Group hexavalent actinide separation from lanthanides using sodium bismuthate chromatography

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A Pub Date : 2024-09-25 DOI:10.1016/j.chroma.2024.465400

Samantha A. Labb , Kelly N. Kmak , John D. Despotopulos , William M. Kerlin , Ralf Sudowe

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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 (NaBiO₃), has been demonstrated to quantitatively oxidize and separate Am from trivalent Cm in a column chromatographic system. This work expands on the use of NaBiO₃ 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 NaBiO₃-based separation following a TRUEX process.

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利用铋酸钠色谱法从镧系元素中分离六价锕系元素

先进的废旧核燃料（UNF）后处理策略受到复杂的放射化学分离和工程技术的限制，无法实现锕系元素（An）与中子清除镧系元素（Ln）的分离。锕系元素（U-Am）的六价氧化态为实现六价锕系元素与三价镧系元素和铯的分离提供了一条途径。固体氧化剂和离子交换剂铋酸钠（NaBiO3）已被证明可以在柱层析系统中定量氧化和分离 Am 与三价 Cm。这项研究拓展了 NaBiO3 色谱法的使用范围，对铀、钚和欧的吸附、动力学和洗脱行为进行了表征。在稀硝酸浓度下，观察到分离因子超过 200，且具有快速动力学特性，在不到一小时的时间内就实现了 An/Ln 的完全分离。对各种后处理废料中存在的关键裂变产物的吸附和色谱行为进行了表征，证明了在 TRUEX 工艺之后应用基于 NaBiO3 的分离技术的潜力。

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来源期刊

Journal of Chromatography A 化学-分析化学

CiteScore

7.90

自引率

14.60%

发文量

742

审稿时长

45 days

期刊介绍： The Journal of Chromatography A provides a forum for the publication of original research and critical reviews on all aspects of fundamental and applied separation science. The scope of the journal includes chromatography and related techniques, electromigration techniques (e.g. electrophoresis, electrochromatography), hyphenated and other multi-dimensional techniques, sample preparation, and detection methods such as mass spectrometry. Contributions consist mainly of research papers dealing with the theory of separation methods, instrumental developments and analytical and preparative applications of general interest.