PNNL

Abstract

Immersion of commercial spent nuclear fuel (CSNF) in deionized water produced two novel corrosion products after a two-year contact period. Another unexpected result was that suspensions of aggregates were observed to form at the air-water interface for each of five samples. These solids were characterized, by SEM and XRD to be nearly pure metastudtite (UO4-2H20); while the corrosion present on the surface of the fuel itself was determined to be studtite (UO4-2H20). The occurrence of the floating phase prompted a radiochemical analysis of these solids. This chemical analysis was a unique opportunity to study the relatively pure corrosion phase for incorporation of radionuclides. The analysis indicated that high concentration of 90Sr, 137Cs, 99Tc, and that lower concentrations 237Np, 238, 239Pu and 243, 244Cm had partitioned with the air-water interface aggregates. The concentrations of 241Am were two orders of magnitude lower than the expected inventory in the suspended solids. The radiochemical analyses of the several leachate samples provide preliminary solubility data for the hydrogen peroxide leaching of CSNF and these data are compared to leaching of the same fuel in J-13 and deionized waters. The extent of fuel dissolution in these media are discussed.