Olefin‐Linked Covalent Organic Frameworks with Electronegative Channels as Cationic Highways for Sustainable Lithium Metal Battery Anodes

Despite the enormous interest in Li metal as an ideal anode material, the uncontrollable Li dendrite growth and unstable solid electrolyte interphase have plagued its practical application. These limitations can be attributed to the sluggish and uneven Li+ migration towards Li metal surface. Here, w...

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Bibliographic Details
Published in:Angewandte Chemie 2023-09, Vol.135 (37), p.n/a
Main Authors: Li, Zhongping, Sun, Linhai, Zhai, Lipeng, Oh, Kyeong‐Seok, Seo, Jeong‐Min, Li, Changqing, Han, Diandian, Baek, Jong‐Beom, Lee, Sang‐Young
Format: Article
Language:English
Subjects:
Anodes
Cationic Membranes
Cations
Channels
Chemistry
Covalent Organic Frameworks
Electrode materials
Electrolytic cells
Electronegative Channels
Electronegativity
Highways
Ion currents
Lithium
Lithium Batteries
Membranes
Metal surfaces
Olefin Linkage
Solid electrolytes
Triazine
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Summary:Despite the enormous interest in Li metal as an ideal anode material, the uncontrollable Li dendrite growth and unstable solid electrolyte interphase have plagued its practical application. These limitations can be attributed to the sluggish and uneven Li+ migration towards Li metal surface. Here, we report olefin‐linked covalent organic frameworks (COFs) with electronegative channels for facilitating selective Li+ transport. The triazine rings and fluorinated groups of the COFs are introduced as electron‐rich sites capable of enhancing salt dissociation and guiding uniform Li+ flux within the channels, resulting in a high Li+ transference number (0.85) and high ionic conductivity (1.78 mS cm−1). The COFs are mixed with a polymeric binder to form mixed matrix membranes. These membranes enable reliable Li plating/stripping cyclability over 700 h in Li/Li symmetric cells and stable capacity retention in Li/LiFePO4 cells, demonstrating its potential as a viable cationic highway for accelerating Li+ conduction. Olefin‐linked covalent organic frameworks (COFs) with electronegative 1D channels are presented as a cationic highway membrane strategy for sustainable Li metal battery anodes. Introduction of triazine rings and fluorinated groups into the COF skeletons played a viable role in enhancing salt dissociation and guiding uniform Li+ flux within the channels. The resulting COF membrane exhibited reliable Li plating/stripping cyclability and stable capacity retention in the Li/LiFePO4 full cell.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202307459