Su Li-Ling, Yao Nan, Li Zheng, Bi Chen-Xi, Chen Zi-Xian, Chen Xiang, Li Bo-Quan, Zhang Xue-Qiang, Huang Jia-Qi
School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, P. R. China.
Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, 100081, P. R. China.
Angew Chem Int Ed Engl. 2024 Mar 4;63(10):e202318785. doi: 10.1002/anie.202318785. Epub 2024 Feb 2.
The cycle life of high-energy-density lithium-sulfur (Li-S) batteries is severely plagued by the incessant parasitic reactions between Li metal anodes and reactive Li polysulfides (LiPSs). Encapsulating Li-polysulfide electrolyte (EPSE) emerges as an effective electrolyte design to mitigate the parasitic reactions kinetically. Nevertheless, the rate performance of Li-S batteries with EPSE is synchronously suppressed. Herein, the sacrifice in rate performance by EPSE is circumvented while mitigating parasitic reactions by employing hexyl methyl ether (HME) as a co-solvent. The specific capacity of Li-S batteries with HME-based EPSE is nearly not decreased at 0.1 C compared with conventional ether electrolytes. With an ultrathin Li metal anode (50 μm) and a high-areal-loading sulfur cathode (4.4 mg cm ), a longer cycle life of 113 cycles was achieved in HME-based EPSE compared with that of 65 cycles in conventional ether electrolytes at 0.1 C. Furthermore, both high energy density of 387 Wh kg and stable cycle life of 27 cycles were achieved in a Li-S pouch cell (2.7 Ah). This work inspires the feasibility of regulating the solvation structure of LiPSs in EPSE for Li-S batteries with balanced performance.
高能量密度锂硫(Li-S)电池的循环寿命受到锂金属负极与活性锂多硫化物(LiPSs)之间持续不断的寄生反应的严重困扰。封装锂多硫化物电解质(EPSE)作为一种有效的电解质设计,在动力学上减轻了寄生反应。然而,采用EPSE的Li-S电池的倍率性能也会同步受到抑制。在此,通过使用己基甲基醚(HME)作为共溶剂,在减轻寄生反应的同时规避了EPSE对倍率性能的牺牲。与传统醚类电解质相比,采用基于HME的EPSE的Li-S电池在0.1 C下的比容量几乎没有下降。使用超薄锂金属负极(50μm)和高面载量硫正极(4.4 mg cm)时,基于HME的EPSE在0.1 C下实现了113次循环的更长循环寿命,而传统醚类电解质为65次循环。此外,在一个Li-S软包电池(2.7 Ah)中实现了387 Wh kg的高能量密度和27次循环的稳定循环寿命。这项工作激发了通过调节EPSE中LiPSs的溶剂化结构来实现性能平衡的Li-S电池的可行性。