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Identifying the Recognition Site for Selective Trapping of 99TcO4- in a Hydrolytically Stable and Radiation Resistant Cationic Metal-Organic Framework

日期:2017-10-7 11:02:41 人气:5 


Abstract

   Effective and selective removal of 99TcO4- from aqueous solution is highly desirable for both waste partitioning and contamination remediation purposes in the modern nuclear fuel cycle, but is of significant challenge. We report here a hydrolytically stable and radiation resistant cationic metal-organic framework (MOF), SCU-101, exhibiting extremely fast removal kinetics, exceptional distribution coefficient, and high sorption capacity towards TcO4-. More importantly, this material can selectively remove TcO4- in the presence of large excesses of NO3- and SO42-, as even 6000 times of SO42- in excess does not significantly affect the sorption of TcO4-. These superior features endow that SCU-101 is capable of effectively separating TcO4- from Hanford low-level waste melter off-gas scrubber simulant stream. The sorption mechanism is directly unraveled by the single crystal structure of TcO4- incorporated SCU-101, as the first reported crystal structure to display TcO4- trapped in a sorbent material. A recognition site for the accommodation of TcO4- is visualized and is consistent with the DFT analysis results, while no such site can be resolved for other anions.