Lee Soochan, Lee Sungmin, Kwak Yuna, Yousaf Masood, Cho Eunchan, Moon Hoi Ri, Cho Sung June, Park Noejung, Choe Wonyoung
Department of Chemistry, Ulsan National Institute of Science and Technology, Ulsan 44919, Republic of Korea.
Center for Multidimensional Carbon Materials, Institute for Basic Science, Ulsan 44919, Republic of Korea.
JACS Au. 2024 Jun 20;4(7):2539-2546. doi: 10.1021/jacsau.4c00285. eCollection 2024 Jul 22.
A new topology previously unknown in metal-organic frameworks (MOFs) provides an important clue to uncovering a new series of polyhedral MOFs. We report a novel MOF crystallized in a parsimonious topology based on Frank-Kasper (FK) polyhedra. The distribution of angles in a tetrahedral arrangement (T-O-T) is crucial for the formation of FK polyhedra in topology. This finding led us to investigate the T-O-T angle distribution in related zeolites and zeolitic imidazolate frameworks (ZIFs). Unlike zeolites, it is extremely difficult to achieve high T-O-T angles in ZIFs, which prevents the formation of some FK topologies. Density functional theory (DFT) total energy calculations support a correlation between T-O-T angles and the feasibility of new tetrahedron-based FK frameworks. This result may lead to innovative ways of accessing new cellular topologies by simple chemical tweaking of T-O-T angles.
一种在金属有机框架（MOF）中前所未有的新拓扑结构为揭示一系列新的多面体MOF提供了重要线索。我们报道了一种基于弗兰克 - 卡斯帕（FK）多面体，以简约拓扑结构结晶的新型MOF。四面体排列（T - O - T）中的角度分布对于拓扑结构中FK多面体的形成至关重要。这一发现促使我们研究相关沸石和沸石咪唑酯框架（ZIF）中的T - O - T角度分布。与沸石不同，在ZIF中极难实现高T - O - T角度，这阻碍了一些FK拓扑结构的形成。密度泛函理论（DFT）总能量计算支持T - O - T角度与基于新四面体的FK框架可行性之间的相关性。这一结果可能会带来通过简单化学调整T - O - T角度来获取新细胞拓扑结构的创新方法。
