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用于选择性铯分离的可回收主体——共价连接的“异鸟嘌呤星”的设计与合成

Design and Synthesis of Covalently Tethered "IsoG-Star" as Recyclable Host for Selective Cesium Separation.

作者信息

Liu Mengjia, He Ying, Wojtas Lukasz, Shi Xiaodong

机构信息

Department of Chemistry, University of South Florida, Tampa, FL 33620 (USA).

出版信息

Green Chem. 2023 Nov 7;25(21):8494-8499. doi: 10.1039/d3gc02932h. Epub 2023 Oct 4.

Abstract

The isoguanosine self-assembled pentamer (isoG-star) has exhibited remarkable selectivity for Cs binding over competing alkali and alkali earth metal cation, rendering it a promising extractor for radioactive waste Cs separation. However, to make isoG-star a pracrtical material for Cs isolation, the development of recyclable isoG-star material is required. In this study, a systematic screening of functional isoG derivatives was performed. By employing well-defined complex formation and post-assembly modification, a covalently tethered isoG-star was prepared through olefin metathesis, utilizing a designed isoG monomer. The application of this newly developed covalently linked isoG-star enabled selective Cs extraction, followed by controled solvent-induced H-bond dessociation. This resulted in the creation of a recyclable Cs extractor, demonstrating excellent cation selectivity and good reusability (over seven cycles) the first time. Consequently, this new supramolecular macrocycle offers a practical new platform for the treatment of radiocesium (Cs and Cs) in an environmentally friendly and highly effective manner.

摘要

异鸟苷自组装五聚体(isoG-star)对铯的结合表现出对竞争性碱金属和碱土金属阳离子的显著选择性,使其成为放射性废物铯分离的有前途的萃取剂。然而,要使isoG-star成为用于铯分离的实用材料,需要开发可回收的isoG-star材料。在本研究中,对功能性异鸟苷衍生物进行了系统筛选。通过采用明确的络合形成和组装后修饰,利用设计的异鸟苷单体,通过烯烃复分解制备了共价连接的isoG-star。这种新开发的共价连接的isoG-star的应用实现了选择性铯萃取,随后通过可控的溶剂诱导氢键解离。这导致创建了一种可回收的铯萃取剂,首次展示了优异的阳离子选择性和良好的可重复使用性(超过七个循环)。因此,这种新的超分子大环为以环境友好和高效的方式处理放射性铯(铯-137和铯-134)提供了一个实用的新平台。

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