Guanidinium-Responsive Crown Ether-Based Macrocyclic Amphiphile in Aqueous Medium
Guanidinium-Responsive Crown Ether-Based Macrocyclic Amphiphile in Aqueous Medium
复制标题
水介质中胍响应性冠醚基大环两亲物
DOI：
10.1021/acs.jpclett.0c02994
复制
发表时间：
2021-07-30
影响因子：
5.7
通讯作者：
Qi, Zhenhui
中科院分区：
文献类型：
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作者：
Pan, Tiezheng;Li, Jiangbo;Qi, Zhenhui
基于低聚乙二醇(OEG)构筑块的超分子组装体以其中性的化学性质和热响应行为而闻名。在这里，循环的“封闭的”和线性的“开放”类型的OEGs导致了对含胍物种的敏感度的显著差异。热力学研究表明，“封闭”型两亲分子与胍盐的结合常数(K-a)为28.7M-1，而“开放”型两亲分子则没有明显的结合亲和力。因此，考虑到离子的特异性，本研究结果表明，具有“封闭”和“开放”拓扑结构的冠醚衍生物提供了一个易于获取的模型对，具有设计的离子识别位置和特殊的功能部分和几何结构(如细胞成员中的酶或离子通道的结合口袋)，允许操纵超分子溶质、水和胍盐之间的交叉关系。这些水溶液中的超分子作用力为制备离子介质中的热响应体系提供了一种替代策略。
Supramolecular assemblies based on oligo(ethylene glycol) (OEG) building blocks are well-known for their neutral chemical property and thermal-responsive behavior. Here, the cyclic "CLOSED" and linear "OPEN" typologies of OEGs led to dramatic difference in the sensitivity to guanidinium-containing species. From thermodynamic studies, the association constant (K-a) between the "CLOSED" form amphiphile and guanidinium salt was determined to be 28.7 M-1, whereas there was no detectable binding affinity for the "OPEN" form. Therefore, considering ion specificity, the present results establish that crown ether derivatives with "CLOSED" and "OPEN" topologies provide an easy-to-access model pair with designed ion-recognition sites and special functional moieties and geometries (like the binding pockets of enzymes or ion channels in cellular members) that allow the manipulation of the intercrossed relationship between supramolecular solutes, waters, and guanidinium salts. These supramolecular forces in aqueous solution offered an alternative strategy to fabricate thermal-responsive systems in ionic medium.