Revealing Lithium Nitrate-Mediated Solid-Electrolyte Interphase of Lithium Metal Anode via Cryogenic Transmission Electron Microscopy

The cycle stability of lithium metal anode (LMA) largely depends on solid-electrolyte interphase (SEI). Electrolyte engineering is a common strategy to adjust SEI properties, yet understanding its impact is challenging due to limited knowledge on ultrafine SEI structures. Herein, using cryogenic tra...

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Bibliographic Details
Published in:Nano letters Vol. 24; no. 22; pp. 6714 - 6721
Main Authors: Zhen, Cheng, Yang, Xuming, Wei, Xianbin, Zhu, Yuanmin, Han, Shaobo, Shi, Xiaobo, Deng, Li, Gu, M. Danny
Format: Journal Article
Language:English
Published: United States American Chemical Society 23-05-2024
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Summary:The cycle stability of lithium metal anode (LMA) largely depends on solid-electrolyte interphase (SEI). Electrolyte engineering is a common strategy to adjust SEI properties, yet understanding its impact is challenging due to limited knowledge on ultrafine SEI structures. Herein, using cryogenic transmission electron microscopy, we reveal the atomic-level SEI structure of LMA in ether-based electrolytes, focusing on the role of LiNO3 additives in SEI modulation at different temperature (25 and 50 °C). Poor cycle stability of LMA in the baseline electrolyte without LiNO3 additives stems from the Li2CO3-rich mosaic-type SEI. Increased LiNO3 content and elevated operating temperature enhance cyclic performance by forming bilayer or multilayer SEI structures via preferential LiNO3 decomposition, but may thicken the SEI, leading to reduced initial Coulombic efficiency and increased overpotential. The optimal SEI features a multilayer structure with Li2O-rich inner layer and closely packed grains in the outer layer, minimizing electrolyte decomposition or corrosion.
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ISSN:1530-6984
1530-6992
DOI:10.1021/acs.nanolett.4c01351