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Electrochemical reduction behavior of simplified simulants of vitrified radioactive waste in molten CaCl2
Journal of Nuclear Materials ( IF 3.1 ) Pub Date : 2018-03-05 , DOI: 10.1016/j.jnucmat.2018.03.006
Yumi Katasho , Kouji Yasuda , Toshiyuki Nohira

The electrochemical reduction of two types of simplified simulants of vitrified radioactive waste, simulant 1 (glass component only: SiO2, B2O3, Na2O, Al2O3, CaO, Li2O, and ZnO) and simulant 2 (also containing long-lived fission product oxides, ZrO2, Cs2O, PdO, and SeO2), was investigated in molten CaCl2 at 1103 K. The behavior of each element was predicted from the potential−pO2− diagram constructed from thermodynamic data. After the immersion of simulant 1 into molten CaCl2 without electrolysis, the dissolution of Na, Li, and Cs was confirmed by inductively coupled plasma atomic emission spectrometry and mass spectrometry analysis of the samples. The scanning electron microscopy/energy dispersive X-ray and X-ray diffraction analyses of simulants 1 and 2 electrolyzed at 0.9 V vs. Ca2+/Ca confirmed that most of SiO2 had been reduced to Si. After the electrolysis of simulants 1 and 2, Al, Zr, and Pd remained in the solid phase. In addition, SeO2 was found to remain partially in the solid phase and partially evaporate, although a small quantity dissolved into the molten salt.



中文翻译:

熔融CaCl 2中玻璃化放射性废料简化模拟物的电化学还原行为

两种类型的玻璃化放射性废物简化模拟物的电化学还原,模拟物1(仅玻璃成分:SiO 2,B 2 O 3,Na 2 O,Al 2 O 3,CaO,Li 2 O和ZnO)和模拟物2 (还包含长寿命的裂变产物氧化物ZrO 2,Cs 2 O,PdO和SeO 2)在1103 K的熔融CaCl 2中进行了研究。每种元素的行为均通过电势-p O 2-图预测根据热力学数据构建。将模拟物1浸入熔融的CaCl 2中之后在不进行电解的情况下,通过电感耦合等离子体原子发射光谱法和样品的质谱分析法确认了Na,Li和Cs的溶解。对在0.9 V vs. Ca 2+ / Ca下电解的模拟物1和2的扫描电子显微镜/能量色散X射线和X射线衍射分析证实,大多数SiO 2已被还原为Si。在模拟物1和2电解后,Al,Zr和Pd保留在固相中。另外,发现SeO 2尽管少量溶解在熔融盐中,但部分保留在固相中并部分蒸发。

更新日期:2018-03-05
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