Department of Materials Science & Engineering, School of Innovation and Entrepreneurship, Southern University of Science and Technology, Southern University of Science and Technology of China, Shenzhen, 518055, China.
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, China.
Nat Commun. 2023 Feb 25;14(1):1081. doi: 10.1038/s41467-023-36793-6.
The electrochemical stability window of the electrolyte solution limits the energy content of non-aqueous lithium metal batteries. In particular, although electrolytes comprising fluorinated solvents show good oxidation stability against high-voltage positive electrode active materials such as LiNiCoMnO (NCM811), the ionic conductivity is adversely affected and, thus, the battery cycling performance at high current rates and low temperatures. To address these issues, here we report the design and synthesis of a monofluoride ether as an electrolyte solvent with Li-F and Li-O tridentate coordination chemistries. The monofluoro substituent (-CHF) in the solvent molecule, differently from the difluoro (-CHF) and trifluoro (-CF) counterparts, improves the electrolyte ionic conductivity without narrowing the oxidation stability. Indeed, the electrolyte solution with the monofluoride ether solvent demonstrates good compatibility with positive and negative electrodes in a wide range of temperatures (i.e., from -60 °C to +60 °C) and at high charge/discharge rates (e.g., at 17.5 mA cm). Using this electrolyte solution, we assemble and test a 320 mAh Li||NCM811 multi-layer pouch cell, which delivers a specific energy of 426 Wh kg (based on the weight of the entire cell) and capacity retention of 80% after 200 cycles at 0.8/8 mA cm charge/discharge rate and 30 °C.
电解液的电化学稳定窗口限制了非水电解质锂金属电池的能量密度。特别是,尽管含氟溶剂的电解液对高压正极活性材料(如 LiNiCoMnO(NCM811))具有良好的氧化稳定性,但离子电导率受到不利影响,从而降低了电池在高电流速率和低温下的循环性能。为了解决这些问题,我们设计并合成了一种单氟醚作为电解质溶剂,具有 Li-F 和 Li-O 三配位化学。溶剂分子中的单氟取代基(-CHF)与二氟(-CHF)和三氟(-CF)不同,在不缩小氧化稳定性的情况下提高了电解质的离子电导率。实际上,具有单氟醚溶剂的电解质溶液在很宽的温度范围内(即从-60°C 到+60°C)和高充放电速率(例如在 17.5 mA cm 下)与正负极具有良好的相容性。使用这种电解质溶液,我们组装并测试了一个 320 mAh 的 Li||NCM811 多层袋式电池,在 0.8/8 mA cm 的充放电速率和 30°C 下,经过 200 次循环后,其比能量为 426 Wh kg(基于整个电池的重量),容量保持率为 80%。