电解质
原位
材料科学
金属
电子显微镜
化学工程
纳米技术
化学
无机化学
电极
冶金
物理化学
光学
有机化学
物理
工程类
作者
Cheng Ma,Yongqiang Cheng,Kuibo Yin,Jian Luo,Asma Sharafi,Jeff Sakamoto,Juchuan Li,Karren L. More,Nancy J. Dudney,Miaofang Chi
出处
期刊:Nano Letters
[American Chemical Society]
日期:2016-10-06
卷期号:16 (11): 7030-7036
被引量:314
标识
DOI:10.1021/acs.nanolett.6b03223
摘要
Despite their different chemistries, novel energy-storage systems, e.g., Li–air, Li–S, all-solid-state Li batteries, etc., face one critical challenge of forming a conductive and stable interface between Li metal and a solid electrolyte. An accurate understanding of the formation mechanism and the exact structure and chemistry of the rarely existing benign interfaces, such as the Li–cubic-Li7–3xAlxLa3Zr2O12 (c-LLZO) interface, is crucial for enabling the use of Li metal anodes. Due to spatial confinement and structural and chemical complications, current investigations are largely limited to theoretical calculations. Here, through an in situ formation of Li–c-LLZO interfaces inside an aberration-corrected scanning transmission electron microscope, we successfully reveal the interfacial chemical and structural progression. Upon contact with Li metal, the LLZO surface is reduced, which is accompanied by the simultaneous implantation of Li+, resulting in a tetragonal-like LLZO interphase that stabilizes at an extremely small thickness of around five unit cells. This interphase effectively prevented further interfacial reactions without compromising the ionic conductivity. Although the cubic-to-tetragonal transition is typically undesired during LLZO synthesis, the similar structural change was found to be the likely key to the observed benign interface. These insights provide a new perspective for designing Li–solid electrolyte interfaces that can enable the use of Li metal anodes in next-generation batteries.
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