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

Lin Zhu, Daopeng Sheng, Chao Xu, Xing Dai, Mark A. Silver, Jie Li, Peng Li, Yaxing Wang, Yanlong Wang, Lanhua Chen, Chengliang Xiao*, Jing Chen, Ruhong Zhou, Chao Zhang, Omar K. Farha, Zhifang Chai, Thomas E. Albrecht-Schmitt, Shuao Wang

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

207 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)14873-14876
Number of pages4
JournalJournal of the American Chemical Society
Volume139
Issue number42
DOIs
StatePublished - Oct 25 2017

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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