Progressing zirconium-alloy corrosion models using synchrotron xanes

Abstract

The corrosion and hydrogen pickup of in-reactor zirconium-based cladding is currently limiting the maximum fuel burnup in light-water reactors. Since the oxidation rate and hydrogen pickup fraction of zirconium alloys vary significantly as a function of exposure time, burnup, and alloy composition, it is critical to better understand the underlying mechanisms to model and predict corrosion behavior. Following the analysis of ~500 autoclave coupons, a physically based zirconium-alloy corrosion model founded on first principles, named “Coupled Current Charge Compensation (C4)”, has been developed. The model reproduces the differences in oxidation kinetics and hydrogen pickup between different zirconium alloys, such as Zr-Nb and Zircaloy-4. Since oxidized solute elements affect the corrosion process through a space-charge compensation mechanism, synchrotron nano-beam X-ray Absorption Near-Edge Spectroscopy has been performed on multiple oxidized Zr-Nb alloys to determine the oxidation-state profile of niobium in the oxide layer. The results inform the C4 model and the associated hydrogen pickup fraction.