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

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:
Grant/Contract Number:
NA0003763
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
Research Org:
Univ. of Notre Dame, IN (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA)
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
OSTI Identifier:
1464461

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., 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. 2018. "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}
}

Works referenced in this record:

An Isoreticular Series of Metal-Organic Frameworks with Dendritic Hexacarboxylate Ligands and Exceptionally High Gas-Uptake Capacity
journal, June 2010
  • Yuan, Daqiang; Zhao, Dan; Sun, Daofeng
  • Angewandte Chemie International Edition, Vol. 49, Issue 31, p. 5357-5361
  • DOI: 10.1002/anie.201001009

Metal–organic framework materials as catalysts
journal, January 2009
  • Lee, JeongYong; Farha, Omar K.; Roberts, John
  • Chemical Society Reviews, Vol. 38, Issue 5, p. 1450-1459
  • DOI: 10.1039/b807080f

Systematic Design of Pore Size and Functionality in Isoreticular MOFs and Their Application in Methane Storage
journal, January 2002
  • Eddaoudi, Mohamed; Kim, Jaheon; Rosi, Nathaniel
  • Science, Vol. 295, Issue 5554, p. 469-472
  • DOI: 10.1126/science.1067208

Carbon Dioxide Capture in Metal–Organic Frameworks
journal, September 2011
  • Sumida, Kenji; Rogow, David L.; Mason, Jarad A.
  • Chemical Reviews, Vol. 112, Issue 2, p. 724-781
  • DOI: 10.1021/cr2003272

Hydrogen storage in metal–organic frameworks
journal, January 2009
  • Murray, Leslie J.; Dincă, Mircea; Long, Jeffrey R.
  • Chemical Society Reviews, Vol. 38, Issue 5, p. 1294-1314
  • DOI: 10.1039/b802256a

Introduction to Metal–Organic Frameworks
journal, September 2011
  • Zhou, Hong-Cai; Long, Jeffrey R.; Yaghi, Omar M.
  • Chemical Reviews, Vol. 112, Issue 2, p. 673-674
  • DOI: 10.1021/cr300014x

Metal–Organic Framework Materials as Chemical Sensors
journal, September 2011
  • Kreno, Lauren E.; Leong, Kirsty; Farha, Omar K.
  • Chemical Reviews, Vol. 112, Issue 2, p. 1105-1125
  • DOI: 10.1021/cr200324t

Selective gas adsorption and separation in metal–organic frameworks
journal, January 2009
  • Li, Jian-Rong; Kuppler, Ryan J.; Zhou, Hong-Cai
  • Chemical Society Reviews, Vol. 38, Issue 5, p. 1477-1504
  • DOI: 10.1039/b802426j

Science and technology for water purification in the coming decades
journal, March 2008
  • Shannon, Mark A.; Bohn, Paul W.; Elimelech, Menachem
  • Nature, Vol. 452, Issue 7185, p. 301-310
  • DOI: 10.1038/nature06599

Contracted Gaussian basis sets for molecular calculations. I. Second row atoms, Z=11–18
journal, May 1980
  • McLean, A. D.; Chandler, G. S.
  • The Journal of Chemical Physics, Vol. 72, Issue 10, p. 5639-5648
  • DOI: 10.1063/1.438980

Self—Consistent Molecular Orbital Methods. XII. Further Extensions of Gaussian—Type Basis Sets for Use in Molecular Orbital Studies of Organic Molecules
journal, March 1972
  • Hehre, W. J.; Ditchfield, R.; Pople, J. A.
  • The Journal of Chemical Physics, Vol. 56, Issue 5, p. 2257-2261
  • DOI: 10.1063/1.1677527