Efficient removal of^(137)Cs and^(90)Sr from radioactive waste liquids is challenging due to their strong radioactivity,solubility,and mobility.Herein,the efficient Cs^(+)/Sr^(2+)capture has been achieved by layered t...Efficient removal of^(137)Cs and^(90)Sr from radioactive waste liquids is challenging due to their strong radioactivity,solubility,and mobility.Herein,the efficient Cs^(+)/Sr^(2+)capture has been achieved by layered thioniobates and thiotantalate with radiation resistance,namely K_(0.36)NbS_(2)·0.54H_(2)O(K-NbS_(2)),Rb_(0.36)NbS_(2)·0.54H_(2)O(Rb-NbS_(2)),and K_(0.33)TaS_(2)·0.75H_2O(K-TaS_(2)).In particular,K-NbS_(2)exhibits high adsorption capacities,fast kinetics,and fantastic p H durability.K-NbS_(2)is an unprecedented scavenger for selective Sr^(2+)capture in acidic solutions containing excess Na^(+)/Mg^(2+)ions.They show successful cleanup for acidic^(90)Sr-liquid-waste generated during industrial production.Importantly,the removal mechanism is revealed as the ion exchange between Cs^(+)/Sr^(2+)and interlayer K^(+)in thioniobates and thiotantalate due to their appropriate interlayer distances,flexible and adjustable frameworks,and strong affinity of soft basic S^(2-)for Cs^(+)/Sr^(2+).Further,the structure-property relationship study indicates that there is an inverted U-curve rule for the relationship between interlayer distances of layered metal sulfides and ion exchange performance.The rule combined with the factors affecting interlayer distance can be used to direct the structural design and predict properties for the specific recognition and separation of radionuclides.This is a pioneering work on the development of thioniobates/thiotantalate ion exchangers with a deep insight into structure-property relationship for radionuclide remediation.展开更多
The large amount of radioactive waste generated by the rapid development of nuclear energy is in urgent need of disposal.Metal chalcogenide ion-exchangers(MCIEs)are newly developed in recent years that show great pote...The large amount of radioactive waste generated by the rapid development of nuclear energy is in urgent need of disposal.Metal chalcogenide ion-exchangers(MCIEs)are newly developed in recent years that show great potential in the field of removing radionuclides.This is a comprehensive review of the latest research progress on the removal of key radioactive ions(e.g.,radioactive Cs^(+),Sr^(2)+,UO_(2)^(2+),lanthanide ions,and actinide ions)by MCIEs.The structure and ion-exchange properties of MCIEs are summarized emphatically.The ion-exchange mechanism of MCIEs is discussed and the structure-function relationship is preliminarily revealed.Easily exchangeable cations in the interlayer/channel,appropriately sized interlayer/channel/window spaces,flexible open framework,and the strong affinity of the Lewis soft base S^(2−)/Se^(2−)sites in the framework for soft or relatively soft metal ions,are the keys to the excellent selectivity and fast adsorption kinetics of MCIEs for radioactive ions.Finally,future research directions of metal chalcogenides for radioactive ions removal are foreseen.It is hoped that the review will provide a reference for the design of new metal chalcogenide ion-exchangers with practical application prospects for radioactive waste treatment and point to new directions for environmental radioactive contamination control.展开更多
The rapid,efficient,and convenient removal of hazardous radionuclides^(137)Cs and^(90)Sr is an urgent need in the remediation of environmental radioactive contamination.Herein,a biomass composite membrane of K_(2x)Sn_...The rapid,efficient,and convenient removal of hazardous radionuclides^(137)Cs and^(90)Sr is an urgent need in the remediation of environmental radioactive contamination.Herein,a biomass composite membrane of K_(2x)Sn_(4-x)S_(8-x)/collagen fibers(KTS-3/CFs)was obtained by successfully loading the metal sulfide ion exchanger of K_(2x)Sn_(4-x)S_(8-x)(KTS-3)on CFs through the principle of fiber papermaking.The membrane is characterized by a homogeneous shape,operability,good water stability,and easy degradation.It exhibits satisfactory capability for removing Cs^(+)and Sr^(2+)ions,achieving maximum adsorption capacities of 82.34 mg/g for Cs^(+)and 32.98 mg/g for Sr^(2+),respectively.Meanwhile,the KTS-3/CFs membrane has fast kinetic performance and a wide pH activity range for removing Cs^(+)and Sr^(2+)ions.Further,it can still efficiently capture Cs^(+)and Sr^(2+)ions under the coexistence of K^(+),Na^(+),Ca^(2+),and Mg^(2+)ions,and even in actual water samples.The removal of Cs^(+)and Sr^(2+)ions by the KTS-3/CFs is mainly attributed to the ion exchange of Cs^(+)and Sr^(2+)with K^(+)in the interlayer spaces of KTS-3,while the CFs act as the support material for the formation of the membrane.Moreover,the KTS-3/CFs composite membrane is also capable of the fast and efficient capture of Cs^(+)and Sr^(2+)ions in a continuous filtration manner.This work not only develops an environmentally friendly,convenient,and accessible method for the preparation of metal sulfide composites but also paves the way for the development of new high-efficiency composite materials for radionuclides remediation.展开更多
