乏燃料熔盐电解后处理动力学模型研究

doi:10.19964/j.issn.1006-4990.2022-0281

摘要/Abstract

摘要：

电解精炼是乏燃料干法后处理工艺中的关键环节。针对氯化锂-氯化钾（LiCl-KCl）熔盐环境中的电解精炼行为，基于电极表面处的反应过程建立了动力学模型。通过与现有实验数据的比较验证了模型的有效性。通过该模型，可以预测电解精炼过程中液镉阳极中乏燃料的溶解和阴极处金属沉积的动力学特征，以及所涉及元素的分电流、电极电位和熔盐中离子浓度的演变。除此之外，该模型还能模拟多元素复杂体系电解精炼的过程。当使用锆、铀、钚及稀土作为阳极时，模拟结果显示在阳极处锕系元素和稀土元素随时间逐渐溶解，而惰性金属几乎不溶解。在熔盐中，钚的浓度逐渐增加而铀的浓度逐渐减少，当钚开始在固体阴极发生沉积后，铀的沉积速率减小，而稀土元素和锆在阴极的沉积量极少。

关键词: 乏燃料, 高温冶金, 电解精炼, 模拟

Abstract:

Electrorefining is the key process in used nuclear fuel dry reprocessing.Aiming at the electrorefining behavior of lithium chloride and potassium chloride（LiCl-KCl） molten salt environment，a kinetic model was established based on the reaction process at the electrode surface.The model was validated the experimental data.The model could predict the dissolution of spent fuel in the anode and the dynamic characteristics of metal deposition at the cathode，as well as the evolution of the partial current，electrode potential and ion concentration in molten salt of the elements involved in the electrorefining process.In addition，the model could also simulate the process of electrorefining in multi-element complex system.When the Zr，U，Pu and rare earth metal were used as the anode，simulation results showed that the actinides and rare earth were dissolved gradually on the anode，but the Zr was hardly dissolved.In the molten salt，the concentration of plutonium was increased but the concentration of uranium was decreased.After the deposition of plutonium，the deposition rate of uranium was decreased，with little rare earth or Zr depositing on the cathode.

Key words: used nuclear fuel, pyroprocessing, electrorefining, modeling

中图分类号:

O646.51

衣峰,周文涛,王德忠. 乏燃料熔盐电解后处理动力学模型研究[J]. 无机盐工业, 2022, 54(11): 45-51.

YI Feng,ZHOU Wentao,WANG Dezhong. Study on kinetic model of electrorefining reprocessing of used nuclear fuel molten salt[J]. Inorganic Chemicals Industry, 2022, 54(11): 45-51.

图/表 6

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	UCl₃	PuCl₃
E_ap （V，vs.Cl₂/Cl^-）	-2.453	-2.756
E_ap Cd（V，vs.Cl₂/Cl^-）	-2.551	-2.566
Cd中的活度系数	82.62	1.74×10^-4
K^m /（cm?s^-1）	4.9×10^-3	4.18×10^-3
K^Cd/（cm?s^-1）	5.9×10^-3	5.9×10^-3

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