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99TcO4-remediation by a cationic polymeric network

Journal Article · · Nature Communications
 [1];  [2];  [2];  [3];  [2];  [2];  [4];  [2];  [5];  [6];  [7];  [2];  [3];  [2];  [8];  [9];  [2];  [2]
  1. Soochow Univ., Suzhou (China). State Key Lab. of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions; University of Notre Dame
  2. Soochow Univ., Suzhou (China). State Key Lab. of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions
  3. Tsinghua Univ., Beijing (China). Collaborative Innovation Center of Advanced Nuclear Energy Technology, Inst. of Nuclear and New Energy Technology
  4. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  5. Suzhou CNNC Huadong Radiation Co., Suzhou (China)
  6. CGN Dasheng Electron Accelerator Technology Co., Suzhou (China)
  7. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Microsystem and Information Technology, State Key Lab. of Functional Materials for Informatics
  8. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; King Abdulaziz Univ., Jeddah (Saudi Arabia). Dept. of Chemistry, Faculty of Science
  9. Florida State Univ., Tallahassee, FL (United States). Dept. of Chemistry and Biochemistry
Direct removal of 99TcO4- from the highly acidic solution of used nuclear fuel is highly beneficial for the recovery of uranium and plutonium and more importantly aids in the elimination of 99Tc discharge into the environment. However, this task represents a huge challenge given the combined extreme conditions of super acidity, high ionic strength, and strong radiation field. Here in this paper we overcome this challenge using a cationic polymeric network with significant TcO4- uptake capabilities in four aspects: the fastest sorption kinetics, the highest sorption capacity, the most promising uptake performance from highly acidic solutions, and excellent radiation-resistance and hydrolytic stability among all anion sorbent materials reported. In addition, this material is fully recyclable for multiple sorption/desorption trials, making it extremely attractive for waste partitioning and emergency remediation. The excellent TcO4 - uptake capability is elucidated by X-ray absorption spectroscopy, solidstate NMR measurement, and density functional theory analysis on anion coordination and bonding.
Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST); Univ. of Notre Dame, IN (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
NA0003763
OSTI ID:
1464461
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 9; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (16)

Anion-adaptive crystalline cationic material for 99TcO4− trapping journal April 2019
Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption journal April 2019
Emerging Functional Porous Polymeric and Carbonaceous Materials for Environmental Treatment and Energy Storage journal November 2019
Functionalized Porous Aromatic Frameworks as High‐Performance Adsorbents for the Rapid Removal of Boric Acid from Water journal February 2019
Successful Decontamination of 99 TcO 4 in Groundwater at Legacy Nuclear Sites by a Cationic Metal‐Organic Framework with Hydrophobic Pockets journal March 2019
A Layered Cationic Aluminum Oxyhydroxide as a Highly Efficient and Selective Trap for Heavy Metal Oxyanions journal June 2020
Successful Decontamination of 99 TcO 4 in Groundwater at Legacy Nuclear Sites by a Cationic Metal-Organic Framework with Hydrophobic Pockets journal March 2019
A Layered Cationic Aluminum Oxyhydroxide as a Highly Efficient and Selective Trap for Heavy Metal Oxyanions journal June 2020
Phosphonate modified MoS2 composite material for effective adsorption of uranium(VI) in aqueous solution journal December 2019
Super-resolution imaging of non-fluorescent reactions via competition journal July 2019
Ultra-highly selective trapping of perrhenate/pertechnetate by a flexible cationic coordination framework journal January 2019
Highly efficient adsorption of uranium( vi ) from aqueous solution by a novel adsorbent: titanium phosphate nanotubes journal January 2018
Macroscopic and microscopic investigation of uranium elimination by Ca–Mg–Al-layered double hydroxide supported nanoscale zero valent iron journal January 2018
Exceptional TcO 4 sorption capacity and highly efficient ReO 4 luminescence sensing by Zr 4+ MOFs journal January 2018
Construction of a cationic organic network for highly efficient removal of anionic contaminants from water journal January 2019
Mechanism unravelling for ultrafast and selective 99 TcO 4 uptake by a radiation-resistant cationic covalent organic framework: a combined radiological experiment and molecular dynamics simulation study journal January 2019

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