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平衡状态下ALSEP过程的表征：萃取络合物的形态和化学计量

Characterization of the ALSEP Process at Equilibrium: Speciation and Stoichiometry of the Extracted Complex.

作者信息

Picayo Gabriela A, Etz Brian D, Vyas Shubham, Jensen Mark P

机构信息

Chemistry Department, Colorado School of Mines, 1012 14th St, Golden, Colorado 80401, United States.

Nuclear Science and Engineering Program, Colorado School of Mines, 920 15th St, Golden, Colorado 80401, United States.

出版信息

ACS Omega. 2020 Mar 30;5(14):8076-8089. doi: 10.1021/acsomega.0c00209. eCollection 2020 Apr 14.

DOI:10.1021/acsomega.0c00209
PMID:32309717
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7161052/
Abstract

We have determined the identity of the complexes extracted into the ALSEP process solvent from solutions of nitric acid. The ALSEP process is a new solvent extraction separation designed to separate americium and curium from trivalent lanthanides in irradiated nuclear fuel. ALSEP employs a mixture of two extractants, 2-ethylhexyl phosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) and ,,','-tetra(2-ethylhexyl)diglycolamide (TEHDGA) in -dodecane, which makes it difficult to ascertain the nature of the extracted metal complexes. It is often asserted that the weak acid extractant HEH[EHP] does not participate in the extracted complex under ALSEP extraction conditions (2-4 M HNO). However, the analysis of the Am extraction equilibria, Nd absorption spectra, and Eu fluorescence emission spectra of metal-loaded organic phases argues for the participation of HEH[EHP] in the extracted complex despite the high acidity of the aqueous phases. The extracted complex was determined to contain fully protonated molecules of HEH[EHP] with an overall stoichiometry of M(TEHDGA)(HEH[EHP])·3NO. Computations also demonstrate that replacing one TEHDGA molecule with one (HEH[EHP]) dimer is likely energetically favorable compared to Eu(TEHDGA)·3NO, whether the HEH[EHP] dimer is monodentate or bidentate.

摘要

我们已经确定了从硝酸溶液中萃取到ALSEP工艺溶剂中的络合物的特性。ALSEP工艺是一种新的溶剂萃取分离方法，旨在从辐照核燃料中的三价镧系元素中分离出镅和锔。ALSEP使用两种萃取剂的混合物，即2-乙基己基膦酸单2-乙基己酯（HEH[EHP]）和N,N,N',N'-四(2-乙基己基)二甘醇酰胺（TEHDGA）溶解于正十二烷中，这使得确定萃取的金属络合物的性质变得困难。人们通常认为，在ALSEP萃取条件（2-4 M HNO₃）下，弱酸萃取剂HEH[EHP]不参与萃取络合物。然而，对负载金属的有机相的镅萃取平衡、钕吸收光谱和铕荧光发射光谱的分析表明，尽管水相酸度很高，但HEH[EHP]仍参与了萃取络合物。确定萃取的络合物含有完全质子化的HEH[EHP]分子，其总化学计量比为M(TEHDGA)₂(HEH[EHP])·3NO₃。计算还表明，与Eu(TEHDGA)₃·3NO₃相比，用一个（HEH[EHP]）二聚体取代一个TEHDGA分子在能量上可能更有利，无论HEH[EHP]二聚体是单齿还是双齿。

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