Multivariate Metal–Organic Frameworks as Multifunctional Heterogeneous Asymmetric Catalysts for Sequential Reactions,Journal of the American Chemical Society

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Multivariate Metal–Organic Frameworks as Multifunctional Heterogeneous Asymmetric Catalysts for Sequential Reactions
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2017-06-06 , DOI: 10.1021/jacs.7b03113
Qingchun Xia ₁ , Zijian Li ₁ , Chunxia Tan ₁ , Yan Liu ₁ , Wei Gong ₁ , Yong Cui _{1,

2}

Affiliation

The search for versatile heterogeneous catalysts with multiple active sites for broad asymmetric transformations has long been of great interest, but it remains a formidable synthetic challenge. Here we demonstrate that multivariate metal-organic frameworks (MTV-MOFs) can be used as an excellent platform to engineer heterogeneous catalysts featuring multiple and cooperative active sites. An isostructural series of 2-fold interpenetrated MTV-MOFs that contain up to three different chiral metallosalen catalysts was constructed and used as efficient and recyclable heterogeneous catalysts for a variety of asymmetric sequential alkene epoxidation/epoxide ring-opening reactions. Interpenetration of the frameworks brings metallosalen units adjacent to each other, allowing cooperative activation, which results in improved efficiency and enantioselectivity over the sum of the individual parts. The fact that manipulation of molecular catalysts in MTV-MOFs can control the activities and selectivities would facilitate the design of novel multifunctional materials for enantioselective processes.

中文翻译：

多元金属-有机框架作为用于顺序反应的多功能多相不对称催化剂

长期以来，人们对寻找具有多个活性位点的多功能多相催化剂进行广泛的不对称转化一直很感兴趣，但它仍然是一个艰巨的合成挑战。在这里，我们证明了多元金属有机框架 (MTV-MOF) 可用作设计具有多个协同活性位点的多相催化剂的绝佳平台。构建了包含多达三种不同手性金属盐催化剂的 2 倍互穿 MTV-MOF 的同构系列，并将其用作各种不对称顺序烯烃环氧化/环氧化物开环反应的高效且可回收的多相催化剂。框架的相互渗透使金属盐单元彼此相邻，允许协同激活，这导致在单个部分的总和上提高效率和对映选择性。在 MTV-MOF 中操纵分子催化剂可以控制活性和选择性的事实将有助于设计用于对映选择性过程的新型多功能材料。

更新日期：2017-06-06

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