Dissolution Testing of a Metallic Waste Form in Chloride Brine. Scientific Basis for Nuclear Waste Management

摘要

This paper is intended for publication in the peer-reviewed proceedings from the Scientific Basis for Nuclear Waste Management (at the Fall 2006 meeting of the Materials Research Society). The same material was presented in a 15-minute talk. Argonne National Laboratory has developed an electrometallurgical process for conditioning spent sodium-bonded metallic reactor fuel from the Experimental Breeder Reactor II (EBR-II). One waste stream from this process consists of a metal waste form (MWF) whose baseline composition is stainless steel alloyed with 15 wt% Zr (SS-15Zr) and whose microstructure is a eutectic intergrowth of iron solid solutions and Fe-Zr-Cr-Ni intermetallics. This paper reports scanning electron microscope (SEM) observations of corrosion products formed during static immersion tests in which coupons of surrogate MWF containing 10 wt% U (SS-15Zr-10U) were immersed in solutions with nominal pH values of 3 and 4 and 1000 ppm added chloride for 70 days at 50 DGC. Although the majority of the surface areas of the coupons appear unchanged, linear areas with localized corrosion products apparently consisting of porous materials overlying corrosion-product-filled channels formed on both coupons, cross-cutting phase boundaries in the original eutectic microstructures. Many of the linear areas intersected the sample edge at notches present before the tests or followed linear flaws visible in pre-test images. Compositions of corrosion products differed significantly from the bulk composition, and the maximum observed concentration of U in corrosion products (approx. 25 at%) slightly exceeded the highest reported values in actinide-bearing phases in uncorroded surrogate MWF samples with comparable concentrations of U (approx. 17-19 at%).