Conventional electrolytic methods for separating chemically similar lanthanides(Ln)and actinides(An)are limited by thermodynamics and slow reaction kinetics,restricting their efficiency in rare-earth refining and nucl...Conventional electrolytic methods for separating chemically similar lanthanides(Ln)and actinides(An)are limited by thermodynamics and slow reaction kinetics,restricting their efficiency in rare-earth refining and nuclear fuel recycling.Herein,we report an electroextraction and oxidative back-extraction(EOB)strategy utilizing a LiCl-KCl-KAlCl_(4) molten salt that overcomes these limitations by leveraging divergent interfacial reactivity.The EOB process achieves an exceptional separation factor for Ln/An(>1000),while simultaneously increasing the separation rate by at least one order of magnitude.Through in-situ synchrotron radiation X-ray micro-computed tomography(SR-μCT)and X-ray diffraction(SR-XRD),we capture selective oxidation-induced destabilization of Ln-Al alloys while actinides retain phase stability-directly visualizing the electrochemical alloy transition mechanism.This research redefines the separation of f-block elements in molten salt systems and introduces a multimodal approach to investigating transient interfacial phenomena that are usually inaccessible to conventional metallurgical diagnostics under extreme conditions.展开更多
Hydrophilic chelators are crucial for coordinating and separating radioactive f-block elements in nuclear fuel recycling,hazardous waste treatment,environmental remediation,radiopharmaceuticals,and related fields.Howe...Hydrophilic chelators are crucial for coordinating and separating radioactive f-block elements in nuclear fuel recycling,hazardous waste treatment,environmental remediation,radiopharmaceuticals,and related fields.However,their development and understanding lag behind their lipophilic counterparts.This review summarizes the development of hy-drophilic ligands across four categories based on their structural similarities and chronological order.For each category,representative examples are discussed,highlighting their advantages and disadvantages.The review also benchmarks ligands from different groups,outlines current design challenges,and emphasizes the importance of establishing structure-function relationships to guide future ligand design.Additionally,we propose four novel f-block chelating ligands,some of which have shown efficiency in solid-liquid or membrane-based radionuclide separation,aiming to inspire the search for more robust systems for f-block element utilization and recycling.This review aims to provide a comprehensive overview of hydrophilic f-block element chelators and suggest promising approaches for future ligand development.展开更多
基金supported by the National Science Fund for Distinguished Young Scholars(21925603)the National Natural Science Foundation of China(22306185)the China Postdoctoral Science Foundation(2023M732032)。
文摘Conventional electrolytic methods for separating chemically similar lanthanides(Ln)and actinides(An)are limited by thermodynamics and slow reaction kinetics,restricting their efficiency in rare-earth refining and nuclear fuel recycling.Herein,we report an electroextraction and oxidative back-extraction(EOB)strategy utilizing a LiCl-KCl-KAlCl_(4) molten salt that overcomes these limitations by leveraging divergent interfacial reactivity.The EOB process achieves an exceptional separation factor for Ln/An(>1000),while simultaneously increasing the separation rate by at least one order of magnitude.Through in-situ synchrotron radiation X-ray micro-computed tomography(SR-μCT)and X-ray diffraction(SR-XRD),we capture selective oxidation-induced destabilization of Ln-Al alloys while actinides retain phase stability-directly visualizing the electrochemical alloy transition mechanism.This research redefines the separation of f-block elements in molten salt systems and introduces a multimodal approach to investigating transient interfacial phenomena that are usually inaccessible to conventional metallurgical diagnostics under extreme conditions.
基金the National Natural Science Foundation of China (U2067213, 22325603)the National Natural Science Foundation of China (22105205)the Beijing Natural Science Foundation (2232002)
文摘Hydrophilic chelators are crucial for coordinating and separating radioactive f-block elements in nuclear fuel recycling,hazardous waste treatment,environmental remediation,radiopharmaceuticals,and related fields.However,their development and understanding lag behind their lipophilic counterparts.This review summarizes the development of hy-drophilic ligands across four categories based on their structural similarities and chronological order.For each category,representative examples are discussed,highlighting their advantages and disadvantages.The review also benchmarks ligands from different groups,outlines current design challenges,and emphasizes the importance of establishing structure-function relationships to guide future ligand design.Additionally,we propose four novel f-block chelating ligands,some of which have shown efficiency in solid-liquid or membrane-based radionuclide separation,aiming to inspire the search for more robust systems for f-block element utilization and recycling.This review aims to provide a comprehensive overview of hydrophilic f-block element chelators and suggest promising approaches for future ligand development.
