In the current era marked by energy shortages,the advancement of nuclear energy stands as an inevitable progression.The reprocessing of spent nuclear fuel plays a crucial role in determining the sustainability of nucl...In the current era marked by energy shortages,the advancement of nuclear energy stands as an inevitable progression.The reprocessing of spent nuclear fuel plays a crucial role in determining the sustainability of nuclear energy as a viable energy source.Among these processes,the separation and recovery of Pu(Ⅳ)from high-level liquid waste(HLLW)hold paramount significance in terms of safety and strategic implications.Herein,this work focused on the synthesis of two acid-and radiation-resistant pyridine-based sp^(2)c-COFs(COF-IHEP3 and COF-IHEP4),followed by the creation of two pyridine-based ionized sp^(2)c-COFs named COF-IHEP3-CH_(3)NO_(3)and COF-IHEP4-CH3NO3through post-modification.These materials have potential anion exchange capacity for the selective separation of Pu(Ⅳ)in highly acidic conditions.Notably,in 8 mol/L nitric acid solution,COF-IHEP3-CH3NO3demonstrated the capability to eliminate plutonium within 20 min in 98%removal efficiency with a Kdvalue of 2450 m L/g.Experimental and theoretical analysis suggest that the ionized sp^(2)c-COFs exhibit exceptional stability,selectivity,and prevention of secondary contamination towards Pu(Ⅳ)in the presence of multiple ions environments.In short,this work provides an appropriate anion exchange strategy to design ionic sp^(2)c-COFs as a promising platform for Pu(Ⅳ)recovery from HLLW.展开更多
基金supported by the National Natural Science Foundation of China(Nos.U2067212,22176191)the National Science Fund for Distinguished Young Scholars(No.21925603)。
文摘In the current era marked by energy shortages,the advancement of nuclear energy stands as an inevitable progression.The reprocessing of spent nuclear fuel plays a crucial role in determining the sustainability of nuclear energy as a viable energy source.Among these processes,the separation and recovery of Pu(Ⅳ)from high-level liquid waste(HLLW)hold paramount significance in terms of safety and strategic implications.Herein,this work focused on the synthesis of two acid-and radiation-resistant pyridine-based sp^(2)c-COFs(COF-IHEP3 and COF-IHEP4),followed by the creation of two pyridine-based ionized sp^(2)c-COFs named COF-IHEP3-CH_(3)NO_(3)and COF-IHEP4-CH3NO3through post-modification.These materials have potential anion exchange capacity for the selective separation of Pu(Ⅳ)in highly acidic conditions.Notably,in 8 mol/L nitric acid solution,COF-IHEP3-CH3NO3demonstrated the capability to eliminate plutonium within 20 min in 98%removal efficiency with a Kdvalue of 2450 m L/g.Experimental and theoretical analysis suggest that the ionized sp^(2)c-COFs exhibit exceptional stability,selectivity,and prevention of secondary contamination towards Pu(Ⅳ)in the presence of multiple ions environments.In short,this work provides an appropriate anion exchange strategy to design ionic sp^(2)c-COFs as a promising platform for Pu(Ⅳ)recovery from HLLW.
