Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, UK.
Global Phasing Ltd., Sheraton House, Castle Park, Cambridge CB3 0AX, UK.
Nat Chem. 2015 Apr;7(4):354-8. doi: 10.1038/nchem.2205.
Interlocked molecules possess properties and functions that depend upon their intricate connectivity. In addition to the topologically trivial rotaxanes, whose structures may be captured by a planar graph, the topologically non-trivial knots and catenanes represent some of chemistry's most challenging synthetic targets because of the three-dimensional assembly necessary for their construction. Here we report the synthesis of a cyclic [3]catenane, which consists of three mutually interpenetrating rings, via an unusual synthetic route. Five distinct building blocks self-assemble into a heteroleptic triangular framework composed of two joined Fe(II)3L3 circular helicates. Subcomponent exchange then enables specific points in the framework to be linked together to generate the cyclic [3]catenane product. Our method represents an advance both in the intricacy of the metal-templated self-assembly procedure and in the use of selective imine exchange to generate a topologically complex product.
互锁分子具有依赖于其复杂连接性的性质和功能。除了结构可以用平面图捕捉的拓扑平凡轮烷外，拓扑非平凡的结和索烃因其构建所需的三维组装而代表了化学中最具挑战性的合成目标之一。在这里，我们报告了一种通过不寻常的合成途径合成的由三个相互贯穿的环组成的环状[3]索烃。五个不同的构筑块自组装成一个由两个连接的 Fe(II)3L3 圆形螺旋体组成的杂配位三角形框架。然后，亚组分交换使框架中的特定点连接在一起，生成环状[3]索烃产物。我们的方法不仅在金属模板自组装过程的复杂性方面取得了进展，而且在使用选择性亚胺交换生成拓扑复杂的产物方面也取得了进展。
