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Title: Evaluation of Technetium Getters to Improve the Performance of Cast Stone

Cast Stone has been selected as the preferred waste form for solidification of aqueous secondary liquid effluents from the Hanford Tank Waste Treatment and Immobilization Plant (WTP) process condensates and low-activity waste (LAW) melter off-gas caustic scrubber effluents. Cast Stone is also being evaluated as a supplemental immobilization technology to provide the necessary LAW treatment capacity to complete the Hanford tank waste cleanup mission in a timely and cost effective manner. One of the major radionuclides that Cast Stone has the potential to immobilize is technetium (Tc). The mechanism for immobilization is through the reduction of the highly mobile Tc(VII) species to the less mobile Tc(IV) species by the blast furnace slag (BFS) used in the Cast Stone formulation. Technetium immobilization through this method would be beneficial because Tc is one of the most difficult contaminants to address at the U.S. Department of Energy (DOE) Hanford Site due to its complex chemical behavior in tank waste, limited incorporation in mid- to high-temperature immobilization processes (vitrification, steam reformation, etc.), and high mobility in subsurface environments. In fact, the Tank Closure and Waste Management Environmental Impact Statement for the Hanford Site, Richland, Washington (TC&WM EIS) identifies technetium-99 (99Tc) as one of themore » radioactive tank waste components contributing the most to the environmental impact associated with the cleanup of the Hanford Site. The TC&WM EIS, along with an earlier supplemental waste-form risk assessment, used a diffusion-limited release model to estimate the release of different contaminants from the WTP process waste forms. In both of these predictive modeling exercises, where effective diffusivities based on grout performance data available at the time, groundwater at the 100-m down-gradient well exceeded the allowable maximum permissible concentrations for 99Tc. (900 pCi/L). Recent relatively short-term (63 day) leach tests conducted on both LAW and secondary waste Cast Stone monoliths indicated that 99Tc diffusivities were at or near diffusivities where the groundwater at the 100-m down-gradient well would exceed the allowable maximum permissible 99Tc concentrations. There is, therefore, a need and an opportunity to improve the retention of Tc in the Cast Stone waste form. One method to improve the performance of the Cast Stone waste form is through the addition of “getters” that selectively sequester Tc inside Cast Stone.« less
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
OSTI Identifier:
1228352
Report Number(s):
PNNL--23667 Rev. 1;EMSP-RPT--026 Rev1
EY4049110; TRN: US1600027
DOE Contract Number:
AC05-76RL01830
Resource Type:
Technical Report
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; TECHNETIUM 99; WASTE FORMS; LIQUID WASTES; HANFORD RESERVATION; WASTE PROCESSING; TANKS; GROUND WATER; MAXIMUM PERMISSIBLE CONCENTRATION; PERFORMANCE; TEMPERATURE RANGE 0400-1000 K; GETTERS; EVALUATION; LEACHING; REDUCTION; SOLIDIFICATION; UNDERGROUND; ENVIRONMENTAL IMPACTS; ABUNDANCE; DIFFUSION; GROUTING; MOBILITY; RETENTION; SIMULATION; SLAGS; RADIONUCLIDE MIGRATION; VITRIFICATION; GASEOUS WASTES; LOW-LEVEL RADIOACTIVE WASTES Cast stone