Hubei Key Laboratory of Bioinorganic Chemistry & Materia Medica, Hubei Engineering Research Center for Biomaterials and Medical Protective Materials, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, P. R. China.
Nat Commun. 2021 May 11;12(1):2659. doi: 10.1038/s41467-021-22984-6.
The communication of chirality at a molecular and supramolecular level is the fundamental feature capable of transmitting and amplifying chirality information. Yet, the limitation of one-step communication mode in many artificial systems has precluded the ability of further processing the chirality information. Here, we report the chirality communication of aromatic oligoamide sequences within the interpenetrated helicate architecture in a hierarchical manner, specifically, the communication is manipulated by three sequential steps: (i) coordination, (ii) concentration, and (iii) ion stimulus. Such approach enables the information to be implemented progressively and reversibly to different levels. Furthermore, the chiral information on the side chains can be accumulated and transferred to the helical backbones of the sequences, resulting in that one of ten possible diastereoisomers of the interpenetrated helicate is finally selected. The circular dichroism experiments with a mixture of chiral and achiral ligands demonstrate a cooperative behavior of these communications, leading to amplification of chiral information.
手性在分子和超分子水平上的传递是能够传递和放大手性信息的基本特征。然而,许多人工系统中一步传递模式的局限性限制了对手性信息的进一步处理。在这里,我们以分级的方式报告了在穿插螺旋结构内的芳香族寡酰胺序列的手性传递,具体而言,通过三个连续的步骤来操纵传递:(i)配位,(ii)浓度,和(iii)离子刺激。这种方法使得信息能够逐步和可逆地传递到不同的水平。此外,侧链上的手性信息可以被积累并转移到序列的螺旋骨架上,从而最终选择穿插螺旋结构的十种可能非对映异构体中的一种。带有手性和非手性配体的混合物的圆二色性实验证明了这些传递的协同行为,导致手性信息的放大。