Carbon-Bonding Metal Catalysis (CBMC): A Supramolecular Complex Directs Structural-Isomer Selection in Gold-Catalyzed Reactions.
Carbon-Bonding Metal Catalysis (CBMC): A Supramolecular Complex Directs Structural-Isomer Selection in Gold-Catalyzed Reactions.
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DOI：
10.1021/jacs.3c07551
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发表时间：
2023-09
影响因子：
15
通讯作者：
Xinxin Li;Lingfei Hu;Gang Lu;Yao Wang
中科院分区：
文献类型：
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作者：
Xinxin Li;Lingfei Hu;Gang Lu;Yao Wang
碳是构成有机分子的主要元素，而金属催化是有机合成的基本工具。因此，在普遍存在的碳键和金属催化之间建立联系是一个根本性的重要问题。然而，目前还没有实验实例来介绍碳键在金属催化过程中的作用。在这里，我们将碳键和金属催化的主题合并在一起，证明超分子碳键金属配合物不仅可以产生催化活性，更值得注意的是，可以在金催化反应中直接产生结构异构体选择事件。实验结果揭示了这样一个事实：在金络合物上施加弱碳键相互作用可以改变卡宾以及这些催化剂的路易斯酸性质。这些结果说明了弱碳键相互作用在金属催化调节中的不可忽视的作用。因此，碳键金属催化不仅可用作反应开发的常规工具，而且更常用于分析金属催化反应过程。
Carbon is a primary element to constitute organic molecules, while metal catalysis is a basic tool in organic synthesis. The establishment of a link between the ubiquitous carbon bonding and metal catalysis is thus a fundamentally important problem. However, there is yet no experimental example to introduce the role of carbon bonding in a metal catalysis process. Herein, we merged the topics of carbon bonding and metal catalysis together and demonstrated that a supramolecular carbon-bonding metal complex can not only give rise to catalytic activity but, more remarkably, direct structural-isomer selection events in gold-catalyzed reactions. The experimental results unveil the fact that the imposing of weak carbon-bonding interactions on a gold complex can alter the carbene as well as the Lewis acid property of these catalysts. These results illustrate a non-negligible role of weak carbon-bonding interactions in the modulation of metal catalysis. As such, carbon-bonding metal catalysis is suggested to be used as a routine tool not only in the development of reactions but more frequently in analyzing reaction processes in metal catalysis.