Chu Juan, Liu Zhaoli, Yu Jie, Wang Heng-Guo, Cui Fengchao, Zhu Guangshan
Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry, Northeast Normal University, 130024, Changchun, P. R. China.
Nat Commun. 2025 Apr 14;16(1):3549. doi: 10.1038/s41467-025-58759-6.
Two-dimensional conjugated metal organic frameworks (2D c-MOFs) hold significant promise as electrode materials for alkali metal ion batteries while their electrochemical properties still lack reasonable and effective regulation. Here, two representative 2D c-MOFs (M-HHTQ/M-HHTP, M=Cu or Ni) as positive electrodes are used as models to explore the basic/microscopic principles of their complex storage mechanism in sodium ion batteries (SIBs). It is demonstrated that the energy storage mechanism of 2D c-MOFs is determined by the interaction between coordination covalent bonds and organic linkers. Theoretical calculations and experiment results have jointly demonstrated that the redox potential and theoretical capacity can be regulated based on the valence of M-O bond and the utilization of anions and cations, respectively. As a result, Cu-HHTQ achieves a high discharge voltage at 2.55 V (vs. Na/Na), a higher stable specific capacity of 208 mAh g at 0.05 A g, and long cyclability with the capacity retention rate of 100% at 1 A g after 2000 cycles.
二维共轭金属有机框架（2D c-MOFs）作为碱金属离子电池的电极材料具有巨大潜力，但其电化学性能仍缺乏合理有效的调控。在此，以两种代表性的二维共轭金属有机框架（M-HHTQ/M-HHTP，M = Cu或Ni）作为正极作为模型，探索其在钠离子电池（SIBs）中复杂存储机制的基本/微观原理。结果表明，二维共轭金属有机框架的储能机制由配位共价键与有机连接体之间的相互作用决定。理论计算和实验结果共同表明，氧化还原电位和理论容量可分别基于M-O键的价态和阴阳离子的利用率进行调控。结果，Cu-HHTQ在2.55 V（相对于Na/Na）时实现了高放电电压，在0.05 A g下具有208 mAh g的更高稳定比容量，并且具有长循环稳定性，在1 A g下经过2000次循环后容量保持率为100%。
