Microstructure and Cs Behavior of Ba-Doped Aluminosilicate Pollucite Irradiated with F+ Ions

作者:Jiang Weilin*; Kovarik Libor; Zhu Zihua; Varga Tamas; Engelhard Mark H; Bowden Mark E
来源:Journal of Physical Chemistry C, 2014, 118(31): 18160-18169.
DOI:10.1021/jp5045223

摘要

Radionuclide Cs-137 is one of the major fission products that dominate heat generation in spent fuels over the first 300 years. A durable waste form for Cs-137 that decays to Ba-137 is needed to minimize its environmental impact. Aluminosilicate pollucite CsAlSi2O6 is selected as a model waste form to study the decay-induced structural effects. Whereas Ba-containing precipitates are not present in charge-balanced Cs0.9Ba0.05AlSi2O6, they are found in Cs0.9Ba0.1AlSi2O6 and identified as monoclinic Ba2Si3O8. Pollucite is susceptible to electron-irradiation-induced amorphization. The threshold density of electronic energy deposition for amorphization was determined to be similar to 235 keV/nm(3). Pollucite can be readily amorphized under F+ ion irradiation at 673 K. A significant amount of Cs diffusion and release from the amorphized pollucite occurs during the irradiation. However, cesium is immobile in the crystalline structure under He+ ion irradiation at room temperature. The critical temperature for amorphization is not higher than 873 K under F+ ion irradiation. If kept at or above 873 K all the time, the pollucite structure is unlikely to be amorphized; Cs diffusion and release are improbable. A general discussion regarding pollucite as a potential waste form is provided in this report.

  • 出版日期2014-8-7