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Successful Decontamination of 99TcO4- in Groundwater at Legacy Nuclear Sites by a Cationic Metal-Organic Framework with Hydrophobic Pockets

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [3];  [4];  [5];  [6];  [3];  [4];  [3];  [7];  [5];  [3];  [3]
  1. Soochow Univ., Suzhou (China); University of Notre Dame
  2. Southwest Univ. of Science and Technology Sichuan Mianyang (China)
  3. Soochow Univ., Suzhou (China)
  4. Tsinghua Univ., Beijing (China)
  5. Northwestern Univ., Evanston, IL (United States)
  6. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  7. Southwest Univ. of Science and Technology Sichuan Mianyang (China)
+ Show Author Affiliations
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.
Research Organization:
Univ. of Notre Dame, IN (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
NA0003763
OSTI ID:
1529892
Alternate ID(s):
OSTI ID: 22813793
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 15 Vol. 58; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (12)

[Ln 6 O 8 ] Cluster‐Encapsulating Polyplumbites as New Polyoxometalate Members and Record Inorganic Anion‐Exchange Materials for ReO 4 − Sequestration journal June 2019
Ammoniating Covalent Organic Framework (COF) for High‐Performance and Selective Extraction of Toxic and Radioactive Uranium Ions journal June 2019
Pore‐Surface Engineering by Decorating Metal‐Oxo Nodes with Phenylsilane to Give Versatile Super‐Hydrophobic Metal–Organic Frameworks (MOFs) journal April 2019
An Ultrastable Metal Azolate Framework with Binding Pockets for Optimal Carbon Dioxide Capture journal September 2019
Three Mechanisms in One Material: Uranium Capture by a Polyoxometalate–Organic Framework through Combined Complexation, Chemical Reduction, and Photocatalytic Reduction journal September 2019
A Layered Cationic Aluminum Oxyhydroxide as a Highly Efficient and Selective Trap for Heavy Metal Oxyanions journal June 2020
Pore‐Surface Engineering by Decorating Metal‐Oxo Nodes with Phenylsilane to Give Versatile Super‐Hydrophobic Metal–Organic Frameworks (MOFs) journal May 2019
An Ultrastable Metal Azolate Framework with Binding Pockets for Optimal Carbon Dioxide Capture journal November 2019
Three Mechanisms in One Material: Uranium Capture by a Polyoxometalate-Organic Framework through Combined Complexation, Chemical Reduction, and Photocatalytic Reduction journal September 2019
A Layered Cationic Aluminum Oxyhydroxide as a Highly Efficient and Selective Trap for Heavy Metal Oxyanions journal June 2020
Waste cigarette filters: activated carbon as a novel sorbent for uranium removal journal April 2019
Specific recognition of toxic allyl alcohol by pore-functionalized metal–organic frameworks journal January 2020

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12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES