Self-Assembled M24L48 Polyhedra and Their Sharp Structural Switch upon Subtle Ligand Variation
Self-Assembled M24L48 Polyhedra and Their Sharp Structural Switch upon Subtle Ligand Variation
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DOI：
10.1126/science.1188605
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发表时间：
2010-05-28
期刊：
影响因子：
56.9
通讯作者：
Fujita, Makoto
中科院分区：
文献类型：
--
作者：
Sun, Qing-Fu;Iwasa, Junji;Fujita, Makoto
自组装是一种自下而上构建离散的、定义明确的纳米级结构的强大技术。大型多组分系统（具有50多个组分）提供了对生物组装的机械见解，但也提出了令人生畏的合成挑战。本文报道了由24个钯离子（M）和48个弯曲桥连配体（L）自组装形成的M24L48巨配位球。该多组分体系的结构对弯曲配体的几何形状高度敏感。即使配体弯曲角的微小变化也会严重地切换在M24 L48和M12 L24配位球之间的整个结构单元系综上观察到的最终结构。这种微小的初始差异放大为结果结构中不可忽视的差异是涌现行为的关键标志。
Self-assembly is a powerful technique for the bottom-up construction of discrete, well-defined nanoscale structures. Large multicomponent systems (with more than 50 components) offer mechanistic insights into biological assembly but present daunting synthetic challenges. Here we report the self-assembly of giant M24L48 coordination spheres from 24 palladium ions (M) and 48 curved bridging ligands (L). The structure of this multicomponent system is highly sensitive to the geometry of the bent ligands. Even a slight change in the ligand bend angle critically switches the final structure observed across the entire ensemble of building blocks between M24L48 and M12L24 coordination spheres. The amplification of this small initial difference into an incommensurable difference in the resultant structures is a key mark of emergent behavior.