One-Step Synthesis of One-Dimensional Supramolecular Assemblies Composed of Helical Macromolecular Building Blocks,Journal of the American Chemical Society

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One-Step Synthesis of One-Dimensional Supramolecular Assemblies Composed of Helical Macromolecular Building Blocks
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2019-08-13 , DOI: 10.1021/jacs.9b07417
Yuya Wada ₁ , Ken-Ichi Shinohara ₂ , Hitoshi Asakawa _{1,

3,

4} , Sayaka Matsui ₁ , Tetsuya Taima _{1,

3} , Tomoyuki Ikai _{1,

5}

Affiliation

Living systems achieve sophisticated functions using supramolecular protein assemblies, in which the protein building blocks possess a specific secondary structure and are noncovalently arranged in a preprogrammed manner. Herein, we demonstrate the one-step synthesis of one-dimensional macromolecular assemblies by simply mixing a glycine-based isocyanide with a nickel catalyst, in which helical constituent polymers are linked end-to-end through multiple hydrogen bonds. The applicable scope of this approach is not confined to a particular monomer bearing a specially designed pendant, but covers a wide range of glycine-based isocyanides with or without aromatic and other functional groups. Surprisingly, copolymerization with an analogous chiral isocyanide (1 mol%) afforded an almost perfect one-handed helical supramolecular fiber owing to intramolecular/intermolecular dual chiral amplifications. The simplicity and broad applicability of this approach, which can also afford exquisite chiral amplification, enable the creation of a wide variety of functional supramolecular assemblies and provides access to new supramolecular materials.

中文翻译：

由螺旋大分子积木组成的一维超分子组装体的一步合成

生命系统使用超分子蛋白质组件实现复杂的功能，其中蛋白质构建块具有特定的二级结构，并以预编程的方式非共价排列。在此，我们展示了通过简单地将甘氨酸基异氰化物与镍催化剂混合来一步合成一维大分子组装体，其中螺旋组成的聚合物通过多个氢键首尾相连。这种方法的适用范围不限于带有专门设计的侧链的特定单体，而是涵盖了各种带有或不带有芳香族和其他官能团的甘氨酸基异氰化物。出奇，由于分子内/分子间双手性放大，与类似的手性异氰化物（1 mol％）共聚提供了几乎完美的单手螺旋超分子纤维。这种方法的简单性和广泛的适用性，也可以提供精美的手性放大，能够创建各种功能性超分子组件，并提供对新超分子材料的访问。

更新日期：2019-08-13

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