张其春Angew:氮杂三角烯三酮基COFs

科技   2024-11-27 16:38   河北  

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1.由于Na+的大半径,钠离子电池(SIBs)具有缓慢的动力学、大的体积变化和有限的比容量。这些问题可以通过使用共价有机框架(COFs)作为电极来解决。

2.本文中,设计并合成了含氮杂三角烯三酮的COF(记为CityU-33)作为SIBs的电极材料。

3.由于其固有的丰富的多个氧化还原活性位点和快速嵌入动力学,CityU-33在0.1 A g-1下提供了410.4 mAh g-1的高放电容量,并显示出显著的长期循环稳定性,其中在0.2 A g-1下实现了313 mAh g-1的放电容量,在1700次循环后保持率约为100%,使其成为SIBs的顶级COF电极材料。


Scheme 1. The synthesis of CityU-33. (Inserted: Crystallographic structure of ATTO-3N (upper right), the hydrogen atoms and solvated dichloromethane are omitted for clarity.) 


Figure 1. FTIR spectra of CityU-33 (a). XPS profiles of CityU-33: (b) C 1s; (c) N 1s. (d) PXRD patterns of experimental (Wine), Pawley-refined (black), simulated stacking (violet), and their difference (light blue), and Bragg positions (green) for CityU-33. (e) Space-filling modes of CityU-33 with layers arranged in an AA stacking mode along c-direction (left) and b-direction (right). (f) Nitrogen adsorption-desorption isotherms of CityU-33 at 77 K (Inserted: pore size distribution). 


Figure 2. (a) CV curves of CityU-33 at various scan rates. (b) Determination of b value according to the relationship between peak current and scan rate. (c) Pseudocapacitive and diffusion-controlled storage contributions at different scan rates. (d) Rate performance. (e) Discharge-charge curves of the CityU-33-based electrode at various current densities. (f) Cycle performance of Na//CityU-33 cell at the current density of 0.2 A g-1. (g) Comparison of electrochemical performance of Na//CityU-33 cell with representative organic electrode materials. 


Figure 3. The corresponding 2D color filled contour plot in Wavenumber vs. Time from of in-situ ATR-FTIR test of Na//CityU-33 cell. 


Figure 4. (a) Schematic diagram of the molecular electrostatic potential (MESP) of the CityU-33 repetitive unit. (b) LUMO plot for per CityU-33 repetitive unit (c) Total energy of unit cells for different Na+ intercalation step of CityU-33. (d) Top and side views of intercalation structure of n (n = 1-12) sodium atoms on each CityU-33 repetitive unit cell. 


https://doi.org/10.1002/ange.202417779


信息来源:COF催化在线




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