Lithicone-Protected Lithium Metal Anodes for Lithium Metal Batteries with Nickel-Rich Cathode Materials

Ridwan A. Ahmed, Kevin V. Carballo, Krishna P. Koirala, Qian Zhao, Peiyuan Gao, Ju-Myung Kim, Cassidy S. Anderson, Xiangbo Meng, Chongmin Wang, Ji-Guang Zhang, Wu Xu
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Abstract

The high energy density advantage of lithium (Li) metal batteries (LMBs) makes them increasingly desirable; however, problems such as strong reactivity and dendrite growth of Li metal anode limit their practical uses. In this work, a novel Li-containing glycerol (LiGL) or lithicone protection layer on a 50 μm thick Li metal anode is employed for improving the performance of LMBs. This LiGL layer was accurately deposited via a molecular layer deposition (MLD) process at 150 °C, using lithium tert-butoxide and glycerol as precursors. The as-formed LiGL coating layer is highly tunable in its thickness by simply adjusting MLD cycles and shows a good stability and outstanding ionic transport properties. The LiGL layer is found to effectively mitigate side reactions and enhance cycling stability in both symmetric cells and full cells. Specifically, the LMBs with LiGL@Li anode of 400 MLD cycles and LiNi0.6Mn0.2Co0.2O2 cathode enable a capacity retention of ≈87%, much higher than ≈35% of the cells with bare Li after 200 cycles at a charge/discharge current density of 2.1 mA cm−2. This work paves a feasible way for practical LMBs with improved capacity and stability through applying an innovative protection layer on Li metal anodes.

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用于含富镍阴极材料的锂金属电池的锂保护金属阳极
锂(Li)金属电池(LMB)的高能量密度优势使其越来越受到人们的青睐;然而,锂金属负极的强反应性和枝晶生长等问题限制了其实际应用。本研究在 50 μm 厚的锂金属阳极上采用了一种新型含锂甘油(LiGL)或有机硅保护层,以提高锂金属电池的性能。这种 LiGL 层是以叔丁醇锂和甘油为前驱体,通过分子层沉积(MLD)工艺在 150 °C 温度下精确沉积而成的。只需调整分子层沉积(MLD)周期,就能高度调节已形成的锂地胶层厚度,并显示出良好的稳定性和出色的离子传输特性。研究发现,无论是对称电池还是全电池,LiGL 涂层都能有效缓解副反应并提高循环稳定性。具体而言,在充放电电流密度为 2.1 mA cm-2 的条件下,使用 LiGL@Li 阳极和 LiNi0.6Mn0.2Co0.2O2 阴极的 LMB 电池在循环 400 次后,容量保持率可达 ≈87%,远高于使用裸锂电池 200 次后的容量保持率 ≈35%。这项研究通过在锂金属阳极上应用创新保护层,为提高容量和稳定性的实用 LMB 铺平了可行的道路。
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