Wang Wei, Li Xinxin, Zhou Pan-Pan, Wang Yao
School of Chemistry and Chemical Engineering, Key Laboratory of the Colloid and Interface Chemistry, Ministry of Education, Shandong University, Jinan, 250100, China.
Key Laboratory of Advanced Catalysis of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, China.
Angew Chem Int Ed Engl. 2021 Oct 11;60(42):22717-22721. doi: 10.1002/anie.202108973. Epub 2021 Sep 13.
Herein, we describe a new catalysis platform, supramolecular carbon-bonding catalysis, which exploits the highly directional weak interactions between carbon centers of catalysts and electron donors to drive chemical reactions. To demonstrate this catalysis approach, we discovered a class of cyclopropane derivatives incorporated with carbonyl, ester and cyano groups as catalysts which showed general catalysis capability in different types of benchmark reactions. Among these typical examples, a challenging tail-to-head terpene cyclization can be achieved by supramolecular carbon-bonding catalysis. The co-crystal structures of catalyst and electron donors, comparison experiments, and titrations support a catalysis mode of carbon-bonding activation of Lewis basic reactants.
在此，我们描述了一种新的催化平台——超分子碳键催化，它利用催化剂的碳中心与电子供体之间高度定向的弱相互作用来驱动化学反应。为了证明这种催化方法，我们发现了一类含有羰基、酯基和氰基的环丙烷衍生物作为催化剂，它们在不同类型的基准反应中表现出普遍的催化能力。在这些典型例子中，超分子碳键催化可以实现具有挑战性的头对头萜烯环化反应。催化剂与电子供体的共晶体结构、对比实验和滴定实验支持了路易斯碱性反应物的碳键活化催化模式。
