高结晶聚酰亚胺共价有机骨架作为高性能锂离子电池的双活性中心阴极,Journal of the American Chemical Society

当前位置： X-MOL 学术 › J. Am. Chem. Soc. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

高结晶聚酰亚胺共价有机骨架作为高性能锂离子电池的双活性中心阴极
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-12-13 , DOI: 10.1021/jacs.2c10534
Liyi Yao ₁ , Chao Ma _{2,

3} , Libo Sun ₄ , Daliang Zhang ₅ , Yuze Chen ₁ , Enquan Jin ₁ , Xiaowei Song ₁ , Zhiqiang Liang ₁ , Kai-Xue Wang ₂

Affiliation

聚酰亚胺共价有机骨架（PI-COF）材料可以通过改变其电活性位点的电荷状态来实现本征氧化还原反应，被认为是可充电设备的新兴电极材料。然而，由于单体之间的快速反应和聚酰亚胺化反应的可逆性差，具有分级孔隙率的高结晶PI-COFs的报道较少。在这里，我们开发了一种水助合成策略来调节聚酰亚胺化的反应速率，以及 PI-COF (COF _TPDA-PMDA ) 具有kgm拓扑结构，由N , N , N ′, N双活性中心组成成功合成了具有高结晶度和孔隙率的 '-四(4-氨基苯基)-1,4-苯二胺 (TPDA) 和苯均四酸二酐 (PMDA) 配体。COF _TPDA-PMDA具有 PI-COF 中表面积最大 (2669 m ² /g) 的多级微孔/中孔通道，可以促进有机物中的 Li ⁺离子和大体积双（三氟甲磺酰基）亚胺 (TFSI ^– ) 离子电解质与 COF 骨架上的双活性位点充分相互作用，以提高正极材料的比容量。作为锂离子电池正极材料，COF _{TPDA-PMDA @50%CNT集成了COF}_TPDA-PMDA的高比表面积和双活性中心通过 π-π 相互作用与碳纳米管结合，初始充电容量高达 233 mAh/g（0.5 A/g），并在 1800 次循环后即使在 5.0 A/g 的高电流密度下也能保持在 80 mAh/g。

"点击查看英文标题和摘要"

Highly Crystalline Polyimide Covalent Organic Framework as Dual-Active-Center Cathode for High-Performance Lithium-Ion Batteries

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 (COF_TPDA-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 COF_TPDA-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, COF_TPDA-PMDA@50%CNT which integrated high surface area and dual active center of COF_TPDA-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.

更新日期：2022-12-13

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南