Journal
NANO LETTERS
Volume 16, Issue 11, Pages 7030-7036Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b03223
Keywords
Solid electrolytes; stability; lithium metal; in situ; electron microscopy; interface; passivation
Categories
Funding
- U.S. Department of Energy (DOE), office of Basic Energy Sciences (BES), Materials Sciences and Engineering Division
- Scientific User Facilities Division, BES-DOE
- DOE - Energy Efficiency and Renewable Energy [DE-EE00006821]
- VirtuES project [ORNL-LDRD 7739]
- NSF [CMMI-1436976]
- NSSEFF [N00014-16-1-2569]
- NSF-China [11674052]
- Directorate For Engineering
- Div Of Civil, Mechanical, & Manufact Inn [1436305, 1436976] Funding Source: National Science Foundation
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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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