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Title: High-temperature leaching of an actinide-bearing, simulated high-level waste glass

Abstract

The chemical durability of a simulated high-level waste glass when exposed to high-temperature geologic solutions was investigated. In this study, simulated high-level waste glass-beads (76 to 68 glass)l doped with technetium, uranium, neptunium, plutonium, curium and americium were leached in deionized water, Waste Isolation Pilot Plant salt brine B, and 0.03M sodium bicarbonate solution at 150 and 250/sup 0/C for 2, 4, 8, 16, and 32 days. The resulting solutions were analyzed for several nonradioactive glass components and for the radioactive dopants. The glass exhibited incongruent leaching behavior, i.e., the normalized releases (g-glass/m/sup 2/) based on the different elements spanned four orders of magnitude. Normalized releases based on boron, molybdenum, sodium, cesium, silicon, and technetium were the same within a factor of three. Most of the nonradioactive components of the glass were released more to the salt brine than to the other two solutions. However, silicon, boron, molybdenum, technetium, and the actinides had their lowest releases in the salt brine. Reaction-layer thickness on the glass surface and weight losses of the glass beads were also smallest in the brine solution. Actinide releases were highest in the sodium bicarbonate solution. Calcium, strontium and barium releases decreased with time and temperature; themore » releases of most other elements increased with time and temperature. Solubility appears to be limiting the release of most elements. The leachate pH is controlled by chemical species within the original leachant and by species released as the glass leached. Carbonate ion complexes with some elements including uranium, effectively increasing their release. The more soluble elements including sodium, boron, molybdenum and technetium provide an indication of the actual rate of reaction between the glass and water.« less

Authors:
; ;
Publication Date:
Research Org.:
Pacific Northwest Lab., Richland, WA (USA)
OSTI Identifier:
6494366
Report Number(s):
PNL-3172
ON: DE83008755
DOE Contract Number:
AC06-76RL01830
Resource Type:
Technical Report
Resource Relation:
Other Information: Portions are illegible in microfiche products. Original copy available until stock is exhausted
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 36 MATERIALS SCIENCE; GLASS; LEACHING; TEMPERATURE EFFECTS; AMERICIUM; BORON; BRINES; CESIUM; CURIUM; HIGH-LEVEL RADIOACTIVE WASTES; MOLYBDENUM; NEPTUNIUM; PLUTONIUM; RADIOACTIVE WASTE DISPOSAL; SALT DEPOSITS; SILICON; SIMULATION; SODIUM; SODIUM CARBONATES; TECHNETIUM; UNDERGROUND DISPOSAL; URANIUM; WATER; ACTINIDES; ALKALI METAL COMPOUNDS; ALKALI METALS; CARBON COMPOUNDS; CARBONATES; DISSOLUTION; ELEMENTS; GEOLOGIC DEPOSITS; HYDROGEN COMPOUNDS; MANAGEMENT; MATERIALS; METALS; OXYGEN COMPOUNDS; RADIOACTIVE MATERIALS; RADIOACTIVE WASTES; SEMIMETALS; SEPARATION PROCESSES; SODIUM COMPOUNDS; TRANSITION ELEMENTS; TRANSPLUTONIUM ELEMENTS; TRANSURANIUM ELEMENTS; WASTE DISPOSAL; WASTE MANAGEMENT; WASTES; 052002* - Nuclear Fuels- Waste Disposal & Storage; 360604 - Materials- Corrosion, Erosion, & Degradation

Citation Formats

Westsik, J.H. Jr., Harvey, C.O., and Kuhn, W.L. High-temperature leaching of an actinide-bearing, simulated high-level waste glass. United States: N. p., 1983. Web. doi:10.2172/6494366.
Westsik, J.H. Jr., Harvey, C.O., & Kuhn, W.L. High-temperature leaching of an actinide-bearing, simulated high-level waste glass. United States. doi:10.2172/6494366.
Westsik, J.H. Jr., Harvey, C.O., and Kuhn, W.L. Tue . "High-temperature leaching of an actinide-bearing, simulated high-level waste glass". United States. doi:10.2172/6494366. https://www.osti.gov/servlets/purl/6494366.
@article{osti_6494366,
title = {High-temperature leaching of an actinide-bearing, simulated high-level waste glass},
author = {Westsik, J.H. Jr. and Harvey, C.O. and Kuhn, W.L.},
abstractNote = {The chemical durability of a simulated high-level waste glass when exposed to high-temperature geologic solutions was investigated. In this study, simulated high-level waste glass-beads (76 to 68 glass)l doped with technetium, uranium, neptunium, plutonium, curium and americium were leached in deionized water, Waste Isolation Pilot Plant salt brine B, and 0.03M sodium bicarbonate solution at 150 and 250/sup 0/C for 2, 4, 8, 16, and 32 days. The resulting solutions were analyzed for several nonradioactive glass components and for the radioactive dopants. The glass exhibited incongruent leaching behavior, i.e., the normalized releases (g-glass/m/sup 2/) based on the different elements spanned four orders of magnitude. Normalized releases based on boron, molybdenum, sodium, cesium, silicon, and technetium were the same within a factor of three. Most of the nonradioactive components of the glass were released more to the salt brine than to the other two solutions. However, silicon, boron, molybdenum, technetium, and the actinides had their lowest releases in the salt brine. Reaction-layer thickness on the glass surface and weight losses of the glass beads were also smallest in the brine solution. Actinide releases were highest in the sodium bicarbonate solution. Calcium, strontium and barium releases decreased with time and temperature; the releases of most other elements increased with time and temperature. Solubility appears to be limiting the release of most elements. The leachate pH is controlled by chemical species within the original leachant and by species released as the glass leached. Carbonate ion complexes with some elements including uranium, effectively increasing their release. The more soluble elements including sodium, boron, molybdenum and technetium provide an indication of the actual rate of reaction between the glass and water.},
doi = {10.2172/6494366},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Mar 01 00:00:00 EST 1983},
month = {Tue Mar 01 00:00:00 EST 1983}
}

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