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Parker-Quaife, Elizabeth H

Publications and source records attributed to Parker-Quaife, Elizabeth H.

Milestone 1.2.16. Reconciling the Impacts of Thermal Pretreatment on Radiation-Induced H2 Generation from Aluminum-Clad Spent Nuclear Fuel Surrogate Materials

To support the technical basis for the extended dry storage of aluminum-clad spent nuclear fuel (ASNF), thermal pretreatment procedures to minimize the radiation-induced generation of molecular hydrogen (H2) have been investigated. The aim of thermal pretreatment is to eliminate the residual adsorbed water content on the ASNF’s corrosion layers, precursors for H2 generation. To date, irradiation studies in this area have found conflicting results for the effectiveness of thermal pretreatment procedures. The aim of this study was to reconcile those differences. However, the presented results, which utilized a modified in situ thermal pretreatment procedure, afforded H2 yield data that further indicates that thermal pretreatment does not significantly reduce the radiation-induced yield of H2 from gamma irradiated ASNF surrogate materials. Assessment of the differences between thermal pretreatment studies suggests that stainless-steel—present in the irradiation setup of studies that demonstrated a reduction in the yield of H2 with thermal pretreatment—may afford not only unanticipated interfacial chemistry, but also the formation and radiolytic contribution of iron oxides to the chemistry underpinning the formation of H2 in these systems. Given the Department of Energy Standard Canister—proposed for the extended dry storage of ASNF—is predominantly composed of stainless-steel, the potential contribution of stainless-steel and its corrosion layers to radiolytic H2 production should be further investigated. This research was funded by the U.S. Department of Environmental Management, Office of Technology Development, under contract DE-AC07-05ID14517.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Milestone 1.2.9: Radiolytic Gas Generation Measurements from Helium Backfilled Samples of AA1100 and AA6061 Coupons

Nearly 18 metric tons of aluminum-clad spent nuclear fuel (ASNF) is safely managed by the U.S. Department of Energy (DOE). These assemblies are currently in interim storage, with the intention of extended storage (>50 years) until final disposal. Strategies for the continued safe storage of this material are under evaluation, of which a key criterion is the extent of molecular hydrogen gas (H2) formation from the radiolysis of hydrated (oxy)hydroxide aluminum corrosion layers arising from in-reactor and wet storage conditions. Radiation-induced H2 formation has the potential to compromise cladding and storage canister integrity, in addition to promoting the formation of unfavorable gaseous environments. Consequently, understanding this radiation-induced phenomenon is essential for the development of predictive modeling capabilities to support technical considerations and the identification of radiation related challenges for the extended storage of ASNF. Here, we report radiolytic H2 yields (G-values, G(H2)) from the gamma irradiation of ‘pristine’ and pre-corroded aluminum coupons in helium (He) environments as a function of alloy composition (AA1100 and AA6061), relative humidity, and absorbed gamma dose. Measured yields were lower than corresponding values reported for argon environments, a positive result for proposed extended dry storage strategies that would employ helium as a backfill gas. Interestingly, the presented G(H2)He values are comparable to those previously measured in nitrogen environments, suggesting a He mediated H2 inhibition process, attributed here to Penning ionization.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Milestone 2.7: Evaluation of Techniques for the Measurement of Molecular Hydrogen Gas in Helium Matrices

Published data by Task 2 (Oxyhydroxide Layer Radiolytic Gas Generation Resolution) for Technical Considerations and Challenges for Extended (>50 yrs) Dry Storage of Aluminum Cladded Spent Nuclear Fuel (ASNF), demonstrated that radiolytic molecular hydrogen (H2) production from gamma irradiated aluminum alloy 1100 (Al-1100) coupons exhibited significant dependence on backfill gaseous environment conditions: air, due to the presence of oxygen, completely inhibited H2 production; nitrogen promoted H2 production; and argon yielded more H2 than nitrogen environments. The concern here is that helium has been proposed as the backfill gas for extended storage and is more inert than argon, which may translate into significantly more H2 production than current Task 3 argon-based models predict. However, the measurement of H2 in helium media was not possible using the previously establish gas chromatography (GC) flame ionization detector, due to similarities in thermal conductivity. This milestone was initiated to evaluate an alternative GC approach that employed a mercuric oxide (HgO) reduction gas detector (RGD). Using the HgO RGD setup, H2 was successfully calibrated in the presence of a helium carrier gas, and then subsequently measured in control and irradiated crush-tube sample vials, consistent with previous sample measurements. Overall, the HgO RGD approach was found to be sufficient for future helium environment irradiations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Task 2 INL Updated Test Matrix and Updated Milestones

Test plan for FY20 work on ASNF work. Current Status and Proposed Test Matrix: Corrosion testing has been delayed due to iron contamination of corroded samples – investigations as to the source of this is underway and plans for mitigation for the next round in place. Completed pristine Al1100 coupon irradiations under argon and nitrogen atmospheres of various relative humidities were undertaken and reported in December 2019. This work contributed to Milestone 2.6 and Milestone 2.8. The agreed total absorbed doses for this work were 250, 500, 750, and 1000 kGy. However, the new proposed work to be undertaken at SRNL includes total doses of 50 and 100 kGy. Additional total gamma doses will also include pre-corroded samples, so thorough comparisons can be made. Samples in helium head spaces will be prioritized.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