99TcO4-remediation by a cationic polymeric network

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

doi:10.1038/s41467-018-05380-5

Title: ⁹⁹TcO₄^-remediation by a cationic polymeric network

Journal Article · 01 August 2018 · Nature Communications

DOI: https://doi.org/10.1038/s41467-018-05380-5 · OSTI ID:1464461

Li, Jie ^[1]; Dai, Xing ^[2]; Zhu, Lin ^[2]; Xu, Chao ^[3]; Zhang, Duo ^[2];

^[2];

^[4]; Chen, Lanhua ^[2]; Li, Yongzhong ^[5]; Zuo, Douwen ^[6]; Zhang, Hui ^[7]; Xiao, Chengliang ^[2]; Chen, Jing ^[3]; Diwu, Juan ^[2]; Farha, Omar K. ^[8]; Albrecht-Schmitt, Thomas E. ^[9]; Chai, Zhifang ^[2]; Wang, Shuao ^[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
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
Tsinghua Univ., Beijing (China). Collaborative Innovation Center of Advanced Nuclear Energy Technology, Inst. of Nuclear and New Energy Technology
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Suzhou CNNC Huadong Radiation Co., Suzhou (China)
CGN Dasheng Electron Accelerator Technology Co., Suzhou (China)
Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Microsystem and Information Technology, State Key Lab. of Functional Materials for Informatics
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; King Abdulaziz Univ., Jeddah (Saudi Arabia). Dept. of Chemistry, Faculty of Science
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.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST); University 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, Vol. 9, 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; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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