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 particular, the SAMs endow the full cells with substantially enhanced cyclability under high cathode loading, limited Li excess, and lean electrolyte conditions.

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• 1 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.
• 2 Hence, an SEI with enriched lithium fluoride (LiF) nanocrystals is generated, facilitating rapid Li + transfer and suppressing dendritic Li growth.
• 3 In particular, the SAMs endow the full cells with substantially enhanced cyclability under high cathode loading, limited Li excess, and lean electrolyte conditions.

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