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金属-有机骨架材料(metal-organic frameworks,MOFs)的纳微结构可根据特定需求进行功能化调控,有望成为良好的工业催化材料。由于溶剂环境可对其界面微环境及催化性能产生较大影响,因此研究溶剂化效应对于MOF材料的影响具有重要的意义。以Cu-BTC和MOP-15两种典型MOF材料作为研究对象,采用密度泛函理论与COSMO溶剂模型相结合的方法,考察了溶剂效应对材料几何结构与电子稳定性的影响,并研究了不同溶剂对其Lewis酸性的影响。结果表明,溶剂环境可以使材料中的电子从不饱和配位金属处转移到有机配体上,进而使材料具有更强的Lewis酸性,并且电负性较大有机配体构成的MOF材料,受溶剂效应的影响更加显著。本工作将有助于深入理解溶剂化对调控MOF材料液相催化活性的影响。
The nanostructures of metal-organic frameworks (MOFs) can be functionally regulated according to specific requirements and are expected to be good industrial catalytic materials. As the solvent environment can have a great influence on the interface microenvironment and catalytic performance, it is of great significance to study the effect of solvation on the MOF material. Two typical MOF materials, Cu-BTC and MOP-15, were selected as the research objects. The effects of solvent effect on the geometry and electron stability of the material were investigated by means of density functional theory and COSMO solvent model. Effect of solvent on Lewis acidity. The results show that the solvent environment can make the material from the unsaturated coordination metal at the organic ligand transfer, and thus make the material has a stronger Lewis acidity, and electronegativity greater organic ligands MOF material composition, The effect of solvent effect is more pronounced. This work will help to understand the effect of solvation on the liquid-phase catalytic activity of MOF.