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Successful Decontamination of 99 TcO 4 − in Groundwater at Legacy Nuclear Sites by a Cationic Metal‐Organic Framework with Hydrophobic Pockets
Author(s) -
Sheng Daopeng,
Zhu Lin,
Dai Xing,
Xu Chao,
Li Peng,
Pearce Carolyn I.,
Xiao Chengliang,
Chen Jing,
Zhou Ruhong,
Duan Tao,
Farha Omar K.,
Chai Zhifang,
Wang Shuao
Publication year - 2019
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201814640
Subject(s) - human decontamination , cationic polymerization , chemistry , sorption , environmental remediation , radioactive waste , ion exchange , scavenger , selectivity , metal , inorganic chemistry , radiochemistry , contamination , nuclear chemistry , ion , adsorption , organic chemistry , radical , waste management , engineering , ecology , catalysis , biology
99 Tc contamination at legacy nuclear sites is a serious and unsolved environmental issue. The selective remediation of 99 TcO 4 − in the presence of a large excess of NO 3 − and SO 4 2− from natural waste systems represents a significant scientific and technical challenge, since anions with a higher charge density are often preferentially sorbed by traditional anion‐exchange materials. We present a solution to this challenge based on a stable cationic metal‐organic framework, SCU‐102 (Ni 2 (tipm) 3 (NO 3 ) 4 ), which exhibits fast sorption kinetics, a large capacity (291 mg g −1 ), a high distribution coefficient, and, most importantly, a record‐high TcO 4 − uptake selectivity. This material can almost quantitatively remove TcO 4 − in the presence of a large excess of NO 3 − and SO 4 2− . Decontamination experiments confirm that SCU‐102 represents the optimal Tc scavenger with the highest reported clean‐up efficiency, while first‐principle simulations reveal that the origin of the selectivity is the recognition of TcO 4 − by the hydrophobic pockets of the structure.