Self-assembly of tetravalent Goldberg polyhedra from 144 small components
Self-assembly of tetravalent Goldberg polyhedra from 144 small components
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DOI：
10.1038/nature20771
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发表时间：
2016-12-22
期刊：
影响因子：
64.8
通讯作者：
Fujita, Makoto
中科院分区：
文献类型：
--
作者：
Fujita, Daishi;Ueda, Yoshihiro;Fujita, Makoto
合理控制大型结构的自组装是化学中的关键挑战之一(1-9)，据信随着所涉及的组件数量的增加，这一挑战变得越来越困难，最终是不可能的。到目前为止，还不可能设计出由100多个组分组成的自组装离散分子。这类分子--例如球形病毒衣壳(10)--在自然界中普遍存在，这表明设计这些非常大的自组装分子的困难是由于缺乏对基本设计原理的理解。例如，通过考虑它们的拓扑结构(17)，实现了一系列包含多达30个钯离子与多达60个弯曲的有机配体(11-16)配位的一系列大型球形结构的定向组装。在这里，我们报告了一种球形结构的自组装，该结构还包含30个钯离子和60个弯曲的配体，但属于以前从未在实验中观察到的形状家族。新结构由8个三角形和24个正方形组成，具有四价Goldberg多面体(18，19)的对称性。柏拉图和阿基米德固体以前是通过自组装制备的，三价Goldberg多面体也是如此，它以病毒衣壳(20)和富勒烯(21)的形式自然出现。但是四价Goldberg多面体在分子水平上还没有报道，尽管它们的拓扑结构已经用图论预测过了。我们使用图论来预测更大的四价Goldberg多面体的自组装，它应该更稳定，使这个多面体家族的另一个成员能够由144个组分组装而成：48个钯离子和96个弯曲配体。
Rational control of the self-assembly of large structures is one of the key challenges in chemistry(1-9), and is believed to become increasingly difficult and ultimately impossible as the number of components involved increases. So far, it has not been possible to design a self-assembled discrete molecule made up of more than 100 components. Such molecules-for example, spherical virus capsids(10)-are prevalent in nature, which suggests that the difficulty in designing these very large self-assembled molecules is due to a lack of understanding of the underlying design principles. For example, the targeted assembly of a series of large spherical structures containing up to 30 palladium ions coordinated by up to 60 bent organic ligands(11-16) was achieved by considering their topologies(17). Here we report the self-assembly of a spherical structure that also contains 30 palladium ions and 60 bent ligands, but belongs to a shape family that has not previously been observed experimentally(17). The new structure consists of a combination of 8 triangles and 24 squares, and has the symmetry of a tetravalent Goldberg polyhedron(18,19). Platonic and Archimedean solids have previously been prepared through self-assembly, as have trivalent Goldberg polyhedra, which occur naturally in the form of virus capsids(20) and fullerenes(21). But tetravalent Goldberg polyhedra have not previously been reported at the molecular level, although their topologies have been predicted using graph theory. We use graph theory to predict the self-assembly of even larger tetravalent Goldberg polyhedra, which should be more stable, enabling another member of this polyhedron family to be assembled from 144 components: 48 palladium ions and 96 bent ligands.