Zhang Kai, An Yongling, Wei Chuanliang, Qian Yi, Zhang Yuchan, Feng Jinkui
SDU & Rice Joint Center for Carbon Nanomaterials, Key Laboratory for Liquid-Solid Structural Evolution & Processing of Materials (Ministry of Education), School of Materials Science and Engineering, Shandong University, Jinan 250061, P. R. China.
ACS Appl Mater Interfaces. 2021 Nov 3;13(43):50869-50877. doi: 10.1021/acsami.1c12589. Epub 2021 Oct 19.
Lithium metal anodes are promising for their high energy density and low working potential. However, high reactivity and dendrite growth of lithium metal lead to serious safety issues. Lithium dendrite may form "dead lithium" or pierce the separator, which will cause low efficiency and short-circuit inside the battery. A nonflammable phosphate-based electrolyte can effectively solve the flammability problem. Also, it shows poor compatibility with lithium metal anodes, resulting in an unstable solid electrolyte interface (SEI), which leads to dendrite growth and poor electrochemical performance. In this study, trimethyl phosphate is used to ensure the safety of lithium metal batteries. By adjusting the concentration of lithium salt and introducing fluoroethylene carbonate, a stable SEI layer is formed on the surface of the lithium metal anode and dendrite growth of the lithium metal anode is inhibited. Lithium metal batteries with a modified electrolyte achieved stable electrochemical plating/stripping, and the full cell has 93.4% capacity left and the coulombic efficiency is nearly 100%. In addition, the modified electrolyte can also enable reversible intercalation and de-intercalation of Li in the commercial graphite anode. This work may provide an alternative direction for the development of lithium metal batteries with high safety and high energy density.
锂金属阳极因其高能量密度和低工作电位而颇具前景。然而,锂金属的高反应活性和枝晶生长会导致严重的安全问题。锂枝晶可能会形成“死锂”或刺穿隔膜,这将导致电池内部效率低下和短路。一种不可燃的磷酸盐基电解质可以有效解决易燃性问题。此外,它与锂金属阳极的兼容性较差,导致固体电解质界面(SEI)不稳定,进而导致枝晶生长和电化学性能不佳。在本研究中,磷酸三甲酯用于确保锂金属电池的安全性。通过调整锂盐浓度并引入氟代碳酸乙烯酯,在锂金属阳极表面形成了稳定的SEI层,抑制了锂金属阳极的枝晶生长。采用改性电解质的锂金属电池实现了稳定的电化学镀覆/剥离,全电池剩余容量为93.4%,库仑效率接近100%。此外,改性电解质还能使商用石墨阳极中的锂实现可逆嵌入和脱嵌。这项工作可能为开发具有高安全性和高能量密度的锂金属电池提供一个替代方向。