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Title: 99TcO 4 -remediation by a cationic polymeric network

Abstract

Direct removal of 99TcO 4 - 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 TcO 4 - 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 TcO 4 - uptake capability is elucidated by X-ray absorption spectroscopy, solidstate NMR measurement, and density functional theory analysis on anion coordination and bonding.

Authors:
 [1];  [2];  [2];  [3];  [2]; ORCiD logo [2]; ORCiD logo [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
  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
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST); Univ. of Notre Dame, IN (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1464461
Grant/Contract Number:  
NA0003763
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Related Information: Electronic supplementary information (ESI) available: Experimental details, adsorption capacity data, PXRD patterns, nitrogen isotherms, and SEM images. CCDC 1843055 and 1843056. For ESI and crystallographic data in CIF or other electronic format see DOI: 10.1039/c8ce00992a; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE

Citation Formats

Li, Jie, Dai, Xing, Zhu, Lin, Xu, Chao, Zhang, Duo, Silver, Mark A., Li, Peng, Chen, Lanhua, Li, Yongzhong, Zuo, Douwen, Zhang, Hui, Xiao, Chengliang, Chen, Jing, Diwu, Juan, Farha, Omar K., Albrecht-Schmitt, Thomas E., Chai, Zhifang, and Wang, Shuao. 99TcO4-remediation by a cationic polymeric network. United States: N. p., 2018. Web. doi:10.1038/s41467-018-05380-5.
Li, Jie, Dai, Xing, Zhu, Lin, Xu, Chao, Zhang, Duo, Silver, Mark A., Li, Peng, Chen, Lanhua, Li, Yongzhong, Zuo, Douwen, Zhang, Hui, Xiao, Chengliang, Chen, Jing, Diwu, Juan, Farha, Omar K., Albrecht-Schmitt, Thomas E., Chai, Zhifang, & Wang, Shuao. 99TcO4-remediation by a cationic polymeric network. United States. doi:10.1038/s41467-018-05380-5.
Li, Jie, Dai, Xing, Zhu, Lin, Xu, Chao, Zhang, Duo, Silver, Mark A., Li, Peng, Chen, Lanhua, Li, Yongzhong, Zuo, Douwen, Zhang, Hui, Xiao, Chengliang, Chen, Jing, Diwu, Juan, Farha, Omar K., Albrecht-Schmitt, Thomas E., Chai, Zhifang, and Wang, Shuao. Wed . "99TcO4-remediation by a cationic polymeric network". United States. doi:10.1038/s41467-018-05380-5. https://www.osti.gov/servlets/purl/1464461.
@article{osti_1464461,
title = {99TcO4-remediation by a cationic polymeric network},
author = {Li, Jie and Dai, Xing and Zhu, Lin and Xu, Chao and Zhang, Duo and Silver, Mark A. and Li, Peng and Chen, Lanhua and Li, Yongzhong and Zuo, Douwen and Zhang, Hui and Xiao, Chengliang and Chen, Jing and Diwu, Juan and Farha, Omar K. and Albrecht-Schmitt, Thomas E. and Chai, Zhifang and Wang, Shuao},
abstractNote = {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.},
doi = {10.1038/s41467-018-05380-5},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {8}
}

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    • DOI: 10.1039/c8cc09364d

    Super-resolution imaging of non-fluorescent reactions via competition
    journal, July 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

    • Sheng, Daopeng; Zhu, Lin; Dai, Xing
    • Angewandte Chemie International Edition, Vol. 58, Issue 15
    • DOI: 10.1002/anie.201814640

    Anion-adaptive crystalline cationic material for 99TcO4− trapping
    journal, April 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

    • Li, Cheng-Peng; Ai, Jin-Yun; Zhou, Hang
    • Chemical Communications, Vol. 55, Issue 12
    • DOI: 10.1039/c8cc09364d