Zirconium in the nuclear industry : 15th international symposium

Hydrogen pickup of zirconium-based fuel cladding and structural materials during in-reactor corrosion can degrade fuel components because the ingress of hydrogen can lead to the formation of brittle hydrides. In the boiling water reactor (BWR) environment, Zircaloy-2 fuel cladding and structural components such as water rods and channels can experience accelerated hydrogen pickup, whereas Zircaloy-4 components exposed to similar conditions do not. Because the principal difference between the two alloys is that Zircaloy-2 contains nickel, accelerated hydrogen pickup has been hypothesized to result from the presence of nickel. However, an understanding of the mechanism by which this acceleration occurs is still lacking. We investigated the link between hydrogen pickup and the oxidation behavior of alloying elements when incorporated into the oxide layers formed on zirconium alloys when corroded in the reactor. Manuscript received March 20, 2016; accepted for publication November 10, 2016. Pennsylvania State University, Dept. of Mechanical and Nuclear Engineering, University Park, PA 16802 A. S. http://orcid.org/0000-0001-8515-2756 A. M. http://orcid.org/0000-0001-5735-1491 Electric Power Research Institute, Palo Alto, CA 94304 Advanced Photon Source, Argonne National Laboratory, Argonne, IL 60439 ASTM 18th International Symposium on Zirconium in the Nuclear Industry on May 15-19, 2016 in Hilton Head, SC. Copyright VC 2018 by ASTM International, 100 Barr Harbor Drive, PO Box C700, West Conshohocken, PA 19428-2959. ZIRCONIUM IN THE NUCLEAR INDUSTRY: 18TH INTERNATIONAL SYMPOSIUM 524 STP 1597, 2018 / available online at www.astm.org / doi: 10.1520/STP159720160076 Copyright by ASTM Int'l (all rights reserved); Mon May 13 12:45:02 EDT 2019 Downloaded/printed by Penn State University (Penn State University) pursuant to License Agreement. No further reproductions authorized. Synchrotron radiation microbeam X-ray absorption near-edge spectroscopy (XANES) at the Advanced Photon Source was performed on carefully selected BWR-corroded Zircaloy-2 water rods at an assembly-averaged burnup ranging from 32.8 to 74.6 GWd/MTU to determine the oxidation states of alloying elements, such as iron and nickel, within the oxide layers as a function of distance from the oxide-metal interface at high burnup. Samples were chosen for comparison based on having similar oxide thicknesses, processing, elevation, reactors, and fluences but different hydrogen pickup fractions. Examinations of the oxide layers formed on these samples showed that (1) the oxidation states of these alloying elements changed with distance from the oxide-metal interface, (2) these elements exhibited delayed oxidation relative to the host zirconium, and (3) nickel in Zircaloy-2 remained metallic in the oxide layer at a longer distance from the oxide-metal interface than iron. An analysis of these results showed an apparent correlation between the delayed oxidation of nickel and higher hydrogen pickup of Zircaloy-2 at high burnup.

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