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

Abstract

99Tc contamination at legacy nuclear sites is a serious and unsolved environmental issue. The selective remediation of 99TcO 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-. Finally, 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.

Authors:
 [1]; ORCiD logo [2];  [1]; ORCiD logo [3];  [4];  [5]; ORCiD logo [1];  [3]; ORCiD logo [1]; ORCiD logo [6];  [4];  [1]; ORCiD logo [1]
  1. Soochow Univ., Suzhou (China)
  2. Southwest Univ. of Science and Technology Sichuan Mianyang (China)
  3. Tsinghua Univ., Beijing (China)
  4. Northwestern Univ., Evanston, IL (United States)
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  6. Southwest Univ. of Science and Technology Sichuan Mianyang (China)
Publication Date:
Research Org.:
Univ. of Notre Dame, IN (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1529892
Grant/Contract Number:  
NA0003763
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 58; Journal Issue: 15; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES

Citation Formats

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, and Wang, Shuao. Successful Decontamination of 99TcO4- in Groundwater at Legacy Nuclear Sites by a Cationic Metal-Organic Framework with Hydrophobic Pockets. United States: N. p., 2019. Web. doi:10.1002/anie.201814640.
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. Successful Decontamination of 99TcO4- in Groundwater at Legacy Nuclear Sites by a Cationic Metal-Organic Framework with Hydrophobic Pockets. United States. doi:10.1002/anie.201814640.
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, and Wang, Shuao. Tue . "Successful Decontamination of 99TcO4- in Groundwater at Legacy Nuclear Sites by a Cationic Metal-Organic Framework with Hydrophobic Pockets". United States. doi:10.1002/anie.201814640.
@article{osti_1529892,
title = {Successful Decontamination of 99TcO4- in Groundwater at Legacy Nuclear Sites by a Cationic Metal-Organic Framework with Hydrophobic Pockets},
author = {Sheng, Daopeng and Zhu, Lin and Dai, Xing and Xu, Chao and Li, Peng and Pearce, Carolyn I. and Xiao, Chengliang and Chen, Jing and Zhou, Ruhong and Duan, Tao and Farha, Omar K. and Chai, Zhifang and Wang, Shuao},
abstractNote = {99Tc contamination at legacy nuclear sites is a serious and unsolved environmental issue. The selective remediation of 99TcO4- in the presence of a large excess of NO3- and SO42- 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 (Ni2(tipm)3(NO3)4), which exhibits fast sorption kinetics, a large capacity (291 mg g1), a high distribution coefficient, and, most importantly, a record-high TcO4 - uptake selectivity. This material can almost quantitatively remove TcO4- in the presence of a large excess of NO3- and SO42-. Finally, 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 TcO4- by the hydrophobic pockets of the structure.},
doi = {10.1002/anie.201814640},
journal = {Angewandte Chemie (International Edition)},
number = 15,
volume = 58,
place = {United States},
year = {2019},
month = {3}
}

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