Solubility and Valence Variation of Ce in Low-Alkali Borosilicate Glass and Glass Network Structure Analysis

Abstract

Low-alkali borosilicate glass was used as the immobilization substrate, and Ce was used to replicate the trivalent and tetravalent actinides, in order to create simulated waste glass through melt heat treatment. The valence of Ce and solubility of CeO2 in waste glass were studied as well as its network structure and thermal and chemical stability. The solubility of Ce in waste glass was examined by XRD and SEM. The network structure was examined by Raman spectroscopy. The valence of Ce was determined by X-ray photoelectron spectroscopy. Thermal analysis and product consistency (PCT) were employed to determine the thermal and chemical stability of waste glasses. The results show that the solubility of cerium in low-alkali borosilicate glasses is at least 25.wt.% and precipitates a spherical CeO2 crystalline phase when it exceeds the solid solution limit; Ce is immobilized in the glass by entering the interstices of the glass network. Depolymerization and the transition from [BO3] to [BO4] occurs when CeO2 doping levels rise. About 60 percent of Ce4+ is converted to Ce3+, and the thermal stability of glass rises then falls with the increase of CeO2. All samples exhibit strong leaching resistance, with the average mass loss of Ce at 28 days being less than 10−4 gm−2d−1.