cost-effectiveness features. In this work, the feasibilities of fullerenes and fluorinated fullerenes as typical bis(fluorosulfonyl)imide/1,2-dimethoxymethane (LiFSI/DME) electrolyte additives are rationally evaluated based on density functional theory calculations and molecular dynamic simulations. Interestingly, electronic structures of C, CF, CF, CF, 1-CF, and 2-CF are found to be compatible with the properties required as additives. It is noted that that different numbers and positions of F atoms lead to changes in the deformation and electronic properties of fullerenes. The F atoms not only show strong covalent interactions with C cages, but also affect the C-C covalent interaction in C cages. In addition, molecular dynamic simulations unravel that the addition of trace amounts of CF, CF, and 2-CF can effectively enhance the Li mobility in LiFSI/DME electrolytes. The results expand the range of applications for fullerenes and their derivatives and shed light on the research into novel additives for high-performance electrolytes.
目前，锂离子电池对高性能电解质的需求日益迫切，添加剂因其便利性和成本效益特性而备受重视。在这项工作中，基于密度泛函理论计算和分子动力学模拟，合理评估了富勒烯和氟化富勒烯作为典型双（氟磺酰）亚胺/1,2 - 二甲氧基甲烷（LiFSI/DME）电解质添加剂的可行性。有趣的是，发现C、CF、CF、CF、1 - CF和2 - CF的电子结构与作为添加剂所需的性质相匹配。值得注意的是，F原子数量和位置的不同会导致富勒烯的变形和电子性质发生变化。F原子不仅与C笼表现出强烈的共价相互作用，还会影响C笼中的C - C共价相互作用。此外，分子动力学模拟表明，添加痕量的CF、CF和2 - CF可以有效提高LiFSI/DME电解质中Li的迁移率。这些结果扩展了富勒烯及其衍生物的应用范围，并为高性能电解质新型添加剂的研究提供了启示。
