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99TcO4− removal from legacy defense nuclear waste by an alkaline-stable 2D cationic metal organic framework

Author

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  • Nannan Shen

    (State Key Laboratory 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 University)

  • Zaixing Yang

    (State Key Laboratory 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 University)

  • Shengtang Liu

    (State Key Laboratory 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 University)

  • Xing Dai

    (State Key Laboratory 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 University)

  • Chengliang Xiao

    (College of Chemical and Biological Engineering, Zhejiang University)

  • Kathryn Taylor-Pashow

    (Savannah River National Laboratory)

  • Dien Li

    (Savannah River National Laboratory)

  • Chuang Yang

    (State Key Laboratory 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 University)

  • Jie Li

    (State Key Laboratory 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 University)

  • Yugang Zhang

    (State Key Laboratory 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 University)

  • Mingxing Zhang

    (State Key Laboratory 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 University)

  • Ruhong Zhou

    (State Key Laboratory 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 University)

  • Zhifang Chai

    (State Key Laboratory 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 University)

  • Shuao Wang

    (State Key Laboratory 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 University)

Abstract

Removal of 99TcO4− from legacy defense nuclear tank waste at Savannah River Site is highly desirable for the purpose of nuclear safety and environmental protection, but currently not achievable given the extreme conditions including high alkalinity, high ionic strength, and strong radiation field. Herein, we present a potential solution to this long-term issue by developing a two-dimensional cationic metal organic framework SCU-103, showing ultrahigh stability in alkaline aqueous media and great resistance to both β and γ radiation. More importantly, it is very effective for 99TcO4− separation from aqueous media as demonstrated by fast exchange kinetics, high sorption capacity, and superior selectivity, leading to the successful removal of 99TcO4− from actual Savannah River Site high level tank waste for the first time, to the best of our knowledge. In addition, the uptake mechanism is comprehensively elucidated by molecular dynamics simulation and density functional theory calculation, showing a unique chemical recognition of anions with low charge density.

Suggested Citation

  • Nannan Shen & Zaixing Yang & Shengtang Liu & Xing Dai & Chengliang Xiao & Kathryn Taylor-Pashow & Dien Li & Chuang Yang & Jie Li & Yugang Zhang & Mingxing Zhang & Ruhong Zhou & Zhifang Chai & Shuao Wa, 2020. "99TcO4− removal from legacy defense nuclear waste by an alkaline-stable 2D cationic metal organic framework," Nature Communications, Nature, vol. 11(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-19374-9
    DOI: 10.1038/s41467-020-19374-9
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    Cited by:

    1. Cheng-Rong Zhang & Wei-Rong Cui & Shun-Mo Yi & Cheng-Peng Niu & Ru-Ping Liang & Jia-Xin Qi & Xiao-Juan Chen & Wei Jiang & Xin Liu & Qiu-Xia Luo & Jian-Ding Qiu, 2022. "An ionic vinylene-linked three-dimensional covalent organic framework for selective and efficient trapping of ReO4− or 99TcO4−," Nature Communications, Nature, vol. 13(1), pages 1-8, December.

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