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Selective Separation of Americium(III), Curium(III), and Lanthanide(III) by Aqueous and Organic Competitive Extraction.
Wu, Qiang; Hao, Huaixin; Liu, Yang; Sha, Lei-Tao; Wang, Wei-Jia; Shi, Wei-Qun; Wang, Zhipeng; Yan, Ze-Yi.
Afiliación
  • Wu Q; Radiochemistry Laboratory, School of Nuclear Science and Technology, Lanzhou University, Lanzhou 730000, Gansu, China.
  • Hao H; Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China.
  • Liu Y; Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100084, China.
  • Sha LT; Radiochemistry Laboratory, School of Nuclear Science and Technology, Lanzhou University, Lanzhou 730000, Gansu, China.
  • Wang WJ; Radiochemistry Laboratory, School of Nuclear Science and Technology, Lanzhou University, Lanzhou 730000, Gansu, China.
  • Shi WQ; Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100084, China.
  • Wang Z; Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China.
  • Yan ZY; Radiochemistry Laboratory, School of Nuclear Science and Technology, Lanzhou University, Lanzhou 730000, Gansu, China.
Inorg Chem ; 63(1): 462-473, 2024 Jan 08.
Article en En | MEDLINE | ID: mdl-38141022
ABSTRACT
Adding hydrophilic ligands into aqueous solutions for the selective binding of actinides(III) is acknowledged as an advanced strategy in Ln(III)/An(III) separation. In view of the recycling and radioactive waste disposal of the minor actinide, there remains an urgent need to design and develop the appropriate ligand for selective separation of An(III) from Ln(III). Herein, four novel hydrophilic ligands with hard-soft hybrid donors, derived from the pyridine and phenanthroline skeletons, were designed and synthesized as masking agents for selective complexation of An(III) in the aqueous phase. The known N,N,N',N'-tetraoctyl diglycolamide (TODGA) was used as lipophilic extractant in the organic phase for extraction of Ln(III), and a new strategy for the competitive extraction of An(III) and Ln(III) was developed based on TODGA and the above hydrophilic ligands. The optimal hydrophilic ligand of N,N'-bis(2-hydroxyethyl)-2,9-dicarboxamide-1,10-phenanthroline (2OH-DAPhen) displayed exceptional selectivity toward Am(III) over Ln(III), with the concentrations of HNO3 ranging from 0.05 to 3.0 M. The maximum separation factors were up to 1365 for Eu/Am, 417.66 for Eu/Cm, and 42.38 for La/Am. The coordination mode and bonding property of 2OH-DAPhen with Ln(III) were investigated by 1H NMR titration, UV-vis spectrophotometric titration, luminescence titration, FT-IR, ESI-HRMS analysis, and DFT calculations. The results revealed that the predominant species formed in the aqueous phase was a 11 ligand/metal complex. DFT calculations also confirmed that the affinity of 2OH-DAPhen for Am(III) was better than that for Eu(III). The present work using a competitive extraction strategy developed a feasible alternative method for the selective separation of trivalent actinides from lanthanides.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Inorg Chem Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Inorg Chem Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos