Dissolving uptake-hindering surface defects in metal–organic frameworks†,Chemical Science

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Dissolving uptake-hindering surface defects in metal–organic frameworks†
Chemical Science ( IF 7.6 ) Pub Date : 2018-10-10 00:00:00 , DOI: 10.1039/c8sc03735c
Kai Müller _{1,

2,

3} , Nina Vankova _{3,

4,

5,

6,

7} , Ludger Schöttner _{1,

2,

3} , Thomas Heine _{3,

4,

5,

6,

7} , Lars Heinke _{1,

2,

3}

Affiliation

Metal–organic frameworks (MOFs) have unique properties which make them perfectly suited for various adsorption and separation applications; however, their uses and efficiencies are often hindered by their limited stability. When most MOFs are exposed to water or humid air, the MOF structure, in particular at the surface, is destroyed, creating surface defects. These surface defects are surface barriers which tremendously hinder the uptake and release of guest molecules and, thus, massively decrease the performance in any application of MOFs. Here, the destruction by exposure to water vapor is investigated by using well-defined MOF films of type HKUST-1 as a model system for uptake experiments with different-sized probe molecules as well as for spectroscopic investigations, complemented by density functional theory calculations of the defect structure. In addition to the characterization of the surface defects, it is found that the pristine MOF structure can be regenerated. We show that the surface defects can be dissolved by exposure to the synthesis solvent, here ethanol, enabling fast uptake and release of guest molecules. These findings show that the storage of MOF materials in a synthesis solvent results in healing of surface defects and enables ideal performance of MOF materials.

中文翻译：

解决金属有机框架中阻碍吸收的表面缺陷†

金属有机骨架（MOF）具有独特的性能，使其非常适合各种吸附和分离应用。但是，它们的使用和效率通常会因其有限的稳定性而受到阻碍。当大多数MOF暴露于水或潮湿空气中时，MOF结构，特别是在表面上，会被破坏，从而产生表面缺陷。这些表面缺陷是表面障碍，极大地阻碍了客体分子的吸收和释放，因此，在任何MOF应用中都会大大降低性能。在这里，通过使用清晰定义的HKUST-1型MOF膜作为模型系统，研究了暴露于水蒸气的破坏，该系统用于使用不同大小的探针分子进行吸收实验以及用于光谱学研究，补充缺陷结构的密度泛函理论计算。除了表征表面缺陷外，还发现原始的MOF结构可以再生。我们显示表面缺陷可以通过暴露于合成溶剂（在此为乙醇）而溶解，从而能够快速吸收和释放客体分子。这些发现表明，MOF材料在合成溶剂中的存储可导致表面缺陷的修复，并使MOF材料具有理想的性能。

更新日期：2018-10-10

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