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Towards homochiral supramolecular entities from achiral molecules by vortex mixing-accompanied self-assembly

机译:通过涡旋混合伴随自组装从非手性分子向同手性超分子实体发展

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摘要

Achieving homochirality is challenging both at the molecular and the supramolecular levels. While the origin of molecular homochirality still remains mysterious, the fabrication of homochiral assemblies from achiral molecules has attracted considerable interest since it provides many clues to understand the origin of molecular chirality. Here, by using a vortex mixing-accompanied self-assembly strategy, we obtained near-unity homochiral entities with controlled handedness from supramolecular gels that consist of exclusively achiral molecules without any chiral additives. The common supramolecular gelation process via heating and cooling of the achiral molecules only resulted in racemic gels. However, if vortex mixing is applied during the self-assembly, near-unity homochiral assemblies with uncontrolled handedness were obtained. Vortex mixing during the nucleation stage was found to be crucial in this case. On the other hand, if a small amount of the above vortex mixing produced assemblies was added as chiral seeds into the racemic gels, the racemic gels turned into near-unity homochiral suspensions with controlled handedness via a ripening process. Our studies provide an intriguing approach for achieving homochiral supramolecular assemblies from achiral molecules.
机译:在分子和超分子水平上,实现同手性都具有挑战性。尽管分子手性的起源仍然是个谜,但由非手性分子制造手性组装体却引起了极大的兴趣,因为它提供了许多线索来理解分子手性的起源。在这里,通过使用涡旋混合伴有的自组装策略,我们从超分子凝胶中获得了具有可控手性的近统一同手性实体,该分子由专门的非手性分子组成,没有任何手性添加剂。通过加热和冷却非手性分子的普通超分子凝胶化过程仅产生外消旋凝胶。但是,如果在自组装过程中进行涡旋混合,则会获得具有不受控制的旋性的近统一同手性组装。在这种情况下,在成核阶段的涡流混合至关重要。另一方面,如果将少量上述涡旋混合产生的组装体作为手性种子加入外消旋凝胶中,则外消旋凝胶通过成熟过程变成具有受控手性的近统一手性悬浮液。我们的研究提供了一种从非手性分子实现同手性超分子组装的有趣方法。

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