Revealing Lithium Nitrate-Mediated Solid-Electrolyte Interphase of Lithium Metal Anode via Cryogenic Transmission Electron Microscopy.
basic_science · Level V
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- Record sourced from PubMed, PMID 38781452.
- Also identified by DOI 10.1021/acs.nanolett.4c01351.
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Abstract
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 LiNO<sub>3</sub> additives in SEI modulation at different temperature (25 and 50 °C). Poor cycle stability of LMA in the baseline electrolyte without LiNO<sub>3</sub> additives stems from the Li<sub>2</sub>CO<sub>3</sub>-rich mosaic-type SEI. Increased LiNO<sub>3</sub> content and elevated operating temperature enhance cyclic performance by forming bilayer or multilayer SEI structures via preferential LiNO<sub>3</sub> decomposition, but may thicken the SEI, leading to reduced initial Coulombic efficiency and increased overpotential. The optimal SEI features a multilayer structure with Li<sub>2</sub>O-rich inner layer and closely packed grains in the outer layer, minimizing electrolyte decomposition or corrosion.