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

作　　者：Lei Zhu Hai-Ruo Li Yi-Ning Mao Ruiying Liu Bo Zhang Jing Chen Wengui Xu Libo Zhang Cheng-Peng Li 

机构地区：[1]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 [2]Tianjin Key Laboratory of Structure and Performance for Functional Molecules,College of Chemistry,Tianjin Normal University,Tianjin 300387,China [3]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

出　　处：《Chinese Chemical Letters》2024年第12期522-526,共5页中国化学快报（英文版）

基　　金：supported by National Natural Science Foundation of China(No.22171210);Research Project of Tianjin Education Commission(No.2023KJ182);Tianjin Research Innovation Project for Postgraduate Students(No.2022BKY200)。

摘　　要：The sequestration of^(99)Tc represents one of the most challenging tasks in nuclear waste decontamination In the event of a radioactive waste leak,^(99)TcO_(4)^(-)(a main form of^(99)Tc)would spread into the groundwa ter,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,featuring3D four-fold interpenetrated networks.TNU-143 exhibits efficient ReO_(4)^(-)(a nonradioactive analogue o^(99)TcO_(4)^(–))removal with fast anion exchange kinetics(<1 min),high sorption capacity(844 mg/g for ReO_(4)^(-))and outstanding selectivity over common anions.More importantly,TNU-143 shows superior stability in alkaline solution and can remove 91.6%ReO_(4)^(-)from simulated alkaline high-level waste(HLW)stream with solid-liquid ratio of 40 g/L.The uptake mechanism is elucidated by the single-crystal structure o TNU-143(Re),showing that ReO_(4)^(-)anions are firmly coordinated to nickel cation to result in a 2D lay ered 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 Re O_(4)^(-)/^(99)TcO_(4)^(-)from alkaline nulcear fuel using MOF sorbents.

关 键 词：Metal-organic framework Perrhenate/pertechnetate adsorption Single crystal to single crystal transformation Alkaline nuclear effluents 

分 类 号：X771[环境科学与工程—环境工程] TQ424[化学工程]