Spent nuclear fuel (SNF) released from reactors possesses significant radioactivity, heat release properties, and high-value radioactive nuclides. Therefore, using chemical methods for reprocessing can enhance economic efficiency and reduce the potential environmental risks of nuclear energy. Due to the presence of relatively diffuse f-electrons, the chemical properties of trivalent lanthanides (Ln(III)) and actinides (An(III)) in SNF solutions are quite similar. Separation methods have several limitations, including poor separation efficiency and the need for multiple stripping agents. The use of novel multi-dental phenanthroline-derived extractants with nitrogen donor atoms to effectively separate An(III) over Ln(III) has been widely accepted. This review first introduces the development history of phenanthroline-derived extractants for extraction and complexation with An(III) over Ln(III). Then, based on structural differences, these extractants are classified into four categories: nitrogen-coordinated, ,-hybrid coordinated, highly preorganized structure, and unsymmetric structure. Each category's design principles, extraction, and separation performance as well as their advantages and disadvantages are discussed. Finally, we have summarized and compared the unique characteristics of the existing extractants and provided an outlook. This work may offer a reliable reference for the precise identification and selective separation between An(III) and Ln(III), and point the way for future development and exploration.
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http://dx.doi.org/10.1039/d4cc03810j | DOI Listing |
JACS Au
December 2024
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310058, China.
The chemical similarities between trivalent actinides [An(III)] and lanthanides [Ln(III)] present a significant challenge in differentiating and separating them, which is a key step toward closing the nuclear fuel cycle. However, the existing separation approaches commonly suffer from demerits such as inadequate separation factors, limited stripping efficiency, and undesired coextraction. In this study, a novel unsymmetrical phenanthroline-derived amide-triazine (Et-Tol-CyMe-ATPhen) extractant was first designed and then screened with theoretical computation.
View Article and Find Full Text PDFChem Commun (Camb)
October 2024
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310058, China.
Spent nuclear fuel (SNF) released from reactors possesses significant radioactivity, heat release properties, and high-value radioactive nuclides. Therefore, using chemical methods for reprocessing can enhance economic efficiency and reduce the potential environmental risks of nuclear energy. Due to the presence of relatively diffuse f-electrons, the chemical properties of trivalent lanthanides (Ln(III)) and actinides (An(III)) in SNF solutions are quite similar.
View Article and Find Full Text PDFInorg Chem
May 2024
Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China.
Excellent "CHON" compatible ligands based on a heterocyclic skeleton for the separation of trivalent actinides [An(III)] from lanthanides [Ln(III)] have been widely explored, the aim being spent nuclear fuel reprocessing. The combination mode of a soft/hard (N/O) donor upon the coordination chemistry of An(III) and Ln(III) should play a vital role with respect to the performance of ligands. As such, in this work, two typical experimentally available phenanthroline-derived tetradentate ligands, CyMe-BTPhen () and Et-Tol-DAPhen (), and two theoretically designed asymmetric tetradentate heterocyclic ligands, and , with various N/O donors were investigated using scalar relativistic density functional theory.
View Article and Find Full Text PDFChemistry
June 2023
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310058, China.
The separation of actinides from lanthanides in spent nuclear fuel reprocessing is a vital step of nuclear fuel cycle process. As one class of mature industrial extractants, the organophosphorus extractants have been widely used for the extraction and separation of actinides and lanthanides in spent fuel reprocessing due to their strong extraction ability and low-cost acquisition. In this concept, the application scope of tributyl phosphate (TBP), bis(2-ethylhexyl) phosphate (HDEHP), octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO), trialkyl phosphine oxide (TRPO), and purified Cyanex 301 (bis(2,4,4-trimethylpentyl) dithiophosphinic acid, HA301) are introduced, and their extraction mechanism, as well as structure-function relationships for separation of actinides over lanthanides are also discussed.
View Article and Find Full Text PDFMolecules
March 2022
Department of Radiochemistry, China Institute of Atomic Energy, P.O. Box 275, Beijing 102413, China.
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