Extraction of Nd(III), Eu(III), Am(III) and Cm(III) With 6-Carboxylic Di(2-Ethylhexyl) Amide Pyridine

IF 0.4 Q4 NUCLEAR SCIENCE & TECHNOLOGY Journal of Nuclear Fuel Cycle and Waste Technology Pub Date : 2022-08-08 DOI:10.1115/icone29-90818
Chao Xu, Yu Du, Tingting Liu, Suliang Yang
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Abstract

Solvent extraction has been widely used in spent fuel reprocessing because of its advantages such as high mass transfer rate, short production cycle, easy operation and large extraction capacity. The ligands containing soft S and N atoms usually have a good effect on the separation of trivalent lanthanides actinides. Herein, a novel extractant, 6-carboxylic di(2-ethylhexyl) amide pyridine (DEHAPA, HA), containing carboxyl and amide pyridine, was designed. The extraction of Nd(III), Eu(III), Am(III) and Cm(III), representing trivalent lanthanides and actinides, from nitric solution has been carried out by DEHAPA diluted in toluene as the organic phase. According to the slope analysis, the results show that the extraction of Ln(III) and An(III) with DEHAPA was governed by ion-exchange mechanism and the extraction equilibrium constants of Nd(III), Eu(III), Am(III) and Cm(III) have been calculated. The effect of concentration indicated that the structure of extraction complexes are 1:3/LnA3 and 1:3/AnA3. The temperature has a slight influence to distribution ratio of extraction Nd(III) and Eu(III). The infrared spectrum of DEHAPA and extracted complex analysis showed that -N-C = O and -O-C = O group coordinated with Nd(III). According to 1:3/LnA3 extracted complex structure, the Nd(III) ion in complex was coordinated with three -N-C = O, -O-C = O and pyridine group from three tridentate A− ligands by three tridentate A− ligand in organic solvent. This work reveals the unique extraction and coordination structure and provides a value reference to design more effective extraction ligands for Ln(III)/An(III) separation.
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6-羧基二(2-乙基己基)酰胺吡啶萃取Nd(III)、Eu(III)、Am(III)和Cm(III
溶剂萃取具有传质速率高、生产周期短、操作简单、萃取量大等优点,在乏燃料后处理中得到了广泛的应用。含有软S和软N原子的配体通常对三价系镧系锕系的分离有很好的效果。本文设计了一种含有羧基和酰胺吡啶的新型萃取剂- 6-羧基二(2-乙基己基)酰胺吡啶(DEHAPA, HA)。用DEHAPA在甲苯中稀释作为有机相,从硝酸溶液中萃取三价镧系元素Nd(III)、Eu(III)、Am(III)和Cm(III)。由斜率分析可知,DEHAPA萃取Ln(III)和An(III)受离子交换机制支配,并计算出Nd(III)、Eu(III)、Am(III)和Cm(III)的萃取平衡常数。浓度的影响表明萃取配合物的结构为1:3/LnA3和1:3/AnA3。温度对萃取Nd(III)和Eu(III)的分布比例影响较小。DEHAPA红外光谱和萃取配合物分析表明-N-C = O和-O-C = O基团与Nd(III)配位。根据1:3/LnA3萃取的配合物结构,配合物中的Nd(III)离子在有机溶剂中与三个三齿A -配体中的三个-N-C = O、-O-C = O和吡啶基团配位。本研究揭示了独特的萃取配位结构,为设计更有效的萃取配体用于Ln(III)/An(III)分离提供了有价值的参考。
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来源期刊
CiteScore
0.80
自引率
25.00%
发文量
35
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