High-Throughput Discovery of a Rhombohedral Twelve-Connected Zirconium-Based Metal-Organic Framework with Ordered Terephthalate and Fumarate Linkers.
High-Throughput Discovery of a Rhombohedral Twelve-Connected Zirconium-Based Metal-Organic Framework with Ordered Terephthalate and Fumarate Linkers.
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DOI：
10.1002/anie.202108150
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发表时间：
2021-12-20
影响因子：
16.6
通讯作者：
Rosseinsky, Matthew J.
中科院分区：
文献类型：
--
作者：
Tollitt, Adam M.;Vismara, Rebecca;Daniels, Luke M.;Antypov, Dmytro;Gaultois, Michael W.;Katsoulidis, Alexandros P.;Rosseinsky, Matthew J.
关键词：
我们报告了一种金属有机框架，其中两个具有不同长度和几何形状的连接体的有序阵列将 [Zr6(OH)4O4]12+ 簇连接成十二连接的 fcu 网络，该网络从立方对称性发生菱面体扭曲。等量的对苯二甲酸酯和富马酸酯二位羧酸连接基在三角反棱柱形 Zr6 核心处有序结合，形成富马酸酯连接簇的密堆积层，这些簇通过对苯二甲酸酯沿单个剩余的三重轴连接。这种明确的连接体排列保留了基于 Zr 簇的 UiO 家族的三维孔隙率，同时在通道内创建了两个不同的窗口，定义了两个不同的客体扩散路径。有序材料是通过高通量合成确定的成分和工艺参数的有限组合来获得的。对苯二甲酸酯和富马酸酯连接体在 fcu 网上的有序排列产生了具有两个不同窗口和多个客体扩散路径的锆基 MOF Zr6(BDC)3(Fum)3。该相是在可用化学空间的狭窄区域中通过单步合成形成的，其识别需要大量的合成实验，而这些实验是通过自动化高通量方法来促进的。
We report a metal‐organic framework where an ordered array of two linkers with differing length and geometry connect [Zr6(OH)4O4]12+ clusters into a twelve‐connected fcu net that is rhombohedrally distorted from cubic symmetry. The ordered binding of equal numbers of terephthalate and fumarate ditopic carboxylate linkers at the trigonal antiprismatic Zr6 core creates close‐packed layers of fumarate‐connected clusters that are connected along the single remaining threefold axis by terephthalates. This well‐defined linker arrangement retains the three‐dimensional porosity of the Zr cluster‐based UiO family while creating two distinct windows within the channels that define two distinct guest diffusion paths. The ordered material is accessed by a restricted combination of composition and process parameters that were identified by high‐throughput synthesis. The ordered arrangement of terephthalate and fumarate linkers over the fcu net produces a zirconium‐based MOF Zr6(BDC)3(Fum)3 with two distinct windows and multiple guest diffusion pathways. This phase is formed by single‐step synthesis in a narrow region of the available chemical space, and its identification required a large set of synthetic experiments that were facilitated by automated high‐throughput methods.
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