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通过分子间氢原子转移机制的钌催化脱氢反应。

Ruthenium-Catalyzed Dehydrogenation Through an Intermolecular Hydrogen Atom Transfer Mechanism.

作者信息

Huang Lin, Bismuto Alessandro, Rath Simon A, Trapp Nils, Morandi Bill

机构信息

Max-Planck-Institut für Kohlenforschung, Kaiser-Wihelm-Platz 1, 45470, Mülheim an der Ruhr, Germany.

Laboratorium für Organische Chemie ETH Zürich, Vladimir-Prelog-Weg 3, HCI, 8093, Zürich, Switzerland.

出版信息

Angew Chem Int Ed Engl. 2021 Mar 22;60(13):7290-7296. doi: 10.1002/anie.202015837. Epub 2021 Feb 25.

Abstract

The direct dehydrogenation of alkanes is among the most efficient ways to access valuable alkene products. Although several catalysts have been designed to promote this transformation, they have unfortunately found limited applications in fine chemical synthesis. Here, we report a conceptually novel strategy for the catalytic, intermolecular dehydrogenation of alkanes using a ruthenium catalyst. The combination of a redox-active ligand and a sterically hindered aryl radical intermediate has unleashed this novel strategy. Importantly, mechanistic investigations have been performed to provide a conceptual framework for the further development of this new catalytic dehydrogenation system.

摘要

烷烃的直接脱氢是获得有价值烯烃产物的最有效方法之一。尽管已经设计了几种催化剂来促进这种转化,但遗憾的是,它们在精细化学合成中的应用有限。在此,我们报告了一种使用钌催化剂进行催化、分子间烷烃脱氢的概念上新颖的策略。氧化还原活性配体和空间位阻芳基自由基中间体的结合开启了这一新颖策略。重要的是,已经进行了机理研究,为进一步开发这种新的催化脱氢系统提供了概念框架。

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