Spatiotemporal control and superselectivity in supramolecular polymers using multivalency
Spatiotemporal control and superselectivity in supramolecular polymers using multivalency
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DOI：
10.1073/pnas.1303109110
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发表时间：
2013-07-23
影响因子：
11.1
通讯作者：
Meijer, E. W.
中科院分区：
文献类型：
--
作者：
Albertazzi, Lorenzo;Martinez-Veracoechea, Francisco J.;Meijer, E. W.
多价态在分子自组织中有着重要但知之甚少的作用。我们提出了一种多组分超分子聚合物的非共价合成，其中化学上不同的单体自发地共组装成一个动态的，功能性的结构。我们发现，一个多价的招聘是能够选择性地结合到一个子集的单体（受体），并触发他们的集群沿着自组装聚合物，行为模仿筏形成细胞膜。这种现象是可逆的，并提供超选择性结合的单链DNA带正电荷的受体的超分子聚合物内的单体分布的时空控制。我们的研究结果揭示了多价性在使水溶性超分子聚合物的结构有序性和非线性识别中的关键作用，并且它为功能性的、结构定义的超分子结构提供了设计原则。
Multivalency has an important but poorly understood role in molecular self-organization. We present the noncovalent synthesis of a multicomponent supramolecular polymer in which chemically distinct monomers spontaneously coassemble into a dynamic, functional structure. We show that a multivalent recruiter is able to bind selectively to one subset of monomers (receptors) and trigger their clustering along the self-assembled polymer, behavior that mimics raft formation in cell membranes. This phenomenon is reversible and affords spatiotemporal control over the monomer distribution inside the supramolecular polymer by superselective binding of single-strand DNA to positively charged receptors. Our findings reveal the pivotal role of multivalency in enabling structural order and nonlinear recognition in water-soluble supramolecular polymers, and it offers a design principle for functional, structurally defined supramolecular architectures.