摘要
为探究氯化锌(ZnCl2)与金属铀制备LiCl-KCl-UCl3初始熔盐体系的反应过程,本工作拟在500℃下的LiCl-KCl共晶熔盐中,首先对可能反应进行热力学计算,确定可能反应路径;再通过循环伏安法和原位吸收光谱法原位监测金属铀与ZnCl2的反应过程,并观察反应过程中熔盐的颜色变化,结合电感耦合等离子体质谱(ICP-MS)分析样品中元素含量的变化,对反应产物进行X射线衍射(XRD)、扫描电镜能谱分析(SEM-EDS)表征,综合确定反应行为和反应机制。研究结果表明:在金属铀与ZnCl2的反应过程中,Zn(Ⅱ)直接将铀金属氧化为U(Ⅲ),生成的Zn金属在铀金属表面形成U-Zn合金。ZnCl2与金属铀制备的电解精炼初始熔盐体系LiCl-KCl-UCl3过程,反应在240 min达到平衡,最终Zn质量分数维持在0.01%。
In order to investigate the reaction process of using zinc chloride(ZnCl_(2))and uranium metal to prepare the electrolytic refining initial molten salt system LiCl-KCl-UCl3.In LiCl-KCl eutectic molten salt at 500℃,the thermodynamic calculation of the possible reaction was firstly carried out,the calculated results were used to determine the possible reaction path.The reaction process of uranium metal and zinc chloride was monitored by in-situ cyclic voltammetry and in-situ absorption spectroscopy.The color change of molten salt during the reaction was observed,and the change of element content in the sample was analyzed by ICP-MS.The reaction products were characterized by XRD and SEM-EDS.Summary all of them,the reaction behavior and reaction mechanism were finally determined.The results show that during the process of uranium metal and zinc chloride,Zn(Ⅱ)directly oxidizes uranium metal to U(Ⅲ),and the resulting Zn metal forms U-Zn alloy on the surface of the uranium metal.The process of initial molten salt system LiCl-KCl-UCl3 prepared by zinc chloride and uranium metal reaches equilibrium within 240 min,the final mass fraction of Zn is maintained at 0.01%.
作者
曾国智
肖益群
姚本林
杨明帅
贾红伟
何辉
张琳
夏良树
ZENG Guo-zhi;XIAO Yi-qun;YAO Ben-lin;YANG Ming-shuai;JIA Hong-wei;HE Hui;ZHANG Lin;XIA Liang-shu(Institute of Nuclear Science and Technology,University of South China,Hengyang 421001,China;Department of Radiochemistry,China Institute of Atomic Energy,Beijing 102413,China)
出处
《核化学与放射化学》
CAS
CSCD
北大核心
2024年第3期205-212,I0001,共9页
Journal of Nuclear and Radiochemistry
