Topological Strain-Induced Regioselective Linker Elimination in a Chiral Zr(IV)-Based Metal-Organic Framework
| Autor: | Yong Cui, Kuiwei Yang, Xinfa Chen, Zhijie Chen, Jianwen Jiang, Wei Gong, Florencia A. Son, Yan Liu, Omar K. Farha, Wenqiang Zhang |
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| Rok vydání: | 2021 |
| Předmět: |
chemistry.chemical_classification
Materials science General Chemical Engineering Biochemistry (medical) Regioselectivity 02 engineering and technology General Chemistry 010402 general chemistry 021001 nanoscience & nanotechnology Topology 01 natural sciences Biochemistry 0104 chemical sciences chemistry Materials Chemistry Environmental Chemistry Chemical stability Metal-organic framework 0210 nano-technology Porosity Linker Crown ether Topology (chemistry) Bond cleavage |
| Zdroj: | Chem. 7:190-201 |
| ISSN: | 2451-9294 |
| DOI: | 10.1016/j.chempr.2020.11.008 |
| Popis: | Summary Zr-carboxylate metal-organic frameworks (MOFs) are structurally robust materials, in part due to their strong coordination bonds. The regioselective Zr–O bond cleavage and formation between 3D architectures are thus challenging and are heretofore unexplored. In this work, by introducing highly flexible 18-crown-6-ether functionalities into a homochiral Zr-MOF, we report an unprecedented topology transition in which a 4,10-connected framework undergoes a rapid solid-state transition into a thermodynamically more stable 4,8-connected analog by a regioselective-linker-elimination under ambient conditions. The transition process was unambiguously unraveled by single-crystal and powder X-ray diffraction studies, and we proposed a possible transition mechanism based on various control experiments and theoretical calculations. The excellent chemical stability and substantially expanded porosity and pore apertures endowed the transformed chiral MOF with an exceptional capacity for the enantioadsorptive and solid-phase extractive separation of the racemic drug molecule of lansoprazole with 98% ee and 93% ee, respectively. |
| Databáze: | OpenAIRE |
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