基金supported by the National Natural Science Foundation of China(22325605,U21A20296,22076185,22406185)the Natural Science Foundation of Fujian Province(2024J08105)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB1170000)。
文摘Efficient removal of^(137)Cs and^(90)Sr from radioactive waste liquids is challenging due to their strong radioactivity,solubility,and mobility.Herein,the efficient Cs^(+)/Sr^(2+)capture has been achieved by layered thioniobates and thiotantalate with radiation resistance,namely K_(0.36)NbS_(2)·0.54H_(2)O(K-NbS_(2)),Rb_(0.36)NbS_(2)·0.54H_(2)O(Rb-NbS_(2)),and K_(0.33)TaS_(2)·0.75H_2O(K-TaS_(2)).In particular,K-NbS_(2)exhibits high adsorption capacities,fast kinetics,and fantastic p H durability.K-NbS_(2)is an unprecedented scavenger for selective Sr^(2+)capture in acidic solutions containing excess Na^(+)/Mg^(2+)ions.They show successful cleanup for acidic^(90)Sr-liquid-waste generated during industrial production.Importantly,the removal mechanism is revealed as the ion exchange between Cs^(+)/Sr^(2+)and interlayer K^(+)in thioniobates and thiotantalate due to their appropriate interlayer distances,flexible and adjustable frameworks,and strong affinity of soft basic S^(2-)for Cs^(+)/Sr^(2+).Further,the structure-property relationship study indicates that there is an inverted U-curve rule for the relationship between interlayer distances of layered metal sulfides and ion exchange performance.The rule combined with the factors affecting interlayer distance can be used to direct the structural design and predict properties for the specific recognition and separation of radionuclides.This is a pioneering work on the development of thioniobates/thiotantalate ion exchangers with a deep insight into structure-property relationship for radionuclide remediation.
基金financial supports from the National Natural Science Foundation of China(22325605,U21A20296,22076185 and 21771183)the Natural Science Foundation of Fujian Province(2020J06033).
文摘The large amount of radioactive waste generated by the rapid development of nuclear energy is in urgent need of disposal.Metal chalcogenide ion-exchangers(MCIEs)are newly developed in recent years that show great potential in the field of removing radionuclides.This is a comprehensive review of the latest research progress on the removal of key radioactive ions(e.g.,radioactive Cs^(+),Sr^(2)+,UO_(2)^(2+),lanthanide ions,and actinide ions)by MCIEs.The structure and ion-exchange properties of MCIEs are summarized emphatically.The ion-exchange mechanism of MCIEs is discussed and the structure-function relationship is preliminarily revealed.Easily exchangeable cations in the interlayer/channel,appropriately sized interlayer/channel/window spaces,flexible open framework,and the strong affinity of the Lewis soft base S^(2−)/Se^(2−)sites in the framework for soft or relatively soft metal ions,are the keys to the excellent selectivity and fast adsorption kinetics of MCIEs for radioactive ions.Finally,future research directions of metal chalcogenides for radioactive ions removal are foreseen.It is hoped that the review will provide a reference for the design of new metal chalcogenide ion-exchangers with practical application prospects for radioactive waste treatment and point to new directions for environmental radioactive contamination control.
基金supported by the National Natural Science Foundation of China(Grant Nos.U21A20296,22325605,22076185,22406185)the Natural Science Foundation of Fujian Province(Grant No.2020J06033)。
文摘The rapid,efficient,and convenient removal of hazardous radionuclides^(137)Cs and^(90)Sr is an urgent need in the remediation of environmental radioactive contamination.Herein,a biomass composite membrane of K_(2x)Sn_(4-x)S_(8-x)/collagen fibers(KTS-3/CFs)was obtained by successfully loading the metal sulfide ion exchanger of K_(2x)Sn_(4-x)S_(8-x)(KTS-3)on CFs through the principle of fiber papermaking.The membrane is characterized by a homogeneous shape,operability,good water stability,and easy degradation.It exhibits satisfactory capability for removing Cs^(+)and Sr^(2+)ions,achieving maximum adsorption capacities of 82.34 mg/g for Cs^(+)and 32.98 mg/g for Sr^(2+),respectively.Meanwhile,the KTS-3/CFs membrane has fast kinetic performance and a wide pH activity range for removing Cs^(+)and Sr^(2+)ions.Further,it can still efficiently capture Cs^(+)and Sr^(2+)ions under the coexistence of K^(+),Na^(+),Ca^(2+),and Mg^(2+)ions,and even in actual water samples.The removal of Cs^(+)and Sr^(2+)ions by the KTS-3/CFs is mainly attributed to the ion exchange of Cs^(+)and Sr^(2+)with K^(+)in the interlayer spaces of KTS-3,while the CFs act as the support material for the formation of the membrane.Moreover,the KTS-3/CFs composite membrane is also capable of the fast and efficient capture of Cs^(+)and Sr^(2+)ions in a continuous filtration manner.This work not only develops an environmentally friendly,convenient,and accessible method for the preparation of metal sulfide composites but also paves the way for the development of new high-efficiency composite materials for radionuclides remediation.
