Evaluation of a Sulfate Solubility Limit Greater Than 0.65 Weight Percent in Sludge Batch 10 Glasses
- Savannah River National Laboratory (SRNL), Aiken, SC (United States); Savannah River Nuclear Solutions (SRNS), Aiken, SC (United States)
- Savannah River Nuclear Solutions (SRNS), Aiken, SC (United States)
Previous laboratory-scale crucible testing with batch chemicals confirmed that the sulfate (SO42-) limit for Sludge Batch 10 (SB10) was 0.65 weight percent (wt.%) in glass. This limit signifies that 0.65 wt.% SO42- can be retained in the glass without the formation of a sulfate phase. The Defense Waste Processing Facility imposes this constraint in the Material Tracking Program. Based on preliminary calculations to support the Material Tracking Program, it was anticipated that transfer volumes of the monosodium titanate/sludge solids (MST/SS) stream from the Salt Waste Processing Facility (SWPF) may need to be reduced to maintain projected sulfate concentrations below 0.65 wt.% in glass. Savannah River Mission Completion requested that the Savannah River National Laboratory perform additional sulfate testing to determine whether a sulfate solubility limit greater than 0.65 wt.% is feasible for SB10, which could allow for higher transfer volumes of the MST/SS stream. This report documents the results of the testing at higher sulfate concentrations for the glass composition region defined by the most recent SB10 projection (November 2022) and Frits 473 and 625. Frit 473 was recommended for SB10 and Frit 625 was used during SB9 processing and the SB9 to SB10 transition. A total of twenty-one glass compositions were developed based on the expected compositional variables, which include sludge-only (SO) and coupled processing with the SWPF, waste loading (WL), and frit composition. The target sulfate concentrations were varied from 0.65-0.85 wt.% at 32 and 40% WL. Each glass was prepared from reagent grade chemicals and melted at 1150 °C. Visual observations were used to confirm the presence of a sulfate salt phase on the cooled glass surfaces. Representative samples of each glass were submitted for chemical composition analysis by inductively coupled plasma-optical emission spectroscopy and Cs analysis by inductively coupled plasma-mass spectrometry. Overall the majority of mean measured values are consistent with the target values for each major oxide of interest with less than 5% error. The percent errors for the measured SO42- concentrations are generally less than 10%, which is comparable with previous sulfate solubility study measurements and acceptable. Only the SO glasses based on Frit 625 formed a sulfate phase at a 0.80 wt.% SO42- target concentration at both 32 and 40% WL. The remainder of the glasses did not form a sulfate layer. Due to the formation of the sulfate phase, the limit is conservatively set at 0.70 wt.% based on the measured sulfate concentrations of 0.71 wt.% and 0.75 wt.% for these two glasses. None of the SO or coupled operation glasses based on Frit 473 formed a sulfate salt phase, which supports a sulfate limit of 0.80 wt.%. The following SO42- concentration limits are recommended during SO and coupled SB10 processing: (1) 0.70 wt.% during processing with Frit 625, and (2) 0.80 wt.% during processing with Frit 473.
- Research Organization:
- Savannah River Site (SRS), Aiken, SC (United States); Savannah River National Laboratory (SRNL), Aiken, SC (United States)
- Sponsoring Organization:
- USDOE Office of Environmental Management (EM)
- DOE Contract Number:
- 89303321CEM000080
- OSTI ID:
- 1991098
- Report Number(s):
- SRNL-STI-2023-00207; TRN: US2404321
- Country of Publication:
- United States
- Language:
- English
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