摘要
As a pivotal technology for high-level liquid waste (HLW) treatment, vitrification plays a crucial role in ensuring the sustainable development of nuclear energy. The two-step vitrification process, which involves initial calcination of HLW into solid calcine followed by melting with base glass, has demonstrated significant improvements in immobilization efficiency. This study investigated the capacity of simulated HLW calcine to be incorporated within a borosilicate glass matrix.Through comprehensive characterization techniques including field emission scanning electron microscopy coupled with energy dispersive spectroscopy (SEM-EDS), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), and Raman spectroscopy, the effects of calcine content (18-32 wt%) on the microstructure, chemical composition, phase distribution, and network structure of the vitrified matrixs were examined. Homogeneous glass matrices are achieved at 18–26 wt% calcine content, while phase separation and crystalline precipitation occur at higher concentrations. However, when the content reaches 28 wt%, the initial precipitation of granular CaMoO 4 crystals occurs, maintaining relatively uniform distribution. Further increasing the content to 30 wt% leads to the formation of acicular CaMoO 4 phases accompanied by minor Zr x Ce 1-x O 2 particle precipitation. Notably, at 32 wt% calcined product content, a distinct phase separation layer emerges on the surface of the vitrified matrix, with a substantial increase in Zr x Ce 1-x O 2 precipitates. These research findings have clarified the incorporation capacity limits of simulated HLW calcine in borosilicate glass matrix, providing valuable theoretical guidance for enhancing waste loading in vitrified forms during the vitrification process.
危险品化学品经营许可证(带存储)