Polymer-on-HOF:a new strategy for fabricating“armour-plated”HOFs to sequester radioactive anions  

作　　者：Hai-Ruo Li Shitao Wu Xuezhuo Jing Zhengyi Di Kun Liu Lu Wang Cheng-Peng Li Zhong Liu Miao Du 

机构地区：[1]College of Chemistry,Tianjin Key Laboratory of Structure and Performance for Functional Molecules,Tianjin Normal University,Tianjin 300387,China [2]Shanghai Key Laboratory of High-Resolution Electron Microscopy,School of Physical Science and Technology,ShanghaiTech University,Shanghai 201210,China [3]Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources,Qinghai Provincial Key Laboratory of Resources and Chemistry of Salt Lakes,Qinghai Institute of Salt Lakes,Chinese Academy of Sciences,Xining 810008,China [4]College of Material and Chemical Engineering,Institute of New Energy Science and Technology,School of Future Hydrogen Energy Technology,Zhengzhou University of Light Industry,Zhengzhou 450001,China

出　　处：《Science China Chemistry》2024年第9期2958-2967,共10页中国科学（化学英文版）

基　　金：supported by the National Natural Science Foundation of China(22171210,21771139,U20A20141,U23A20119);CAS Project for Young Scientists in Basic Research(YSBR-039);Tianjin Research Innovation Project for Postgraduate Students(2022BKY200);C?EM,School of Physical Sciences and Technology,Shanghai Tech University(#EM02161943)for the scientific and financial support of EM facilities。

摘　　要：The development of hydrogen-bonded organic frameworks(HOFs)faces significant constraints,primarily attributed to their fragile architectures and limited functionalization capabilities.To overcome these limitations,this work presents a new polymeron-HOF strategy by covalently tethering armor-like polymers onto the surface of HOFs.The application of this approach not only bolsters the stability of HOFs,but also facilitates the customization of their functional expansion in radionuclide sequestration.The optimized HOF-polymer materials display extraordinary ability in radionuclide sequestration,achieving uptake of I^(-)(0.699 g g^(-1)),IO_(3)^(-)(0.285 g g^(-1))and ReO_(4)^(-)(1.616 g g^(-1),setting a world record),fast adsorption kinetics(~100% removal within 45 s),and exceptional regeneration capability(>30 cycles)under continuous flow conditions.These outstanding performances benefit from the internal porous channels and surface imidazolium polymer coatings of HOFs,as proved by density functional theory calculation and molecular dynamics simulations.This work paves the way for the rational design of HOF-based hybrid materials tailored to versatile applications.

关 键 词：hydrogen-bonded organic frameworks(HOFs) post-synthetic modification radionuclide sequestration 

分 类 号：TB383.4[一般工业技术—材料科学与工程] O641.3[理学—物理化学]