Enabling Homochirality and Hydrothermal Stability in Zn4O-Based Porous Crystals,Journal of the American Chemical Society

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Enabling Homochirality and Hydrothermal Stability in Zn4O-Based Porous Crystals
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-10-16 , DOI: 10.1021/jacs.8b08316
Xiang Zhao _{1,

2} , Huajun Yang ₁ , Edward T. Nguyen ₁ , Joshua Padilla ₁ , Xitong Chen ₂ , Pingyun Feng ₂ , Xianhui Bu ₁

Affiliation

The [Zn4O]6+ cluster is well-known to form the archetypal MOF-5 topology with dicarboxylate ligands. Here we report two new materials (CPM-300 and -301) that show dramatic alteration of topological and chemical behaviors of [Zn4O]6+ clusters. In CPM-300, [Zn4O]6+ untypically forms the MIL-88/MOF-235 type framework with a small pentane-ring-based chiral dicarboxylate. In contrast, in CPM-301, when mediated by [Zn9(btz)12]6+ clusters (btz = benzotriazolate), the MOF-5 topology is regenerated with the same chiral ligand, albeit with alternating [Zn4O]6+ and [Zn9(btz)12]6+ clusters. Importantly, both CPM-300 and CPM-301 are homochiral, hydrothermally stable in boiling water and alcohol, and thermally stable to 440 °C or higher. It is concluded that small methyl groups on the chiral ligand is sufficiently powerful to shield [Zn4O]6+ clusters from degradation by water, even at high temperatures. These results reveal a promising platform for the development of a new class of cluster-based homochiral and hydrothermally stable porous materials.

中文翻译：

实现 Zn4O 基多孔晶体的同手性和水热稳定性

众所周知，[Zn4O]6+ 簇与二羧酸盐配体形成典型的 MOF-5 拓扑结构。在这里，我们报告了两种新材料（CPM-300 和 -301），它们显示出 [Zn4O]6+ 簇的拓扑和化学行为的显着改变。在 CPM-300 中，[Zn4O]6+ 与一个小的基于戊烷环的手性二羧酸盐不典型地形成 MIL-88/MOF-235 型骨架。相比之下，在 CPM-301 中，当由 [Zn9(btz)12]6+ 簇（btz = 苯并三唑酸盐）介导时，MOF-5 拓扑结构使用相同的手性配体再生，尽管 [Zn4O]6+ 和 [Zn4O]6+ 和 [ Zn9(btz)12]6+ 簇。重要的是，CPM-300 和 CPM-301 都是同手性的，在沸水和酒精中水热稳定，在 440°C 或更高温度下热稳定。结论是手性配体上的小甲基基团足以保护 [Zn4O]6+ 簇免受水降解，即使在高温下也是如此。这些结果为开发一类新的基于簇的单手性和水热稳定多孔材料提供了一个有前景的平台。

更新日期：2018-10-16

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