Effect of Sulfate on Rhenium Partitioning during Melting of Low-Activity Waste Glass Feeds
The volatile loss of technetium-99 (99Tc) is a major concern of the low-activity waste (LAW) vitrification at Hanford. We investigated the incorporation and volatile loss of Re (a nonradioactive surrogate for 99Tc) during batch-to-glass conversion up to 1100°C. The AN-102 feed, which is one of the representative Hanford LAW feeds, containing 0.59 wt% of SO3 (in glass if 100% retained) was used. The modified sulfate-free AN-102_0S feed was also tested to investigate the effect of sulfate on Re partitioning and retention during melting. After heating of the dried melter feed (mixture of LAW simulant and glass forming/modifying additives) to different temperatures, the heat-treated samples were quenched. For each heat-treated sample, the salts (soluble components in room temperature leaching), early glass forming melt (soluble components in 80°C leaching), and insoluble solids were separated by a two-step leaching and the chemical compositions of each phase were quantitatively analyzed. The final retention ratio of AN-102 and AN-102_0S in glass (insoluble solids) are 32% and 63% respectively. The presence of sulfate in the salt phase between 600 and 800°C leads to a significantly higher Re loss via volatilization from the salt layer. At ≥800°C, for both samples, there is no more incorporation of Re into the insoluble phase because: for AN-102_0S there is no salt left i.e., the split into the insoluble and gas phases is complete by 800°C and for AN-102 all the Re contained in the remaining salt phase is lost through volatilization. The present results on the effect of sulfate, although not directly applicable to LAW vitrification in the melter, will be used to understand the mechanism of Re incorporation into glass to eventually develop the methods that can increase the 99Tc retention during LAW vitrification at Hanford.
- Research Organization:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 1254603
- Report Number(s):
- PNNL-SA-99664; 830403000
- Resource Relation:
- Conference: WM Symposia (WM 2014): 40 Years of Meeting Global Radioactive Waste Management Challenges, March 2-6, 2014, Phoenix, Arizona, Paper No. 14116
- Country of Publication:
- United States
- Language:
- English
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