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首页> 外文期刊>Chemistry: A European journal >Helicate,Macrocycle,or Catenate:Dynamic Topological Control over Subcomponent Self-Assembly
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Helicate,Macrocycle,or Catenate:Dynamic Topological Control over Subcomponent Self-Assembly

机译：Helicate，Macrocycle或Catenate：子组件自组装的动态拓扑控制

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摘要

The aqueous reaction between equimolar amounts of 2-(2-(2-aminoethoxy)ethoxy)ethanamine,1,10-phenanthroline-2,9-dialdehyde and copper(I)produced a dimeric helical macrocycle in quantitative yield.This ring could also be generated by the addition of two equivalents of the diamine to an acyclic helicate containing four mono-imine residues:A transimi-nation occurred,the chelate effect being implicated as a driving force.In the case of a helicate containing mono-imines derived from anilines,the substitution of diamine for monoamine was reversible upon lowering the pH.The aliphatic diamine was protonated at a higher pH than the arylamine,which left the arylamine free for incorporation instead of the alkyl diamine.This reaction thus opened the possibility of switching between closed macro-cyclic and open helicate topologies by changing the pH.An additional closed topology became accessible through the use of a diamine that incorporates two rigid phenylene spacer groups between a flexible chain and the imine-forming nitrogen atoms.The resulting catenate consists of a pair of topologi-cally interlinked macrocycles.The presence of the phenylene groups appeared to dictate the topology of the final product,making the formation of a single macrocycle energetically disfavoured.
机译：等摩尔量的2-（2-（2-（2-氨基乙氧基）乙氧基）乙胺，1,10-菲咯啉-2,9-二醛与铜（I）之间的水反应产生了定量的二聚螺旋大环。通过在含有四个单亚胺残基的无环螺旋物中加入两当量的二胺而生成：发生了半透明反应，螯合效应被认为是驱动力。降低pH值可逆地用二胺代替单胺。脂肪族二胺在比芳基胺更高的pH下被质子化，从而使芳基胺可以自由地引入而不是烷基二胺。该反应因此提供了在之间切换的可能性通过改变pH值可以实现封闭的大环和螺旋状开放拓扑。通过使用在二胺之间引入两个刚性亚苯基间隔基的二胺，可以获得另一种封闭的拓扑亚硝酸根和亚胺形成的氮原子。所得的门酸盐由一对拓扑-羧基相互连接的大环组成。亚苯基的存在似乎决定了最终产物的拓扑结构，使单个大环的形成受到强烈的不利影响。

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