无机盐工业
主管:中海油天津化工研究设计院有限公司
主办:中海油天津化工研究设计院有限公司
   中海油炼油化工科学研究院(北京)有限公司
   中国化工学会无机酸碱盐专业委员会
ISSN 1006-4990 CN 12-1069/TQ

无机盐工业 ›› 2024, Vol. 56 ›› Issue (4): 64-71.doi: 10.19964/j.issn.1006-4990.2023-0267

• 研究与开发 • 上一篇    下一篇

基于相场方法的铀枝晶生长电化学-流场耦合研究

赵干(), 许晓锐, 周文涛(), 王亚飞, 王德忠   

  1. 上海交通大学,上海 200240
  • 收稿日期:2023-05-12 出版日期:2024-04-10 发布日期:2024-04-18
  • 通讯作者: 周文涛(1990— ),男,博士,副教授,研究方向为乏燃料熔盐电解后处理等;E-mail:zhwentao@sjtu.edu.cn
  • 作者简介:赵干(1995— ),男,硕士,研究方向为熔盐电解精炼仿真;E-mail:underworld@sjtu.edu.cn
  • 基金资助:
    中国科协青年人才托举项目(YESS20200327);国家自然科学基金项目(11805121)

Study on electrochemical coupling with flow field for uranium dendrite growth based on phase field method

ZHAO Gan(), XU Xiaorui, ZHOU Wentao(), WANG Yafei, WANG Dezhong   

  1. Shanghai Jiao Tong University,Shanghai 200240,China
  • Received:2023-05-12 Published:2024-04-10 Online:2024-04-18

摘要:

铀枝晶生长是导致乏燃料后处理电解精炼装置发生意外短路的潜在威胁因素,同时会使铀产物夹杂大量熔盐,影响产物纯度。为了更好地理解铀枝晶生长的微观机理,掌握阴极沉积形貌的控制方法,基于相场方法建立了铀在阴极的电沉积模型,研究了铀枝晶的底部沉积宽度、主枝晶干高度和总沉积面积等形貌参数对流场速度变化的依赖规律。发现外加流场的引入会使铀枝晶的底部沉积宽度降低37.18%,主枝晶干高度降低30.5%,总沉积面积降低49.3%。说明外加流场可以抑制铀枝晶生长,改善铀沉积形貌,但同时也会使破碎的枝晶须重新溶解到熔盐体系中,降低铀电解精炼效率。另外,通过对流场与电解电压、初始浓度等沉积条件耦合影响下铀枝晶形貌特征相图的分析可知,在实际电解精炼过程中,应在保证电解精炼效率的基础上尽量选择高初始浓度和高电解电压的沉积条件,同时设置合理的流场速度以获得理想的铀枝晶沉积形貌。

关键词: 铀枝晶生长, 相场方法, 流场

Abstract:

The growth of uranium dendrites is a potential threat factor that leads to accidental short circuit in the electrolytic refining unit of spent fuel reprocessing,and at the same time,it will incline a lot of molten salt in the uranium product,which will affect the purity of the product.In order to better understand the microscopic mechanism of uranium dendrite growth and grasp the control method of cathode deposition morphology,an electrodeposition model of uranium in cathode was established based on the phase field method.The dependence of topography parameters such as bottom deposition width,main dendrite height and total deposition area on the change of flow field velocity was studied.It was found that the introduction of external flow field could reduce the bottom deposition width of uranium dendrites by 37.18%,the main dendrite height was lowered by 30.5%,and the total deposition area was decreased by 49.3%.The results showed that the applied flow field could inhibit the growth of uranium dendrites and improve the morphology of uranium deposition,but at the same time,the broken dendrites would be redissolved into the molten salt system,and the efficiency of uranium electrolytic refining would be reduced.In addition,through the analysis of the phase diagram of uranium dendrite morphology under the coupling effect of deposition conditions such as flow field,electrolytic voltage and initial concentration,it could be seen that in the actual electrolytic refining process,a higher initial concentration and a lower electrolytic voltage should be selected as far as possible on the basis of ensuring the efficiency of electrolytic refining,and a reasonable flow field velocity should be set to obtain an ideal uranium dendrite deposition morphology.

Key words: uranium dendrite growth, phase field method, flow field

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