Sandia solidification process: consolidation and characterization. Part I. Consolidation studies

Abstract

The consolidation behavior of a complex polycrystalline ceramic nuclear waste form composed of titanates, zeolite, and metallic silicon was studied. Initial solidification takes place by an ion exchange process. The resulting powder exhibits a large surface area, approximately 350 m/sup 2//g, and several decomposition, crystallization and phase change reactions from room temperature to 1100/sup 0/C. In spite of the large surface area, consolidation by cold pressing and atmospheric sintering to 1100/sup 0/C was not satisfactory. Vacuum hot pressing was found to produce fully dense pellets (less than 1% residual porosity) under very mild conditions, 6.9 MPa (1100 psi) and 1100/sup 0/C. The dominant densification mechanism was viscous flow. Under less than optimum hot pressing conditions, three stages of densification were observed. Initial densification took place by particle rearrangement which was described with a viscous flow model. Second stage densification occurred by a solution-precipitation process controlled by a phase boundary dissolution reaction. In several cases, a third, final densification stage was observed. Detailed studies describe the effects of heating rate, processing temperature, pressure, residence time, atmosphere, composition, heat treatment, and the addition of consolidation aids on the densification behavior. In addition, fully radioactive high level mixed fission product titanate/waste pellets (1.27 cm diameter) were hot pressed at Oak Ridge National Laboratory to demonstrate the feasibility of such a process in a remotely operated hot cell. High density uniform pellets were obtained.