Department of Chemistry , Boston College , Chestnut Hill , Massachusetts 02467 , United States.
School of Physical Science and Technology , ShanghaiTech University , Shanghai 201210 , People's Republic of China.
J Am Chem Soc. 2018 Jul 5;140(26):8082-8085. doi: 10.1021/jacs.8b04047. Epub 2018 Jun 22.
The aperture-opening process resulting from dissociative linker exchange in zirconium-based metal-organic framework (MOF) UiO-66 was used to encapsulate the ruthenium complex (PNP)Ru(CO)HCl in the framework (PNP = 2,6-bis((di- tert-butyl-phosphino)methyl)pyridine). The resulting encapsulated complex, [Ru]@UiO-66, was a very active catalyst for the hydrogenation of CO to formate. Unlike the analogous homogeneous catalyst, [Ru]@UiO-66 could be recycled five times, showed no evidence for bimolecular catalyst decomposition, and was less prone to catalyst poisoning. These results demonstrated for the first time how the aperture-opening process in MOFs can be used to synthesize host-guest materials useful for chemical catalysis.
基于锆的金属-有机骨架（MOF）UiO-66 中离解连接体交换导致的孔径打开过程被用于将钌配合物（PNP）Ru（CO）HCl 封装在骨架中（PNP = 2,6-双（（二-叔丁基膦基）甲基）吡啶）。所得封装的配合物 [Ru]@UiO-66 是 CO 加氢形成甲酸盐的非常活跃的催化剂。与类似的均相催化剂不同，[Ru]@UiO-66 可以回收使用五次，没有双分子催化剂分解的证据，并且不易受到催化剂中毒。这些结果首次证明了 MOFs 中的孔径打开过程如何可用于合成用于化学催化的主客体材料。
