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Chen, Ming‐Zhu; Li, Jian; Liao, Sheng; Guo, Yi‐Hang; Liu, Tao; Ma, Rui‐Fang; Xie, Tian‐Yi; Liu, Wei‐Dong; Peng, Si‐Xu; Kuang, Xiaojun; Yin, Zheng; Zhao, Yingbo; Zeng, Ming‐Hua
Angewandte Chemie International Edition, July 17, 2023, Volume: 62, Issue: 29Journal Article
Glassy and liquid state metal–organic frameworks (MOFs) are emerging type of materials subjected to intense research for their rich physical and chemical properties. In this report, we obtained the first glassy MOF that involves metal‐carboxylate cluster building units via multi‐stage structural transformations. This MOF is composed of linear Mn3(COO)6 node and flexible pyridyl‐ethenylbenzoic linker. The crystalline MOF was first perturbed by vapor hydration and thermal dehydration to give an amorphous state, which can go through a glass transition at 505 K into a super‐cooled liquid. The super‐cooled liquid state is stable through a wide temperature range of 40 K and has the largest fragility index of 105, giving a broad processing window. Remarkably, the super‐cooled liquid can not only be quenched into glass, but also recrystallize into the initial MOF when heated to a higher temperature above 558 K. The mechanism of the multi‐stage structural transformations was studied by systematic characterizations of in situ X‐ray diffraction, calorimetry, rheological, spectroscopic and pair‐distribution function analysis. These multi‐stage transformations not only represent a rare example of high temperature coordinative recognition and self‐assembly, but also provide new MOF processing strategy through crystal‐amorphous‐liquid‐crystal transformations. The first MOF glass composed of metal‐carboxylate cluster building units is vitrified by multi‐stage transformations: The crystalline MOF is amorphized by vapor hydration and thermal dehydration, goes through a glass transition to enter a super‐cooled liquid state, and recrystallizes into the initial structure. These multi‐stage transformations are a rare example of high‐temperature coordinative recognition and self‐assembly.
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