Статья

Excellent Selectivity for Actinides with a Tetradentate 2,9-Diamide-1,10-Phenanthroline Ligand in Highly Acidic Solution: A Hard–Soft Donor Combined Strategy

Chengliang XiaoKey Laboratory of Nuclear Radiation and Nuclear Energy Technology and Key Laboratory For Biomedical Effects of Nanomaterials and Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P.R. ChinaCong‐Zhi WangKey Laboratory of Nuclear Radiation and Nuclear Energy Technology and Key Laboratory For Biomedical Effects of Nanomaterials and Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P.R. ChinaLi‐Yong YuanKey Laboratory of Nuclear Radiation and Nuclear Energy Technology and Key Laboratory For Biomedical Effects of Nanomaterials and Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P.R. ChinaBin LiDivision of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, P.R. ChinaHui HeDivision of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, P.R. ChinaShuao WangSchool of Radiological and Interdisciplinary Sciences, Soochow University, Suzhou 215123, P.R. ChinaYu-Liang ZhaoKey Laboratory of Nuclear Radiation and Nuclear Energy Technology and Key Laboratory For Biomedical Effects of Nanomaterials and Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P.R. ChinaZhifang ChaiKey Laboratory of Nuclear Radiation and Nuclear Energy Technology and Key Laboratory For Biomedical Effects of Nanomaterials and Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P.R. ChinaWei‐Qun ShiKey Laboratory of Nuclear Radiation and Nuclear Energy Technology and Key Laboratory For Biomedical Effects of Nanomaterials and Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P.R. China

2014en

ABI

Аннотация

In this work, we reported a phenanthroline-based tetradentate ligand with hard-soft donors combined in the same molecule, N,N'-diethyl-N,N'-ditolyl-2,9-diamide-1,10-phenanthroline (Et-Tol-DAPhen), for the group separation of actinides over lanthanides. The synthesis and solvent extraction as well as complexation behaviors of the ligand with actinides and lanthanides are studied experimentally and theoretically. The ligand exhibits excellent extraction ability and high selectivity toward hexavalent, tetravalent, and trivalent actinides over lanthanides in highly acidic solution. The chemical stoichiometry of Th(IV) and U(VI) complexes with Et-Tol-DAPhen is determined to be 1:1 using X-ray crystallography. The stability constants of some typical actinide and lanthanide complexes of Et-Tol-DAPhen are also determined in methanol by UV-vis spectrometry. Density functional theory (DFT) calculations reveal that the An-N bonds of the Et-Tol-DAPhen complexes have more covalent characters than the corresponding Eu-N bonds, which may in turn lead to the selectivity of Et-Tol-DAPhen toward actinides. This ligand possesses merits of both alkylamide and 2,9-bis-(5,6-dialkyl-1,2,4-triazin-3-yl)-1,10-phenanthroline (R-BTPhen) extractants for efficient actinide extraction and the selectivity toward minor actinides over lanthanides and hence renders huge potential opportunities in high-level liquid waste (HLLW) partitioning.

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Идентификаторы

DOI: 10.1021/ic402784c

Цитирования и источники

Цитирований: 2Использованных источников: 0

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