Simulation of Rare Earth Elements Removal Behavior in TRU Product Using HSC Chemistry Code

S. Paek, C. Lee, D. Yoon, Sung-Jai Lee
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Abstract

The feasibility of rare earth (RE) removal process via oxidation reactions with UCl3 was investigated using the HSC Chemistry code to reduce the concentrations of RE in transuranic (TRU) products. The composition and thermodynamic data of TRU and RE elements contained in the reference spent fuel were examined. The reactivity was evaluated by calculating equilibrium data considering oxidation reactions with UCl3. Both RE removal rate and TRU recovery rate were evaluated for the two cases, wherein TRU products with different RE concentrations were used. When TRU products were reacted with UCl3, selective oxidation was driven by the difference in the Gibbs free energy of each element. The calculation results imply that the TRU/RE ratio of the final product can be increased by removing RE elements while maintaining the maximum recovery rate of TRU, which is accomplished by controlling the amount of UCl3 injected. Since the results of this study are based on thermodynamic equilibrium data, there are many limitations to apply to the actual process. However, it is expected to be used as an important data for the process design to supply the TRU product of pyroprocessing to SFR’s fuel demanding low RE concentrations.
利用HSC化学代码模拟TRU产品中稀土元素的去除行为
利用HSC化学代码研究了UCl3氧化脱除稀土的可行性,以降低超铀(TRU)产品中稀土的浓度。研究了参考乏燃料中TRU和RE元素的组成和热力学数据。通过计算考虑UCl3氧化反应的平衡数据来评价反应性。在使用不同RE浓度的TRU产品时,对两种情况下的RE去除率和TRU回收率进行了评估。当TRU产物与UCl3反应时,各元素的吉布斯自由能差异驱动了选择性氧化。计算结果表明,通过控制UCl3的注入量,在去除RE元素的同时保持TRU的最大回收率,可以提高最终产物的TRU/RE比。由于本研究的结果是基于热力学平衡数据,因此应用于实际过程有许多局限性。然而,它有望作为工艺设计的重要数据,为SFR燃料的低RE浓度要求提供热处理的TRU产品。
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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