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用偏铋酸钠色谱法从镧系元素中分离六价锕系元素。

Group hexavalent actinide separation from lanthanides using sodium bismuthate chromatography.

机构信息

Department of Environmental and Radiological Health Sciences, Colorado State University, 1618 Campus Delivery, Fort Collins, CO, 94550 USA; Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, 7000 East Ave., Livermore, CA, 94550, USA.

Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, 7000 East Ave., Livermore, CA, 94550, USA.

出版信息

J Chromatogr A. 2024 Nov 8;1736:465400. doi: 10.1016/j.chroma.2024.465400. Epub 2024 Sep 25.

Abstract

Advanced used nuclear fuel (UNF) reprocessing strategies are limited by the complex radiochemical separations and engineering required to achieve the separation of actinides (An) from neutron scavenging lanthanides (Ln). The accessibility of the hexavalent oxidation state for the actinides (U - Am) provides a pathway to achieving a group hexavalent actinide separation from the trivalent lanthanides and Cm. The solid oxidant and ion exchanger, sodium bismuthate (NaBiO), has been demonstrated to quantitatively oxidize and separate Am from trivalent Cm in a column chromatographic system. This work expands on the use of NaBiO chromatography to characterize the adsorption, kinetic, and elution behavior of U, Pu, and Eu. Separation factors over 200 with rapid kinetics were observed at dilute nitric acid concentrations with a complete An/Ln separation achieved in under an hour. The adsorption and chromatographic behavior of key fission products present in various reprocessing raffinates was characterized which demonstrated potential application of a NaBiO-based separation following a TRUEX process.

摘要

先进的乏核燃料(UNF)后处理策略受到复杂的放射化学分离和工程的限制,这些分离和工程是实现锕系元素(An)与中子清除镧系元素(Ln)分离所必需的。锕系元素(U-Am)的六价氧化态的可及性为实现六价锕系元素与三价镧系元素和 Cm 的组分离提供了途径。固体氧化剂和离子交换剂,五氧化二铋(NaBiO),已被证明可在柱色谱系统中定量氧化和分离 Am 与三价 Cm。这项工作扩展了 NaBiO 色谱法的使用,以表征 U、Pu 和 Eu 的吸附、动力学和洗脱行为。在稀硝酸浓度下观察到超过 200 的分离因子和快速动力学,在不到一个小时的时间内完成了 An/Ln 的完全分离。还对各种后处理萃余液中存在的关键裂变产物的吸附和色谱行为进行了表征,这表明在 TRUEX 工艺之后,基于 NaBiO 的分离具有潜在的应用前景。

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