In Situ Self‐Assembly of Ordered Organic/Inorganic Dual‐Layered Interphase for Achieving Long‐Life Dendrite‐Free Li Metal Anodes in LiFSI‐Based Electrolyte
In Situ Self‐Assembly of Ordered Organic/Inorganic Dual‐Layered Interphase for Achieving Long‐Life Dendrite‐Free Li Metal Anodes in LiFSI‐Based Electrolyte
复制标题
在LiFSI基电解液中原位自组装有序有机/无机双层界面实现长寿命无树枝晶锂金属阳极
DOI：
10.1002/adfm.202007434
复制
发表时间：
2020-11
影响因子：
19
通讯作者：
Jian Wang;Jin Yang;Qingbo Xiao;Jing Zhang;Tie Li;Lujie Jia;Zilan Wang;Shuang Cheng;Linge Li
中科院分区：
文献类型：
--
作者：
Jian Wang;Jin Yang;Qingbo Xiao;Jing Zhang;Tie Li;Lujie Jia;Zilan Wang;Shuang Cheng;Linge Li
具有3860 mA h g−1高容量的金属锂电极是可充电电池最有前途的候选者。然而，其固有的一些问题，如枝晶生长，不均匀的固体电解质界面（SEI），高制造风险限制了它的实际应用。在此，与传统的镶嵌结构不同，提出了在锂表面上具有有序双层结构以抑制枝晶形成的原位自组装有机/无机混合SEI的简易制造。在中等活性的含氟离子液体的帮助下，所形成的氟化锂和稳健有序的有机部分在金属锂表面上原位自组装。双层结构的演化过程通过X射线光谱、原位和频产生光谱和原子力显微镜来揭示。所形成的“双重保护”有序杂化界面层还表现出令人惊讶的抗碳酸盐电解质或干燥空气腐蚀的能力。因此，预处理的金属锂电极表现出优异的剥离/镀覆可逆性（99%）和长达1200 h的长寿命而不形成枝晶，并且在10 mA cm-2的电流密度下保持高性能，这比大多数报道高得多，显示出对未来利用的促进前景。
Metallic lithium electrode with high capacity of 3860 mA h g−1 is the most promising candidate for rechargeable batteries. However, some inherent problems such as dendrite growth, uneven solid electrolyte interphase (SEI), and high manufacturing risk restraint its practical application. Herein, distinct from the conventional mosaic structure, a facile fabrication of in situ self‐assembled organic/inorganic hybrid SEI with ordered dual‐layer structure on the lithium surface to suppress dendrite formation is proposed. With the aid of moderate active fluoric‐containing ionic liquid, the as‐formed lithium fluoride and robust ordered organic moieties are in situ self‐assembled on the metallic lithium surface. The evolution process of the dual‐layered structure is revealed by X‐ray spectroscopy, in situ sum frequency generation spectroscopy, and atomic force microscopy. The formed “double protection” ordered hybrid interphase layer also exhibits the surprising ability against the corrosion of carbonate electrolyte or dry air. As a consequence, the pretreated metallic lithium electrode represents excellent stripping/plating reversibility of ≈99% and a long lifespan up to 1200 h without formation of dendrite, and remains high performance at a current density of 10 mA cm−2, which is much higher than most reports, showing the facilitating promising to the future utilization.