Successful Decontamination of 99 TcO 4 in Groundwater at Legacy Nuclear Sites by a Cationic Metal-Organic Framework with Hydrophobic Pockets

Daopeng Sheng, Lin Zhu, Xing Dai, Chao Xu, Peng Li, Carolyn I. Pearce, Chengliang Xiao*, Jing Chen, Ruhong Zhou, Tao Duan, Omar K. Farha, Zhifang Chai, Shuao Wang

*Corresponding author for this work

Research output: Contribution to journalArticle

45 Scopus citations

Abstract

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.

Original languageEnglish (US)
Pages (from-to)4968-4972
Number of pages5
JournalAngewandte Chemie - International Edition
Volume58
Issue number15
DOIs
StatePublished - Apr 1 2019

Keywords

  • anion exchange
  • cationic frameworks
  • metal-organic frameworks
  • nuclear waste
  • pertechnetate

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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