基于铪的金属有机骨架作为一种受自然启发的串联反应催化剂。
A Hafnium-Based Metal-Organic Framework as a Nature-Inspired Tandem Reaction Catalyst.
机构信息
International Institute for Nanotechnology (IIN) and Center for the Chemistry of Integrated Systems (CCIS), Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States.
Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota , 207 Pleasant Street SE, Minneapolis, Minnesota 55455, United States.
出版信息
J Am Chem Soc. 2015 Oct 28;137(42):13624-31. doi: 10.1021/jacs.5b08440. Epub 2015 Oct 15.
Tandem catalytic systems, often inspired by biological systems, offer many advantages in the formation of highly functionalized small molecules. Herein, a new metal-organic framework (MOF) with porphyrinic struts and Hf6 nodes is reported. This MOF demonstrates catalytic efficacy in the tandem oxidation and functionalization of styrene utilizing molecular oxygen as a terminal oxidant. The product, a protected 1,2-aminoalcohol, is formed selectively and with high efficiency using this recyclable heterogeneous catalyst. Significantly, the unusual regioselective transformation occurs only when an Fe-decorated Hf6 node and the Fe-porphyrin strut work in concert. This report is an example of concurrent orthogonal tandem catalysis.
串联催化体系常常受到生物体系的启发，在构建高官能化小分子方面具有许多优势。在此，我们报道了一种具有卟啉骨架和 Hf6 节点的新型金属有机骨架（MOF）。该 MOF 可以在苯乙烯的串联氧化和官能化反应中利用分子氧作为末端氧化剂表现出催化活性。使用这种可回收的多相催化剂，可以选择性地、高效地合成保护的 1,2-氨基醇。重要的是，只有当 Fe 修饰的 Hf6 节点和 Fe-卟啉骨架协同作用时，才会发生这种非寻常的区域选择性转化。本报告是同时发生的正交串联催化的一个例子。
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