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Highly Stable Mesoporous Zirconium Porphyrinic Frameworks with Distinct Flexibility

机译:具有高度灵活性的高度稳定的介孔锆卟啉骨架

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摘要

The construction of highly stable metal-porphyrinic frameworks (MPFs) is appealing as these materials offer great opportunities for applications in artificial light-harvesting systems, gas storage, heterogeneous catalysis, etc. Herein, we report the synthesis of a novel mesoporous metal-porphyrinic framework (denoted as NUPF-1) and its catalytic properties. NUPF-1 is constructed from a new porphyrin linker and a Zr6O8 structural building unit, possessing an unprecedented doubly interpenetrating scu net. The structure exhibits not only remarkable chemical and thermal stabilities, but also a distinct structural flexibility, which is seldom seen in metal-organic framework (MOF) materials. By the merit of high chemical stability, NUPF-1 could be easily post-metallized with [Ru-3(CO)(12)], and the resulting {NUPF-1-RuCO} is catalytically active as a heterogeneous catalyst for intermolecular C(sp(3))-H amination. Excellent yields and good recyclability for amination of small substrates with various organic azides have been achieved.
机译:高度稳定的金属-卟啉骨架(MPF)的构建吸引人,因为这些材料为在人工光收集系统,气体存储,非均相催化等方面的应用提供了巨大的机会。在此,我们报道了新型介孔金属-卟啉的合成骨架(表示为NUPF-1)及其催化性能。 NUPF-1由新的卟啉连接子和Zr6O8结构建筑单元构成,具有前所未有的双重互穿网络。该结构不仅具有出色的化学和热稳定性,而且还具有独特的结构柔性,这在金属有机骨架(MOF)材料中很少见。由于具有高化学稳定性的优点,NUPF-1可以很容易地用[Ru-3(CO)(12)]后金属化,所得的{NUPF-1-RuCO}具有催化活性,可作为分子间C的非均相催化剂(sp(3))-H胺化。对于用各种有机叠氮化物胺化小的基材,已经实现了极好的产率和良好的可回收性。

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