PNNL

Abstract

To predict the long-term fate of low- and high-level waste forms in the subsurface over geologic time scales, it is important to understand the behavior of the corroding waste forms under conditions the mimic to the open flow and transport properties of a subsurface repository. Fluidized bed steam reformation (FBSR), a supplemental treatment technology option, is being considered as a waste form for the immobilization of low-activity tank waste. To obtain the fundamental information needed to evaluate the behavior of the FBSR waste form under repository relevant conditions and to monitor the long-term behavior of this material, an accelerated weathering experiment is being conducted with the pressurized unsaturated flow (PUF) apparatus. Unlike other accelerated weathering test methods (product consistency test, vapor hydration test, and drip test), PUF experiments are conducted under hydraulically unsaturated conditions. These experiments are unique because they mimic the vadose zone environment and allow the corroding waste form to achieve its final reaction state. Results from this on-going experiment suggest the volumetric water content varied as a function of time and reached steady state after 160 days of testing. Unlike the volumetric water content, periodic excursions in the solution pH and electrical conductivity have been occurring consistently during the test. Release of elements from the column illustrates a general trend of decreasing concentration with increasing reaction time. Normalized concentrations of K, Na, P, Re (a chemical analogue for 99Tc), and S are as much as 1 × 104 times greater than Al, Cr, Si, and Ti. After more than 600 days of testing, the solution chemistry data collected to-date illustrate the importance of understanding the long-term behavior of the FBSR product under conditions that mimic the open flow and transport properties of a subsurface repository.