超分子化学
手性(物理)
超分子手性
同手性
化学
螺旋(腹足类)
结晶学
高分子
折叠(DSP实现)
金属
配位复合体
自组装
圆二色性
对映体
立体化学
晶体结构
有机化学
蜗牛
电气工程
工程类
物理
生物
量子力学
生物化学
手征对称破缺
Nambu–Jona Lasinio模型
生态学
夸克
作者
Huimin Duan,Jiawei Li,Jingling Xue,Dongming Qi
出处
期刊:Biomacromolecules
[American Chemical Society]
日期:2022-12-23
卷期号:24 (1): 344-357
标识
DOI:10.1021/acs.biomac.2c01165
摘要
Although the supramolecular helical structures of biomacromolecules have been studied, the examples of supramolecular systems that are assembled using coils to form helical polymer chains are still limited. Inspired by enhanced helical chirality at the supramolecular level in metal coordination-induced protein folding, a series of alanine-based coil copolymers (poly-(l-co-d)-ala-NH2) carrying (l)- and (d)-alanine pendants were synthesized as a fresh research model to study the cooperative processes between homochirality property and metal coordination. The complexes of poly-(l-co-d)-ala-NH2 and metal ions underwent a coil-to-helix transition and exhibited remarkable nonlinear effects based on the enantiomeric excess of the monomer unit in the copolymers, affording enhanced helical chirality compared to poly-(l-co-d)-ala-NH2. More importantly, the synergistic effect of amplification of asymmetry and metal coordination triggered the formation of a helical molecular orbital on the polymer backbone via the coordination with the d orbital of copper ions. Thus, the helical chirality enhancement degree of poly-(l-co-d)-ala-NH2/Cu2+ complexes (31.4) is approximately 3 times higher than that of poly-(l-co-d)-ala-NH2/Ag+ complexes (9.8). This study not only provides important mechanistic insights into the enhancement of helical chirality for self-assembly but also establishes a new strategy for studying the homochiral amplification of asymmetry in biological supramolecular systems.
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