Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

材料科学 电解质 锂(药物) 化学工程 电极 快离子导体 杂质 金属锂 离子电导率 电化学 物理化学 医学 工程类 内分泌学 有机化学 化学
作者
Hongpeng Zheng,Shaoping Wu,Ran Tian,Zhenming Xu,Hong Zhu,Huanan Duan,Hezhou Liu
出处
期刊:Advanced Functional Materials [Wiley]
卷期号:30 (6) 被引量:141
标识
DOI:10.1002/adfm.201906189
摘要

Abstract Solid‐state lithium batteries are widely considered as next‐generation lithium‐ion battery technology due to the potential advantages in safety and performance. Among the various solid electrolyte materials, Li–garnet electrolytes are promising due to their high ionic conductivity and good chemical and electrochemical stabilities. However, the high electrode/electrolyte interfacial impedance is one of the major challenges. Moreover, short circuiting caused by lithium dendrite formation is reported when using Li–garnet electrolytes. Here, it is demonstrated that Li–garnet electrolytes wet well with lithium metal by removing the intrinsic impurity layer on the surface of the lithium metal. The Li/garnet interfacial impedance is determined to be 6.95 Ω cm 2 at room temperature. Lithium symmetric cells based on the Li–garnet electrolytes are cycled at room temperature for 950 h and current density as high as 13.3 mA cm −2 without showing signs of short circuiting. Experimental and computational results reveal that it is the surface oxide layer on the lithium metal together with the garnet surface that majorly determines the Li/garnet interfacial property. These findings suggest that removing the superficial impurity layer on the lithium metal can enhance the wettability, which may impact the manufacturing process of future high energy density garnet‐based solid‐state lithium batteries.
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