Liao Yi-Yu, Li Jian-Rong, Zhang Bo, Sun Hai-Yan, Ma Wen, Jin Jian-Ce, Feng Mei-Ling, Huang Xiao-Ying
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, P. R. China.
University of Chinese Academy of Sciences, Beijing 100049, P. R. China.
ACS Appl Mater Interfaces. 2021 Feb 3;13(4):5275-5283. doi: 10.1021/acsami.0c21756. Epub 2021 Jan 26.
It is imperative yet challenging to efficiently sequester the Cs ion from aqueous solutions because of its highly environmental mobility and extremely high radiotoxicity. The systematical clarification for underlying mechanism of Cs removal and elution at the molecular level is rare. Here, efficient Cs capture is achieved by a thioantimonate [MeNH]SbS (FJSM-SbS) with high capacity, fast kinetics, wide pH durability, excellent β and γ radiation resistances, and facile elution. The Cs removal is not significantly impacted by coexisting Na, K, Ca, Mg, and Sr ions which is beneficial to the remediation of Cs-contaminated real waters. Importantly, the mechanism is directly illuminated by revealing an unprecedented single-crystal to single-crystal structural transformation upon Cs uptake and elution processes. The superior Cs removal results from an unusual synergy from strong affinity of soft S with Cs, easily exchangeable [MeNH] cations, and the flexible and robust framework of FJSM-SbS with open windows as trappers.
由于铯离子具有高度的环境迁移性和极高的放射性毒性,因此从水溶液中高效分离铯离子既迫切又具有挑战性。在分子水平上对铯去除和洗脱潜在机制进行系统的阐明很少见。在此,通过具有高容量、快速动力学、宽pH耐受性、优异的β和γ辐射抗性以及易于洗脱的硫代锑酸盐[MeNH]SbS(FJSM-SbS)实现了高效的铯捕获。共存的钠、钾、钙、镁和锶离子对铯的去除没有显著影响,这有利于对受铯污染的实际水体进行修复。重要的是,通过揭示在铯摄取和洗脱过程中前所未有的单晶到单晶结构转变,直接阐明了其机制。优异的铯去除效果源于软硫与铯的强亲和力、易于交换的[MeNH]阳离子以及具有作为捕集器的开放窗口的FJSM-SbS灵活而坚固的框架之间的异常协同作用。