Self-assembled monolayers direct a LiF-rich interphase toward long-life lithium metal batteries

High-energy density lithium (Li) metal batteries (LMBs) are promising for energy storage applications but suffer from uncontrollable electrolyte degradation and the consequently formed unstable solid-electrolyte interphase (SEI). In this study, we designed self-assembled monolayers (SAMs) with high-...

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Bibliographic Details
Published in:Science (American Association for the Advancement of Science) 2022-02, Vol.375 (6582), p.739-745
Main Authors: Liu, Yujing, Tao, Xinyong, Wang, Yao, Jiang, Chi, Ma, Cong, Sheng, Ouwei, Lu, Gongxun, Lou, Xiong Wen David
Format: Article
Language:English
Subjects:
Aluminum
Aluminum oxide
Dendrites
Fluorides
Interphase
Ion transport
Lithium
Lithium batteries
Lithium fluoride
Lithium ions
Monolayers
Polypropylene
Self-assembled monolayers
Self-assembly
Separators
Solid electrolytes
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Summary:High-energy density lithium (Li) metal batteries (LMBs) are promising for energy storage applications but suffer from uncontrollable electrolyte degradation and the consequently formed unstable solid-electrolyte interphase (SEI). In this study, we designed self-assembled monolayers (SAMs) with high-density and long-range-ordered polar carboxyl groups linked to an aluminum oxide-coated separator to provide strong dipole moments, thus offering excess electrons to accelerate the degradation dynamics of carbon-fluorine bond cleavage in Li bis(trifluoromethanesulfonyl)imide. Hence, an SEI with enriched lithium fluoride (LiF) nanocrystals is generated, facilitating rapid Li transfer and suppressing dendritic Li growth. In particular, the SAMs endow the full cells with substantially enhanced cyclability under high cathode loading, limited Li excess, and lean electrolyte conditions. As such, our work extends the long-established SAMs technology into a platform to control electrolyte degradation and SEI formation toward LMBs with ultralong life spans.
ISSN:0036-8075
1095-9203
DOI:10.1126/science.abn1818