Efficient,green,and economical removal of radioactive iodine (I_(2)) has drawn worldwide attention for the safe development of nuclear energy. Metal–organic frameworks (MOFs) have been demonstrated to be potential ca...Efficient,green,and economical removal of radioactive iodine (I_(2)) has drawn worldwide attention for the safe development of nuclear energy. Metal–organic frameworks (MOFs) have been demonstrated to be potential candidates for I_(2) capture. Herein we report the synthesis of two novel isomeric MOFs bearing stilbene moieties for exceptionally high I_(2) adsorption. [Cd(hsb-2)(tsbdc)]·0.5DMF (HSB-W8) and Cd(hsb-2)(tsbdc) (HSB-W9),which exhibit two-dimensional and twofold interpenetrated three-dimensional structures,respectively,have been assembled from hydrogenated Schiff base ligands,hsb-2 (1,2-bis(4’-pyridylmethylamino)-ethane) and trans-stilbene-4,4-dicarboxylate (tsbdc),and Cd(NO_(3))_(2) by the diffusion method. Such isomers arise from the different conformations of hsb-2 ligands controlled by diffusion temperatures. The π-electron-rich stilbene moieties render these Cd-MOFs ideal platforms for I_(2) capture. The adsorption capacities of HSB-W8 and HSB-W9 in I_(2) vapor at room temperature can reach up to 2.32 and 1.92 g g^(-1),respectively,which are comparable to the best-performing MOF materials reported so far. Furthermore,pseudo-second-order (PSO) kinetic model analysis,Fourier transform infrared (FT-IR) spectroscopy,Raman spectral analysis,density functional theory (DFT) calculations,and control experiments were performed to shed light on host–vip interactions and the iodine adsorption mechanism. This work develops a rational strategy to design and synthesise functional MOF materials for iodine adsorption.展开更多
基金supported by the National Natural Science Foundation of China(NSFC)(21901246)the Strategic Priority Research Program of CAS(XDB20010200)the Natural Science Foundation of Fujian Province(2019J01126).
文摘Efficient,green,and economical removal of radioactive iodine (I_(2)) has drawn worldwide attention for the safe development of nuclear energy. Metal–organic frameworks (MOFs) have been demonstrated to be potential candidates for I_(2) capture. Herein we report the synthesis of two novel isomeric MOFs bearing stilbene moieties for exceptionally high I_(2) adsorption. [Cd(hsb-2)(tsbdc)]·0.5DMF (HSB-W8) and Cd(hsb-2)(tsbdc) (HSB-W9),which exhibit two-dimensional and twofold interpenetrated three-dimensional structures,respectively,have been assembled from hydrogenated Schiff base ligands,hsb-2 (1,2-bis(4’-pyridylmethylamino)-ethane) and trans-stilbene-4,4-dicarboxylate (tsbdc),and Cd(NO_(3))_(2) by the diffusion method. Such isomers arise from the different conformations of hsb-2 ligands controlled by diffusion temperatures. The π-electron-rich stilbene moieties render these Cd-MOFs ideal platforms for I_(2) capture. The adsorption capacities of HSB-W8 and HSB-W9 in I_(2) vapor at room temperature can reach up to 2.32 and 1.92 g g^(-1),respectively,which are comparable to the best-performing MOF materials reported so far. Furthermore,pseudo-second-order (PSO) kinetic model analysis,Fourier transform infrared (FT-IR) spectroscopy,Raman spectral analysis,density functional theory (DFT) calculations,and control experiments were performed to shed light on host–vip interactions and the iodine adsorption mechanism. This work develops a rational strategy to design and synthesise functional MOF materials for iodine adsorption.
