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J Am Chem Soc. 2017 Oct 25;139(42):14873-14876. doi: 10.1021/jacs.7b08632. Epub 2017 Oct 11.

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

Author information

1
School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , Suzhou 215123, China.
2
Collaborative Innovation Center of Advanced Nuclear Energy Technology, Institute of Nuclear and New Energy Technology, Tsinghua University , Beijing 100084, China.
3
Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States.
4
School of Materials Science and Engineering, Anhui University of Science and Technology , Huainan 232001, China.
5
Department of Chemistry, Faculty of Science, King Abdulaziz University , Jeddah 21589, Saudi Arabia.
6
Department of Chemistry and Biochemistry, Florida State University , 95 Chieftain Way, Tallahassee, Florida 32306, United States.

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 toward 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.

PMID:
28985681
DOI:
10.1021/jacs.7b08632

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