Three-Dimensional Covalent Organic Framework with Dense Lithiophilic Sites as Protective Layer to Enable High-Performance Lithium Metal Battery
Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review
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Detail(s)
Original language | English |
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Article number | e202417973 |
Journal / Publication | Angewandte Chemie - International Edition |
Online published | 5 Nov 2024 |
Publication status | Online published - 5 Nov 2024 |
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Abstract
Lithium (Li) metal batteries with remarkable energy densities are restrained by short lifetime and low Coulombic efficiency (CE), resulting from the accumulative Li dendrites and dead Li during cycling. Here, we prepared a new three-dimensional (3D) covalent organic framework (COF) with dense lithiophilic sites (heteoatom weight contents of 32.32 wt %) as an anodic protective layer of Li metal batteries. The 3D COF was synthesized using a [6+4] synthesis strategy by inducing flexible 6-connected cyclotriphosphazene derivative aldehyde and 4-connected porphyrin-based tetraphenylamines. Both phosphazene and porphyrin rings in the COF served as electron-rich and lithiophilic sites, enhancing a homogeneous Li+ flux via 3D direction towards highly smooth and compact Li deposition. The Li/Por-PN-COF-Cu cells achieved a record average CE of 99.1 % for 320 cycles with smooth Li deposition. Meanwhile, the abundant lithiophilic sites can promote fast Li+ transport with Li+ transference number of 0.87, enabling LiFePO4 full cell with stable stripping/plating processes even at a harsh rate of 5 C. Theoretical calculations revealed that the strong interaction force between Li+ and the COF facilitated the dissolution of Li+ from the electrolyte, and the low migration barrier of 1.08 eV indicated a favorable interaction between the Li+ ions and the π-electron system. © 2024 Wiley-VCH GmbH.
Research Area(s)
- abundant lithiophilic sites, covalent organic frameworks, cyclotriphosphazene, lithium metal battery, protective layer
Citation Format(s)
Three-Dimensional Covalent Organic Framework with Dense Lithiophilic Sites as Protective Layer to Enable High-Performance Lithium Metal Battery. / Zheng, Shuang; Fu, Yubin; Bi, Shuai et al.
In: Angewandte Chemie - International Edition, 05.11.2024.
In: Angewandte Chemie - International Edition, 05.11.2024.
Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review