Cascading transformations within a dynamic self-assembled system

Cascading transformations within a dynamic self-assembled system
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DOI:
10.1038/nchem.693
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发表时间:
2010-08-01
期刊:
影响因子:
21.8
通讯作者:
Nitschke, Jonathan R.
Nitschke, Jonathan R.
中科院分区:
化学1区
文献类型:
--
作者:
Campbell, Victoria E.;de Hatten, Xavier;Nitschke, Jonathan R.

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磷酸基团等分子亚组分通常在复杂的信号级联过程中在生物分子之间传递,其流动定义了生命机器的运动。在这里,我们展示了一个由金属离子配位编织在一起的有机子成分组成的非生物系统如何以复杂的方式对简单的信号做出反应。在加入锌(II)后,Cu-3(I)螺旋酸盐转化为其(Zn 2CuI)-Cu-II类似物,并且排出的铜(I)继续诱导溶液中存在的其他游离子组分自组装成Cu-2(I)螺旋酸盐。添加额外的子组分8-氨基喹啉,导致形成第三种更稳定的Cu-3(I)螺旋酸盐,需要破坏(Zn 2CuI)-Cu-II和Cu-2(I)螺旋酸盐以获得足够的Cu-I用于新结构。因此,该系统演示了两个例子,其中一个信号的应用引起两个不同的响应,涉及复杂组件的创建或破坏,因为系统在扰动后寻求热力学平衡。
Molecular subcomponents such as phosphate groups are often passed between biomolecules during complex signalling cascades, the flow of which define the motion of the machinery of life. Here, we show how an abiological system consisting of organic subcomponents knitted together by metal-ion coordination can respond to simple signals in complex ways. A Cu-3(I) helicate transformed into its (Zn2CuI)-Cu-II analogue following the addition of zinc(II), and the ejected copper(I) went on to induce the self-assembly of a Cu-2(I) helicate from other free subcomponents present in solution. The addition of an additional subcomponent, 8-aminoquinoline, resulted in the formation of a third, more stable Cu-3(I) helicate, requiring the destruction of both the (Zn2CuI)-Cu-II and Cu-2(I) helicates to scavenge sufficient Cu-I for the new structure. This system thus demonstrates two examples in which the application of one signal provokes two distinct responses involving the creation or destruction of complex assemblies as the system seeks thermodynamic equilibrium following perturbation.