Chiral Frustrated Lewis Pair@Metal‐Organic Framework as a New Platform for Heterogeneous Asymmetric Hydrogenation
Chiral Frustrated Lewis Pair@Metal‐Organic Framework as a New Platform for Heterogeneous Asymmetric Hydrogenation
复制标题
手性受阻路易斯对@金属有机框架作为多相不对称氢化的新平台
DOI：
10.1002/anie.202213399
复制
发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Ma, Shengqian
中科院分区：
文献类型：
--
作者：
Zhang, Yin;Chen, Songbo;Al‐Enizi, Abdullah M.;Nafady, Ayman;Tang, Zhiyong;Ma, Shengqian
不对称氢化是合成手性分子的一种开创性的策略，但在多相催化剂的非金属中心的活化方面，它在很大程度上仍未得到满足。本文通过理论计算和实验研究相结合的方法，提出了一种将合理设计的分子手性受阻Lewis对(CFLP)与多孔金属有机骨架(MOF)相结合，构建能有效促进多相不对称加氢反应的催化剂CFLP@MOF的一般策略，首次将手性受阻Lewis对的概念从均相体系扩展到多相催化体系。值得注意的是，开发的CFLP@MOF继承了均相和多相催化剂的优点，具有高活性/对映体选择性和良好的回收/再生性能。我们的工作不仅推动了CFLP@MOF作为多相不对称加氢反应新平台的发展，也为设计和制备先进的不对称催化催化剂开辟了一条新的途径。
Asymmetric hydrogenation, a seminal strategy for the synthesis of chiral molecules, remains largely unmet in terms of activation by non‐metal sites of heterogeneous catalysts. Herein, as demonstrated by combined computational and experimental studies, we present a general strategy for integrating rationally designed molecular chiral frustrated Lewis pair (CFLP) with porous metal–organic framework (MOF) to construct the catalyst CFLP@MOF that can efficiently promote the asymmetric hydrogenation in a heterogeneous manner, which for the first time extends the concept of chiral frustrated Lewis pair from homogeneous system to heterogeneous catalysis. Significantly, the developed CFLP@MOF, inherits the merits of both homogeneous and heterogeneous catalysts, with high activity/enantio‐selectivity and excellent recyclability/regenerability. Our work not only advances CFLP@MOF as a new platform for heterogeneous asymmetric hydrogenation, but also opens a new avenue for the design and preparation of advanced catalysts for asymmetric catalysis.