Study of the effect of Ca/Mg alkali-oxides ratio on the structure of a glass-ceramic based on an aluminosilicated glass containing 2wt.% of zirconolite crystalline phase

Abstract

New nuclear glass-ceramics are extensively studied for the radioactive waste confinement, due to the double confinement conferred by the glass-ceramics. In this study, a glass-ceramic constituted by an aluminosilicate glass in the system: SiO2-Al2O3-CaO-MgOZrO2-TiO2, containing 2wt.% of Ca0.83Ce0.17ZrTi1.66Al0.34O7 zirconolite, has been synthesized by the discontinuous method. Cerium, an actinide surrogate is introduced both in the glass and ceramic phases. The synthesis is performed by a double melting at 1350 °C, followed by a nucleation at 564°C, during 2 h, and a crystal growth at 1010°C during 3 h. Then effect of Ca / Mg ratio on the distribution of the crystalline network in the material was studied for Ca / Mg ratios ranging from 0.4 to 5.5. For the whole of the materials, Archimedes density is about 2.80 g/cm3 . X-ray diffraction (XRD) analysis shows that the increase of Ca/Mg ratio leads to the increase of aluminosilicated crystalline phases with high Ca contents; the materials molar volumes remaining constant. The zirconolite phase is not affected by these additive aluminosilicated phases. The scanning electron microscopy analysis (SEM) coupled with energy dispersive X-ray (EDX) analysis confirmed these results; and shows the uniformity of distribution of the ceramics in the bulk of the materials