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Title: Highly crystalline polyimide covalent organic framework as dual-active-center cathode for high-performance lithium-ion batteries
Authors: Yao, Liyi
Ma, Chao
Sun, Libo
Zhang, Daliang
Chen, Yuze
Jin, Enquan
Song, Xiaowei
Liang, Zhiqiang
Wang, Kai-Xue
Keywords: Engineering::Chemical engineering
Issue Date: 2022
Source: Yao, L., Ma, C., Sun, L., Zhang, D., Chen, Y., Jin, E., Song, X., Liang, Z. & Wang, K. (2022). Highly crystalline polyimide covalent organic framework as dual-active-center cathode for high-performance lithium-ion batteries. Journal of the American Chemical Society, 144(51), 23534-23542.
Journal: Journal of the American Chemical Society
Abstract: Polyimide covalent organic framework (PI-COF) materials that can realize intrinsic redox reactions by changing the charge state of their electroactive sites are considered as emerging electrode materials for rechargeable devices. However, the highly crystalline PI-COFs with hierarchical porosity are less reported due to the rapid reaction between monomers and the poor reversibility of the polyimidization reaction. Here, we developed a water-assistant synthetic strategy to adjust the reaction rate of polyimidization, and PI-COF (COFTPDA-PMDA) with kgm topology consisting of dual active centers of N,N,N',N'-tetrakis(4-aminophenyl)-1,4-benzenediamine (TPDA) and pyromellitic dianhydride (PMDA) ligands was successfully synthesized with high crystallinity and porosity. The COFTPDA-PMDA possesses hierarchical micro-/mesoporous channels with the largest surface area (2669 m2/g) in PI-COFs, which can promote the Li+ ions and bulky bis(trifluoromethanesulfonyl)imide (TFSI-) ions in organic electrolyte to sufficiently interact with the dual active sites on COF skeleton to increase the specific capacity of cathode materials. As a cathode material for lithium-ion batteries, COFTPDA-PMDA@50%CNT which integrated high surface area and dual active center of COFTPDA-PMDA with carbon nanotubes via π-π interactions gave a high initial charge capacity of 233 mAh/g (0.5 A/g) and maintains at 80 mAh/g even at a high current density of 5.0 A/g after 1800 cycles.
ISSN: 0002-7863
DOI: 10.1021/jacs.2c10534
Schools: School of Chemical and Biomedical Engineering 
Rights: © 2022 American Chemical Society. All rights reserved.
Fulltext Permission: none
Fulltext Availability: No Fulltext
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