Enhancing the Selectivity of Trivalent Actinide over Lanthanide Using Asymmetrical Phenanthroline Diamide Ligands

化学 镧系元素 菲咯啉 滴定法 选择性 化学计量学 配合物的稳定常数 无机化学 锕系元素 萃取(化学) 结晶学 物理化学 有机化学 水溶液 催化作用 离子
作者
Sheng Wang,Xiaofan Yang,Yaoyang Liu,Lei Xu,Chao Xu,Chengliang Xiao
出处
期刊:Inorganic Chemistry [American Chemical Society]
卷期号:63 (6): 3063-3074 被引量:7
标识
DOI:10.1021/acs.inorgchem.3c03997
摘要

Phenanthroline diamide ligands have been widely used in the separation of trivalent actinides and lanthanides, but little research has focused on extractants with asymmetrical substitutes. Two novel asymmetrical phenanthroline-based ligands N2,N2,N9-triethyl-N9-tolyl-1,10-phenanthroline-2,9-dicarboxamide (DE-ET-DAPhen) and N2-ethyl-N9,N9-dioctyl-N2-tolyl-1,10-phenanthroline-2,9-dicarboxamide (DO-ET-DAPhen) were first synthesized in this work, whose extraction ability and complexation mechanism to trivalent actinides [An(III)] and lanthanides [Ln(III)] were systematically investigated. The ligands dissolved in n-octanol exhibit good extraction ability and high selectivity toward Am(III) in acidic solutions. The complexation mechanism of the ligands with Ln(III) in solution and solid state was analyzed using slope analysis, 1H NMR spectrometric titration, ESI-MS, and calorimetric titration. It is revealed that the ligands complex with Am(III)/Eu(III) with 1:1 stoichiometry. The stability constant (log β) of the complexation reaction of Eu(III) with DE-ET-DAPhen determined by UV–vis spectrophotometric and calorimetric titration is higher than that of DO-ET-DAPhen, indicating the stronger complexation ability of DE-ET-DAPhen. Meanwhile, the calorimetric titration results show that the complexation process is exothermic with a decreased entropy. The structures of 1:1 complexes of Eu(III) and Nd(III) with DE-ET-DAPhen were analyzed through single-crystal X-ray diffraction. This work proves that ligands containing asymmetrical functional groups are promising for An(III)/Ln(III) separation, which shows great significance in efficient extractants designed for the spent nuclear fuel reprocessing process.
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