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Covalent Organic Framework-Derived Ion-Sieving Channels Enabling Stable Lithium Metal Anodes through Interfacial Engineering and Solvation Structure Modulation
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PRE
AI
张
S
M
韩
Y
DOI：10.1021/acsami.5c09152.png)
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Abstract
En 中文
Lithium metal anodes, despite their ultrahigh capacity, suffer from severe interfacial instability due to uncontrolled parasitic reactions and dendritic growth, limiting practical applications. Herein, a 2D covalent organic framework (NUS-9) synthesized via cryogenic interfacial growth was engineered into a NUS-9@PP composite separator to enhance lithium metal battery performance. Its unique layered architecture establishes vertically aligned Li+ transport channels with ion-sieving functionality, while lithiophilic polar groups regulate Li+ solvation structures, suppressing electrolyte–Li parasitic reactions. Modified separators demonstrated lower nucleation overpotentials of 38.2/42.8 mV at 0.3/0.5 mA cm–2 and extended electrochemical stability to 4.7 V. Benefiting from TFSI– anchoring effects and control of Li+ transport flux distribution, NUS-9@PP demonstrated superior Li+ transport properties with a high Li+ transference number (0.71), stable 370 h cycling at 3 mA cm–2, and 99.8% coulombic efficiency. XPS analysis confirmed its capability to promote the LiF-rich solid electrolyte interface (SEI) formation, effectively suppressing lithium dendrite growth. Full-cell tests further validated significantly enhanced cycling longevity and efficiency, establishing a novel strategy for stabilizing lithium metal anodes by using 2D COF materials.
Keywords:
lithium metal anode
covalent organic framework
composite separator
lithium-ion transport
dendrite suppression
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8.2
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6.1W
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38.7W
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