Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Molecular Recognition and Function, Institute of Chemistry, Chinese Academy of Sciences, 100190, Beijing, China.
University of Chinese Academy of Sciences, 100049, Beijing, China.
Nat Commun. 2020 Dec 7;11(1):6257. doi: 10.1038/s41467-020-20081-8.
Xenon binding has attracted interest due to the potential for xenon separation and emerging applications in magnetic resonance imaging. Compared to their covalent counterparts, assembled hosts that are able to effectively bind xenon are rare. Here, we report a tight yet soft chiral macrocycle dimeric capsule for efficient and adaptive xenon binding in both crystal form and solution. The chiral bisurea-bisthiourea macrocycle can be easily synthesized in multi-gram scale. Through assembly, the flexible macrocycles are locked in a bowl-shaped conformation and buckled to each other, wrapping up a tight, completely sealed yet adjustable cavity suitable for xenon, with a very high affinity for an assembled host. A slow-exchange process and drastic spectral changes are observed in both H and Xe NMR. With the easy synthesis, modification and reversible characteristics, we believe the robust yet adaptive assembly system may find applications in xenon sequestration and magnetic resonance imaging-based biosensing.
氙气结合因其在氙气分离方面的潜力以及在磁共振成像方面的新兴应用而受到关注。与共价对应物相比，能够有效结合氙气的组装主体很少。在这里，我们报告了一种紧密而柔软的手性大环二聚体胶囊，可在晶体形式和溶液中有效且自适应地结合氙气。手性双脲-双硫脲大环可以很容易地在多克规模下合成。通过组装，柔性大环被锁定在碗形构象中并相互扣合，形成一个紧密、完全密封但可调节的空腔，适合氙气，对组装主体具有很高的亲和力。在 H 和 Xe NMR 中都观察到缓慢交换过程和剧烈的光谱变化。由于具有易于合成、修饰和可逆的特点，我们相信这种坚固而自适应的组装系统可能在氙气捕获和基于磁共振成像的生物传感方面有应用。
