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Improving Americium/Curium Separation Factors in the AmSel Process through Symmetry Lowering of the Diglycolamide Extractant

机译:通过对称降低二甘酰胺萃取剂来提高 AmSel 工艺中的镅/锔分离因子

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摘要

Partitioning and transmutation are important strategies for closing the nuclear fuel cycle. The diglycolamide extractant TODGA has played a major role in the development of solvent extraction processes for nuclear fuel reprocessing due to its good extraction performance, its hydrolytic and radiolytic stability, and its compliance with the CHON principle. However, due to drawbacks such as the tendency to form a third phase during extraction if no phase modifiers are used, continued research on diglycolamide-type extractants has led to the development of diglycolamides with decreased symmetry. In this study, it is shown that the recently developed diglycolamide, N,N-diisopropyl-N′,N′-didodecyldiglycolamide (iPDdDGA), is a potential alternative to TODGA with improved separation between Am and Cm or the Ln. Using the AmSel system as a reference, the extraction kinetics, influence of the acid concentration, influence of the iPDdDGA concentration, and influence of temperature were evaluated. Slope analysis indicates similar average stoichiometries for iPDdDGA and TODGA complexes, but the extraction efficiency of iPDdDGA is orders of magnitude higher. The feasibility of selective americium stripping in combination with the hydrophilic sulfonated bis-triazinyl bipyridine SO3-Ph-BTBP complexant was demonstrated. Selective stripping of americium was found to be possible, and the use of iPDdDGA gave an unexpected improvement in Am/Cm separation, with SFCm/Am values of up to 3.0. This represents a small but significant improvement compared to the 2.5 value typically found for TODGA, and it demonstrates the potential of this solvent extraction system to improve existing processes based on diglycolamide-type extractants.
机译:分区和嬗变是关闭核燃料循环的重要策略。二甘酰胺萃取剂 TODGA 由于其良好的提取性能、水解和辐射稳定性以及符合 CHON 原理,在核燃料后处理溶剂萃取工艺的开发中发挥了重要作用。然而,由于不使用相改性剂在提取过程中容易形成第三相等缺点,对二甘酰胺型萃取剂的持续研究导致了对称性降低的二甘酰胺的发展。在这项研究中,表明最近开发的二甘酰胺,N,N-二异丙基-N',N'-二十二烷基二甘酰胺 (iPDdDGA) 是 TODGA 的潜在替代品,具有更好的 Am 和 Cm 或 Ln 之间的分离。以 AmSel 系统为参考,评估了萃取动力学、酸浓度的影响、iPDdDGA 浓度的影响和温度的影响。斜率分析表明 iPDdDGA 和 TODGA 复合物的平均化学计量相似,但 iPDdDGA 的提取效率要高出几个数量级。证明了选择性镅剥离与亲水性磺化双三嗪基联吡啶 SO3-Ph-BTBP 络合剂联合使用的可行性。发现镅的选择性剥离是可能的,并且使用 iPDdDGA 在 Am/Cm 分离方面取得了意想不到的改善,SFCm/Am 值高达 3.0。与 TODGA 通常的 2.5 值相比,这是一个微小但显著的改进,它证明了这种溶剂萃取系统在改进基于二甘酰胺类萃取剂的现有工艺方面的潜力。

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