Efficient Trivalent Actinide-Lanthanide Separations Using Hydrophilic CHON-Compliant Phenanthroline-Dicarboxamide Ligands

IF 3.9 3区工程技术 Q2 ENGINEERING, CHEMICAL

Industrial & Engineering Chemistry Research Pub Date : 2025-06-05 DOI:10.1021/acs.iecr.5c0079510.1021/acs.iecr.5c00795

Yong Qiang Wan, Huai Xin Hao, Yang Yang Zhang, Yu Xiao Guo, Zhi Jun Ma, Zhi Peng Wang*, Jun Li* and Pavle Mocilac*,

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Abstract

Experimental studies are reported herein on novel hydrophilic CHON-compliant ligands based on 1,10-phenanthroline-dicarboxamide derivatives bearing ethylene glycol (AE-DAPhen) and diethylene glycol (AEE-DAPhen) hydrophilizing terminal groups. These ligands exhibit high solubility in nitric acid solutions and demonstrate strong selectivity for Am(III) over Eu(III) in mildly acidic conditions against the TODGA (N,N,N′,N′-tetraoctyl diglycolamide) ligand in organic phase using two different extraction methods. The maximum separation factors (SF_Eu/Am) achieved were 325 for AE-DAPhen and 291 for AEE-DAPhen. In addition, solvent extraction tests with Cm(III) were also conducted, and SF_Eu/Cm turned out to be surprisingly lower: 50 for AE-DAPhen and 55 for AEE-DAPhen. Overall, these observations amount to a relative SF_Cm/Am of 7.4–7.8, which is one of the best reported values for any CHON-compliant ligands. The theoretical results from quantum-chemical studies suggest a coordinative role of hydroxyl and etheric oxygen atoms, providing an understanding of the bonding interaction between the metal ions and ligands.

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用亲水顺性苯酚-二羧酰胺配体高效分离三价锕系元素-镧系元素

本文报道了基于1,10-邻菲罗啉-二甲酰胺衍生物的新型亲水顺性配体的实验研究，这些衍生物具有乙二醇（ae - dapen）和二乙二醇（ae - dapen）亲水性末端基团。这些配体在硝酸溶液中具有较高的溶解度，并且在温和酸性条件下对有机相中的TODGA （N，N,N ',N ' -四辛基二甘醇酰胺）配体表现出较强的选择性。ae - dapen获得的最大分离因子（SFEu/Am）为325，ae - dapen为291。此外，还进行了Cm（III）的溶剂萃取试验，结果表明，ae - dapen的SFEu/Cm惊人地低：ae - dapen为50，ae - dapen为55。总的来说，这些观察结果的相对SFCm/Am为7.4-7.8，这是任何符合chon的配体的最佳报告值之一。量子化学研究的理论结果表明，羟基和醚氧原子的协调作用，提供了金属离子和配体之间的键相互作用的理解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Industrial & Engineering Chemistry Research 工程技术-工程：化工

CiteScore

7.40

自引率

7.10%

发文量

1467

审稿时长

2.8 months

期刊介绍： ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.