Laboratory of Macromolecular and Organic Chemistry, Eindhoven University of Technology, PO Box 513, 5600 MB Eindhoven, The Netherlands.
Nat Chem. 2009 May;1(2):151-5. doi: 10.1038/nchem.177. Epub 2009 Apr 19.
Self-assembly offers the possibility to organize molecules in a given architecture through a subtle interplay between different noncovalent interactions. Although the kind of molecular association can often be predicted from information present in the individual molecules, the synthesis of supramolecular assemblies having a perfectly defined size and shape remains challenging. Here, we introduce the use of Coulombic interactions to control the supramolecular synthesis of finite, well-defined nanostructures. In particular, we demonstrate that the energy associated with the separation of ion pairs can regulate very precisely guanosine self-assembly into discrete G-quadruplexes. Assemblies comprising 8, 12, 16 or 24 guanosine molecules can be selectively and quantitatively obtained simply by tuning the stabilization of the dissociated anions in the solvent environment. Thus, factors such as solvent polarity, the nature of the anion and the cation-anion distance are shown to have a decisive role in the growth of G-quadruplexes.
自组装通过不同非共价相互作用之间的微妙相互作用提供了将分子组织在给定结构中的可能性。尽管可以根据单个分子中存在的信息来预测分子的结合类型，但具有精确定义的尺寸和形状的超分子组装的合成仍然具有挑战性。在这里，我们引入了使用库仑相互作用来控制有限的，定义明确的纳米结构的超分子合成。特别地，我们证明了与离子对分离相关的能量可以非常精确地调节鸟苷自组装成离散的 G-四链体。通过简单地调整溶剂环境中离解阴离子的稳定性，可以选择性和定量地获得包含 8、12、16 或 24 个鸟苷分子的组装体。因此，溶剂极性、阴离子的性质以及阳离子-阴离子距离等因素被证明在 G-四链体的生长中具有决定性作用。
