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99 TcO 4 ? removal from legacy defense nuclear waste by an alkaline-stable 2D cationic metal organic framework

机译:99 TCO 4?通过碱性稳定的2D阳离子金属有机框架从遗留防御核废料中移除

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Removal of 99TcO4? from legacy defense nuclear tank waste at Savannah River Site is highly desirable for the purpose of nuclear safety and environmental protection, but currently not achievable given the extreme conditions including high alkalinity, high ionic strength, and strong radiation field. Herein, we present a potential solution to this long-term issue by developing a two-dimensional cationic metal organic framework SCU-103, showing ultrahigh stability in alkaline aqueous media and great resistance to both β and γ radiation. More importantly, it is very effective for 99TcO4? separation from aqueous media as demonstrated by fast exchange kinetics, high sorption capacity, and superior selectivity, leading to the successful removal of 99TcO4? from actual Savannah River Site high level tank waste for the first time, to the best of our knowledge. In addition, the uptake mechanism is comprehensively elucidated by molecular dynamics simulation and density functional theory calculation, showing a unique chemical recognition of anions with low charge density. Separation of 99TcO4? from nuclear waste at the Savannah River Site is hampered by the extreme conditions. Here, the authors propose a solution by developing an alkaline-resistant metal organic framework material featuring unique recognition sites for selective incorporation of 99TcO4? anions.
机译:去除99tCO4?从遗产防御核坦克垃圾处都非常适合核安全和环境保护目的,但鉴于包括高碱度,高离子强度和强辐射场的极端条件,目前无法实现。在此,我们通过开发二维阳离子金属有机框架SCU-103来提出这种长期问题的潜在解决方案,显示出碱性水性介质中的超高稳定性和对β和γ辐射的耐受耐受性的耐受性。更重要的是,它对于99TCO4非常有效?通过快速交换动力学,高吸附能力和优异的选择性,从水性培养基中分离,导致成功去除99tCO4?从实际的大草原河网站高层坦克浪费首次,据我们所知。此外,通过分子动力学模拟和密度泛函理论计算全面地阐明了摄取机制,显示了具有低电荷密度的阴离子的独特化学识别。分离99tCO4?从大草原河网站的核废料受到极端条件的阻碍。在这里,作者通过开发耐碱性金属有机骨架材料来提出解决方案,该耐含金金属有机骨架材料,用于选择性掺入99TCO4?阴离子。

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