Effect of chlorine and chromium on sulfur solubility in low-activity waste glass

Jin, Tongan; Rivers, Eden L.; Kim, Dongsang; Droubay, Timothy C.; Jahrman, Evan P.; Mar, Derek; Weese, Brigitte L.; Seidler, Gerald T.; Kruger, Albert A.

doi:10.1111/ijag.16540

Effect of chlorine and chromium on sulfur solubility in low-activity waste glass

Journal Article · Tue Sep 21 00:00:00 EDT 2021 · International Journal of Applied Glass Science

DOI:https://doi.org/10.1111/ijag.16540· OSTI ID:1829503

^[1]; Rivers, Eden L. ^[1]; ^[1]; ^[1]; Jahrman, Evan P. ^[2]; Mar, Derek ^[3]; Weese, Brigitte L. ^[4]; Seidler, Gerald T. ^[5]; Kruger, Albert A. ^[6]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); USDOE Office of River Protection (ORP), Richland, WA (United States)
Univ. of Washington, Seattle, WA (United States)
Washington State Univ., Pullman, WA (United States); Washington State Department of Ecology, Richland, WA (United States)

According to an empirical sulfur solubility model developed from over 200 simulated low-activity waste (LAW) glasses, chlorine and chromium show strong effects on lowering sulfur solubility in glass. This work was aimed at understanding the mechanism behind the negative effect of chlorine and chromium on sulfur solubility. A simplified LAW glass was prepared and saturated by sodium sulfate, sodium chloride, and sodium chromate salts as single components and as mixtures with different ratios at 25 mol%, 50 mol%, and 75 mol% of sulfate mixed with chloride or chromate. A crucible-scale salt-saturation was performed by mixing the crushed glass powder with an excess amount of salts, melting at 1150 °C for one hour, and quenching. Three mixing-melting-quenching cycles were applied to determine saturation concentrations of sulfur, chromium, and chlorine incorporated into the simplified LAW glass. The glass compositions were analyzed by inductively coupled plasma–atomic emission spectroscopy, ion chromatography, and X-ray emission spectroscopy. It is proposed that the negative effect of chlorine and chromium on sulfur solubility can be explained based on the simple hypothesis that sulfur, chlorine, and chromium are present in the glass as anions competing for the voids or interstitial sites of the glass matrix, and that their solubility strongly depends on the effective size of corresponding anions.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC05-76RL01830; NE0008597

OSTI ID:: 1829503

Report Number(s):: PNNL-SA--146955

Journal Information:: International Journal of Applied Glass Science, Journal Name: International Journal of Applied Glass Science Journal Issue: 1 Vol. 13; ISSN 2041-1286

Publisher:: American Ceramic SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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