Picking the lock of coordination cage catalysis.

Picking the lock of coordination cage catalysis.
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DOI:
10.1039/d3sc02586a
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发表时间:
2023-10-25
期刊:
影响因子:
8.4
通讯作者:
Lusby, Paul J.
Lusby, Paul J.
中科院分区:
化学1区
文献类型:
--
作者:
Piskorz, Tomasz K.;Marti-Centelles, Vicente;Spicer, Rebecca L.;Duarte, Fernanda;Lusby, Paul J.

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金属有机组装反应的设计原则使数百种不同尺寸和形状的配位笼易于使用。这些组装体中有许多具有明确定义的腔体,能够容纳来宾,形象地模仿底物与酶活性位点结合的作用。虽然现在有越来越多的配位笼显示出高度精通的催化作用,表现出出色的活性和高效的周转,但与已知的大量金属有机结构相比,这个数字仍然很小。在这篇综述中,我们将尝试分解和讨论构成有效配位笼催化剂的关键特征,利用从最著名的例子的实验和计算分析中吸取的经验教训,将结构与活性(和选择性)联系起来。我们还将对这一领域进行展望,解释为什么配位笼有可能成为(合成)非共价催化的黄金标准。我们提供了配位笼催化的概述,强调机理理解如何有助于解决该领域的挑战,从而为非共价反应性带来新的机遇。
The design principles of metallo-organic assembly reactions have facilitated access to hundreds of coordination cages of varying size and shape. Many of these assemblies possess a well-defined cavity capable of hosting a guest, pictorially mimicking the action of a substrate binding to the active site of an enzyme. While there are now a growing collection of coordination cages that show highly proficient catalysis, exhibiting both excellent activity and efficient turnover, this number is still small compared to the vast library of metal–organic structures that are known. In this review, we will attempt to unpick and discuss the key features that make an effective coordination cage catalyst, linking structure to activity (and selectivity) using lessons learnt from both experimental and computational analysis of the most notable exemplars. We will also provide an outlook for this area, reasoning why coordination cages have the potential to become the gold-standard in (synthetic) non-covalent catalysis. We provide an overview of coordination cage catalysis, highlighting how mechanistic understanding can help address the challenges in this area leading to new opportunities in non-covalent reactivity.
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