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Resolving the Phase Instability of a Fluorinated Ether, Carbonate-Based Electrolyte for the Safe Operation of an Anode-Free Lithium Metal Battery
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2020-10-28 , DOI: 10.1021/acsaem.0c01767
Teklay Mezgebe Hagos, Tesfaye Teka Hagos, Hailemariam Kassa Bezabh, Gebregziabher Brhane Berhe, Ljalem Hadush Abrha, Shuo-Feng Chiu, Chen-Jui Huang, Wei-Nien Su, Hongjie Dai, Bing Joe Hwang

The anode-free full cell architecture (Cu||NMC111) is an essential milestone for boosting the energy density of lithium metal batteries (LMBs). The LiPF6 dissolved in fluorinated carbonate (fluoroethylene carbonate (FEC)) and partially fluorinated ether (1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE)) solvents has been reported to be a fluorinated electrolyte in the development of LMBs because of their wide electrochemical windows, nonflammable characteristics, and stable LiF-rich solid electrolyte interface. However, its phase instability and high viscosity limit its practical application. In this work, an advanced ethyl methyl carbonate (EMC)-based fluorinated electrolyte (1 M LiPF6 in FEC/TTE/EMC (3:5:2 by vol.) is developed, which is free of phase instability and has higher ionic conductivity, oxidative stability, and nonflammability. It has a higher oxidation potential of >5.3 V and better rate capabilities than the EMC-free electrolyte for lithium metal batteries (Li||NCM111). Meanwhile, the ternary electrolyte also enhances the cycling performance of anode-free lithium metal batteries (AFLMBs) within the potential range of 2.5–4.5 V at room temperature. The Cu||NMC111 cell with 1 M LiPF6 in FEC/TTE/EMC (3:5:2 by vol.) electrolyte delivers superior capacity retention of 40% and average Coulombic efficiency (av CE) of 98.30% for 80 cycles with a cutoff voltage of 4.5 V at the charge and discharge current densities of 0.2 and 0.5 mA/cm2, respectively. Hence, we develop a robust nonflammable electrolyte free of phase instability having wider oxidative stability, high rate capability, and good cyclic performance using an anode-free full cell configuration (Cu||NMC111).

中文翻译:

解决氟化醚碳酸盐基电解质的相不稳定性,以确保无阳极锂金属​​电池的安全运行

无阳极全电池架构(Cu || NMC111)是提高锂金属电池(LMB)能量密度的重要里程碑。据报道,溶解在氟化碳酸盐(碳酸氟亚乙酯(FEC))和部分氟化醚(1,1,2,2-四氟乙基-2,2,3,3-四氟丙基醚(TTE))中的LiPF 6是一种LMBs发展中的氟化电解质,因为它们具有宽的电化学窗口,不可燃的特性以及稳定的富LiF固体电解质界面。但是,其相不稳定和高粘度限制了其实际应用。在这项工作中,使用了高级碳酸乙基甲基酯(EMC)基氟化电解质(1 M LiPF 6在FEC / TTE / EMC(体积比为3∶5∶2)中开发了一种无相不稳定性且具有较高离子传导性,氧化稳定性和不燃性的化合物。它比锂金属电池(Li || NCM111)不含EMC的电解液具有更高的氧化电位> 5.3 V和更好的倍率性能。同时,三元电解质还可在室温下在2.5–4.5 V的电位范围内增强无阳极锂金属​​电池(AFLMB)的循环性能。在FEC / TTE / EMC(体积比为3:5:2)电解质中具有1 M LiPF 6的Cu || NMC111电池可在80个循环中提供40%的出色容量保持率和98.30%的平均库仑效率(av CE)。充放电电流密度分别为0.2和0.5 mA / cm 2时的截止电压为4.5 V, 分别。因此,我们使用无阳极的全电池配置(Cu || NMC111),开发了一种具有相稳定性的,坚固的,不可燃的,无相不稳定的电解质,该电解质具有较宽的氧化稳定性,较高的倍率能力和良好的循环性能。
更新日期:2020-11-23
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