Ghosh Amit, Paul Indrajit, Schmittel Michael
Center of Micro and Nanochemistry and Engineering, Organische Chemie I, University of Siegen, Adolf-Reichwein Strasse 2, 57068, Siegen, Germany.
Angew Chem Int Ed Engl. 2021 Sep 6;60(37):20558-20562. doi: 10.1002/anie.202108269. Epub 2021 Aug 7.
Reversible switching between the closed cyclic dimeric assembly [Cu (1) ] (OFF state) and the extended dimeric homoleptic complex [FeCu (1) ] (ON State) by addition/removal of Fe triggered catalysis of a double-click reaction and high yield preparation of [2]rotaxanes. Mechanistic and computational studies provide valuable general insight for double-click strategies by revealing cooperative effects in the second cycloaddition step due to a distance-tolerant preorganization of the first-click product by the two copper(I)-loaded phenanthroline subunits of [FeCu (1) ] .
通过添加/去除铁，在封闭的环状二聚体组装体[Cu(1)]（关闭状态）和扩展的二聚体同配络合物[FeCu(1)]（开启状态）之间进行可逆切换，引发了双点击反应的催化作用，并高产率地制备了[2]轮烷。机理和计算研究通过揭示由于[FeCu(1)]的两个负载铜(I)的菲咯啉亚基对首次点击产物的距离容忍性预组织，在第二次环加成步骤中产生的协同效应，为双点击策略提供了有价值的一般性见解。
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