Liang Xiaotong, Zhao Ting, Shen Yanling, Fang Lizhi, Chen Long, Zhou Dayang, Wu Wanhua, Yang Cheng
Key Laboratory of Green Chemistry and Technology of Ministry of Education, College of Chemistry and State Key Laboratory of Biotherapy, Sichuan University, Chengdu, 610064, China.
Changjiang River Scientifc Research Institute of Changjiang Water Resources Commission, Wuhan, 430010, China.
Angew Chem Int Ed Engl. 2025 Jan 27;64(5):e202416975. doi: 10.1002/anie.202416975. Epub 2024 Nov 9.
Achieving high enantioselectivity with synthetic receptors, particularly in water, remains a significant challenge despite the success seen in natural biological systems. In this study, we introduce a facile synthesis of Tröger's base (TB)-containing macrocyclic arenes (TBn), where TB units are linked via methylene bridges, providing the macrocycles with a rigid framework. Oxidation of enantiopure TBn yields corresponding chiral nitrogen oxides (TBnNO) with excellent water solubility, attributed to the high polarity of the N-O bond, surpassing the pH limitations of traditional ion-functionalized approaches. Remarkably, TBnNO exhibits exceptional enantioselective recognition toward a wide range of chiral guests in aqueous solution, achieving enantioselectivities as high as 41.0. The underlying mechanism involves a combination of hydrophobic interactions and steric effects caused by rigid chiral cavities. These findings highlight the potential of nitrogen-oxidized macrocycles as a transformative tool for supramolecular application in water.
尽管在天然生物系统中取得了成功,但利用合成受体实现高对映选择性,尤其是在水中实现高对映选择性,仍然是一项重大挑战。在本研究中,我们介绍了一种简便的合成方法,用于制备含特罗格碱(TB)的大环芳烃(TBn),其中TB单元通过亚甲基桥相连,为大环提供了刚性骨架。对映纯的TBn氧化生成相应的手性氮氧化物(TBnNO),其具有优异的水溶性,这归因于N-O键的高极性,超越了传统离子功能化方法的pH限制。值得注意的是,TBnNO在水溶液中对多种手性客体表现出卓越的对映选择性识别,对映选择性高达41.0。其潜在机制涉及刚性手性空腔引起的疏水相互作用和空间效应的结合。这些发现突出了氮氧化大环作为水中超分子应用的变革性工具的潜力。