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Title: Oxidative corrosion of spent UO{sub 2} fuel in vapor and dripping groundwater at 90 C

Conference ·
OSTI ID:20015788

Oxidative dissolution of spent UO{sub 2} fuel in vapor and dripping groundwater at 90 C occurs via general corrosion at fragment surfaces. Dissolution along fuel-grain boundaries is also evident in samples contacted by the largest volumes of groundwater, and corroded grain boundaries extend at least 20 or 30 grains deep (>200 {micro}m), possibly throughout mm-sized fragments. Apparent dissolution of fuel along defects that intersect grain boundaries has produced 50 to 200 nm-diameter dissolution pits that penetrate 1--2 {micro}m into each grain, giving rise to a worm-like texture along fuel-grain boundaries. Sub-micrometer-sized fuel shards are common between fuel grains and may contribute to the reactive surface area of fuel exposed to groundwater. Outer surfaces of reacted fuel fragments develop a fine-grained layer of corrosion products adjacent to the fuel (5--15 {micro}m thick). A more coarsely crystalline layer of corrosion products commonly covers the fine-grained layer, the thickness of which varies considerably among samples (from less than 5 {micro}m to greater than 40 {micro}m). The thickest and most porous corrosion layers develop on fuel fragments exposed to the largest volumes of groundwater. Corrosion-layer compositions depend strongly on water flux, with uranyl oxy-hydroxides predominating in vapor experiments, and alkali and alkaline earth uranyl silicates predominating in high drip-rate experiments. Low drip-rate experiments exhibit a complex assemblage of corrosion products, including phases identified in vapor and high drip-rate experiments.

Research Organization:
Argonne National Lab., IL (US)
Sponsoring Organization:
USDOE
DOE Contract Number:
W-31109-ENG-38
OSTI ID:
20015788
Resource Relation:
Conference: 1998 Materials Research Society Fall Meeting, Boston, MA (US), 11/30/1998--12/04/1998; Other Information: Single article reprints are available from University Microfilms Inc., 300 North Zeeb Road, Ann Arbor, Michigan 48106; PBD: 1999; Related Information: In: Scientific basis for nuclear waste management XXII. Materials Research Society symposium proceedings: Volume 556, by Wronkiewicz, D.J.; Lee, J.H. [eds.], 1355 pages.
Country of Publication:
United States
Language:
English