The efficient separation of fission products,such as TcO_(4)^(-)and I^(-),holds strategic significance for the management of radioactive wastes and environmental protection.In this study,we propose an ultrafast strate...The efficient separation of fission products,such as TcO_(4)^(-)and I^(-),holds strategic significance for the management of radioactive wastes and environmental protection.In this study,we propose an ultrafast strategy for scalable preparation of a highly quaternized organic network to facilitate efficient and synchronous separation of iodide and pertechnetate.The network can be prepared within a few minutes at room temperature,using polyethylenimine and 1,2,4,5-tetrakis(bromomethyl)benzene as building blocks.After chlorine replacement,the network,abundantly decorated with quaternary ammonium groups(Cl@QPN),exhibits an ultrahigh positive charge density of 7.6 mmol/g.This enables the rapid and efficient enrichment of target anions through strong electrostatic Coulomb interactions.As a result,Cl@QPN exhibits significantly higher adsorption rate constants of 0.830 g/(mg min)for ReO_(4)^(-)(a nonradioactive surrogate of TcO_(4)^(-))and 0.677 g/(mg min)for I-compared to other materials.Furthermore,it possesses high adsorption capacities,reaching 1,681 mg/g for ReO_(4)^(-)and 917.4 mg/g for I-.Cl@QPN also demonstrates good selectivity towards target ions and shows efficient adsorption for^(99)TcO_(4)^(-).Additionally,Cl@QPN exhibits high dynamic processing capacities,handling up to 3,100 and 7,400 kg of simulated streams per kilogram of material for I-and ReO_(4)^(-),respectively.展开更多
基金supported by the National Natural Science Foundation of China(22176138,22276129)a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘The efficient separation of fission products,such as TcO_(4)^(-)and I^(-),holds strategic significance for the management of radioactive wastes and environmental protection.In this study,we propose an ultrafast strategy for scalable preparation of a highly quaternized organic network to facilitate efficient and synchronous separation of iodide and pertechnetate.The network can be prepared within a few minutes at room temperature,using polyethylenimine and 1,2,4,5-tetrakis(bromomethyl)benzene as building blocks.After chlorine replacement,the network,abundantly decorated with quaternary ammonium groups(Cl@QPN),exhibits an ultrahigh positive charge density of 7.6 mmol/g.This enables the rapid and efficient enrichment of target anions through strong electrostatic Coulomb interactions.As a result,Cl@QPN exhibits significantly higher adsorption rate constants of 0.830 g/(mg min)for ReO_(4)^(-)(a nonradioactive surrogate of TcO_(4)^(-))and 0.677 g/(mg min)for I-compared to other materials.Furthermore,it possesses high adsorption capacities,reaching 1,681 mg/g for ReO_(4)^(-)and 917.4 mg/g for I-.Cl@QPN also demonstrates good selectivity towards target ions and shows efficient adsorption for^(99)TcO_(4)^(-).Additionally,Cl@QPN exhibits high dynamic processing capacities,handling up to 3,100 and 7,400 kg of simulated streams per kilogram of material for I-and ReO_(4)^(-),respectively.
