Citation: Lei Zhu, Hai-Ruo Li, Yi-Ning Mao, Ruiying Liu, Bo Zhang, Jing Chen, Wengui Xu, Libo Zhang, Cheng-Peng Li. A four-fold interpenetrated MOF for efficient perrhenate/pertechnetate removal from alkaline nuclear effluents[J]. Chinese Chemical Letters, ;2024, 35(12): 109921. doi: 10.1016/j.cclet.2024.109921 shu

A four-fold interpenetrated MOF for efficient perrhenate/pertechnetate removal from alkaline nuclear effluents

Lei Zhu ^{a, 1} ,
Hai-Ruo Li ^{b, 1} ,
Yi-Ning Mao ^b ,
Ruiying Liu ^b ,
Bo Zhang ^{c, *,} ,
Jing Chen ^b ,
Wengui Xu ^a ,
Libo Zhang ^a ,
Cheng-Peng Li ^{b, *,}

a.
Department of Molecular Imaging and Nuclear Medicine, Tianjin Medical University Cancer Institute and Hospital, National Clinical Research Centre for Cancer, Tianjin's Clinical Research Centre for Cancer, Key Laboratory of Cancer Prevention and Therapy, Tianjin 300060, China
b.
Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry, Tianjin Normal University, Tianjin 300387, China
c.
Department of Breast Surgery, Shanxi Province Cancer Hospital, Shanxi Hospital Affiliated to Cancer Hospital & Chinese Academy of Medical Sciences, Cancer Hospital Affiliated to Shanxi Medical University, Taiyuan 030013, China

zhangbo.y@163.com

hxxylcp@tjnu.edu.cn

Received Date: 23 February 2024
Revised Date: 12 April 2024
Accepted Date: 23 April 2024
Available Online: 25 April 2024

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The sequestration of ⁹⁹Tc represents one of the most challenging tasks in nuclear waste decontamination. In the event of a radioactive waste leak, ⁹⁹TcO₄^– (a main form of ⁹⁹Tc) would spread into the groundwater, a scenario difficult to address with conventional anion exchange materials like resin and inorganic cationic sorbents. Herein, we present a nickel(Ⅱ) metal-organic framework (MOF), TNU-143, featuring 3D four-fold interpenetrated networks. TNU-143 exhibits efficient ReO₄^– (a nonradioactive analogue of ⁹⁹TcO₄^–) removal with fast anion exchange kinetics (< 1 min), high sorption capacity (844 mg/g for ReO₄^–), and outstanding selectivity over common anions. More importantly, TNU-143 shows superior stability in alkaline solution and can remove 91.6% ReO₄^– from simulated alkaline high-level waste (HLW) streams with solid-liquid ratio of 40 g/L. The uptake mechanism is elucidated by the single-crystal structure of TNU-143(Re), showing that ReO₄^– anions are firmly coordinated to nickel cation to result in a 2D layered structures. Density functional theory (DFT) calculations confirm the transformation from TNU-143 to TNU-143(Re) is a thermodynamically favorable process. This work presents a new approach to the removal of ReO₄^–/⁹⁹TcO₄^– from alkaline nulcear fuel using MOF sorbents.
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