Optimizing the Structure and Performances of Cu-MOF@Ti3C2TX Hybrid Electrodes by Introducing Modulated Ligand

作者：Sumin Li, Xiaokun Qu, Feng Liu, Pingwei Ye, Bo Yang, Qiang Cheng, Mengkun Yang, Yijing Nie, Maiyong Zhu · 发表于：Nanomaterials · 年份：2025 · DOI：10.3390/nano15110864 · 被引用次数：7 · 研究领域：MXene and MAX Phase Materials、Supercapacitor Materials and Fabrication、Metal-Organic Frameworks: Synthesis and Applications

To date, two-dimensional metal–organic frameworks (2D MOFs) have attracted much attention in many fields. Owing to their ultra-high porosity and specific surface area, great structural diversity and functional tunability, as well as feasible precision design at the molecular level, 2D MOFs have won rapid development in the field of energy storage. However, as a coordination compound, MOFs possess poor structural stability and are prone to structural collapse in electrochemical reactions, which seriously limits their electrochemical performance. Therefore, there is an urgent need to improve the structural stability of MOF electrode materials. In this study, a 2D MOF@Ti3C2TX hybrid was constructed, in which urea pyrimidinone isocyanate (UPy-NCO) units were introduced via a condensation reaction with the active functional groups on MOFs, thus forming multiple hydrogen bonds among MOF frameworks to strengthen their structural stability. Importantly, 2,6-diaminopyridine was utilized to modulate the structure and properties. Initially, the mono-coordination model of the N atom on a pyridine ring with metal ions could create defects and form further pores. Two −NH2 groups helped to improve the grafting reaction degree of UPy-NCO, leading to an increased ratio of forming quadruple hydrogen bonds (H-bonds), further strengthening the structure of the hybrid. As expected, the Cu-MOF@Ti3C2TX-20%DAP-UPy hybrid exhibited a specific capacitance of 148 F g−1 at 1 A g−1, which is 45% higher t...