氧化物乏燃料电沉积中氯氧比对铀、钚存在形态影响研究
收稿日期: 2024-04-23
网络出版日期: 2024-07-17
基金资助
上海市自然科学基金项目(21ZR1435400)
Effect of chlorine⁃oxygen pressure ratio on chemical speciation of uranium and plutonium during oxide spent fuel electrodeposition
Received date: 2024-04-23
Online published: 2024-07-17
随着中国快堆技术的快速发展，与之匹配的干法后处理技术日益受到关注。其中，氧化物电沉积流程（DDP）因其能够实现铀、钚的共沉积并直接制备混合氧化物（MOX）燃料，成为当前研究最为广泛的干法后处理技术之一。在DDP流程的电解分离过程中，需要精确地控制氯氧分压比，以确保铀元素以铀酰离子状态存在，钚元素以钚离子状态存在，从而实现铀、钚的高效共沉积。为探究铀、钚离子存在形态对氯氧分压比的依赖关系，基于铀钚氯氧二重优势区图，研究了铀酰离子与钚离子共存状态下，最小氯氧分压与温度之间的关系，以及两种气体分压之间的相互影响规律。研究结果表明：随着温度升高，氯气的最小分压增长较为缓慢，而氧气分压则随温度升高呈快速增加趋势；随着氧气浓度的增加，氯气的最小分压起初保持稳定，但当氧气浓度达到一定阈值后，氯气分压开始缓慢上升；此外，随着氯气分压的增加，氧气分压立即呈现上升趋势。该研究结果对氧化物电解沉积过程中氯、氧分压的精确控制具有重要的指导意义。
李泓儒 , 丁允聪 , 周文涛 , 王德忠 . 氧化物乏燃料电沉积中氯氧比对铀、钚存在形态影响研究[J]. 无机盐工业, 2025 , 57(5) : 64 -70 . DOI: 10.19964/j.issn.1006-4990.2024-0226
With the development of fast reactor technology in China，the dry reprocessing technology has attracted more and more attention.The dimitrovgrad dry process（DDP） has become one of the most studied dry post⁃processing technologies because it can co⁃deposit uranium and plutonium to directly produce MOX fuel.In the electrolytic separation process of the DDP process，the partial pressure ratio of chlorine to oxygen needs to be precisely controlled to ensure the presence of uranium in the state of uranyl ions and the existence of plutonium in the state of plutonium ions，to achieve efficient co⁃deposition of uranium and plutonium.To grasp the dependence of uranium and plutonium ions on the partial pressure ratio of chloride and oxychloride，the relationship between the minimum partial pressure of oxychloride and temperature and the interaction between the partial pressures of the two gases were studied through the diagram of the double dominant region of uranium⁃plutonium and plutonium ions.It was found that the minimum partial pressure of chlorine was increased slowly with the increase of temperature，while the partial pressure of oxygen was increased rapidly with the increase of temperature.As the oxygen concentration increased，the minimum concentration of chlorine remained unchanged at first，and the partial pressure of chlorine began to increase slowly after the oxygen concentration reached a certain level，and the oxygen pressure began to increase immediately as the chlorine pressure increased.The results of this study had guiding significance for the partial pressure control of chlorine and oxygen in the process of oxide electrolytic deposition.
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