Cheng Hao, Mao Yangjun, Lu Yunhao, Zhang Peng, Xie Jian, Zhao Xinbing
State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, P. R. China.
Department of Physics, Zhejiang University, Hangzhou 310027, P. R. China.
Nanoscale. 2020 Feb 7;12(5):3424-3434. doi: 10.1039/c9nr09749j. Epub 2020 Jan 28.
Lithium metal has attracted considerable attention due to its ultrahigh theoretical capacity. Nevertheless, issues such as dendritic Li formation and instability of the Li metal/electrolyte interface still restrain its practical applications. In this work, we design a Li composite anode with fluorinated carbon nanotubes (FCNT) fabricated by a simple melting-soaking method. It was found that trace amounts of added FCNT (only 1.6 wt%) lead to a significant chemical/electrochemical stability of metallic Li. The obtained Li/FCNT composite electrode (LFCNT) exhibits much better stability in open air and electrolyte than bare Li. The LFCNT enables uniform plating/stripping of metallic Li, preventing the dendrite formation during repeated cycling. In situ optical microscopy observations confirm dendrite-free Li deposition with the mechanism clarified by density functional theory calculations. Compared with bare Li, the LFCNT shows a considerable improvement in rate capability, voltage hysteresis and cycle performance, sustaining stable cycling at a high current density of 3 mA cm or a capacity up to 5 mA h cm. Li-O cells with a LFCNT anode exhibit a long life of 135 cycles at a capacity of 1000 mA h g, which is six-fold than that with the bare Li anode.
锂金属因其超高的理论容量而备受关注。然而,诸如锂枝晶的形成以及锂金属/电解质界面的不稳定性等问题仍然限制了其实际应用。在这项工作中,我们通过一种简单的熔融浸渍法设计了一种含氟化碳纳米管(FCNT)的锂复合阳极。研究发现,添加微量的FCNT(仅1.6 wt%)就能显著提高金属锂的化学/电化学稳定性。所制备的锂/FCNT复合电极(LFCNT)在空气中和电解质中比裸锂表现出更好的稳定性。LFCNT能使金属锂均匀地沉积和剥离,防止在反复循环过程中形成枝晶。原位光学显微镜观察证实了无枝晶的锂沉积,密度泛函理论计算阐明了其机理。与裸锂相比,LFCNT在倍率性能、电压滞后和循环性能方面有显著改善,能在3 mA cm的高电流密度或高达5 mA h cm的容量下维持稳定循环。采用LFCNT阳极的锂氧电池在1000 mA h g的容量下可循环135次,寿命是使用裸锂阳极的六倍。