Radiation-induced molecular hydrogen gas generation in the presence of aluminum alloy 1100

Parker-Quaife, Elizabeth; Verst, Christopher; Heathman, Colt R.; Zalupski, Peter R.; Horne, Gregory P

doi:10.1016/j.radphyschem.2020.109117

Cited by 18 publications

(46 citation statements)

References 38 publications

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“…Previous radiolysis studies performed under Task 2 established baseline estimates of H2 generation rates from the attendant hydrated oxides [3]. The results confirmed that net radiolytic H2 production has a dependency on absorbed gamma dose, as well as relative humidity and cover gas composition (air, nitrogen, and argon).…”

Section: Introductionsupporting

confidence: 64%

“…Boehmite was selected to complement radiolysis experiments conducted by INL in which lab-induced corrosion of aluminum coupons was performed in 95 °C water. This process took 29 days to produce a ~5 µm mixed oxide layer of predominantly bayerite favored by lower water temperatures [3]. Conversely, SRNL efforts focused on the high-temperature crystalline boehmite which is expected to be the dominant form of hydrated oxyhydroxide after undergoing most fuel drying processes, as the elevated temperatures employed would transition gibbsite or bayerite into boehmite [5].…”

Section: Srnl-sti-2021-00625mentioning

confidence: 99%

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Measurement of radiolytic hydrogen generation and impact of drying treatments on reactor exposed and surrogate aluminum materials

Verst

d’Entremont

2021

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Section: Introductionsupporting

confidence: 64%

Section: Srnl-sti-2021-00625mentioning

confidence: 99%

Measurement of radiolytic hydrogen generation and impact of drying treatments on reactor exposed and surrogate aluminum materials

Verst

d’Entremont

2021

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“…• Cover gas: E.g., recent work on radiolysis of physisorbed and chemisorbed water on aluminum coupons under air, N2, or argon cover gas [Parker-Quaife et al, 2019] observed significantly greater initial yield of H2 for argon compared to N2 and no detectable H2 under air (attributed to scavenging of free radicals by O2 in the air). Further comparisons of argon versus helium demonstrated that yields under helium were smaller than under argon, with the different response under the two noble gases attributed to He promoting Penning ionization and decomposition of H2 [Horne et al, 2021].…”

Section: Water Radiolysis and Hydrogen Generationmentioning

confidence: 99%

Measurement of radiolytic hydrogen generation from surrogate zr-based materials in a "mini-canister"

D'Entremont

VERST

Sindelar

2022

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This report describes a test campaign to investigate radiolytic hydrogen generation from surrogate materials resembling the (Zr-based) cladding of commercial spent nuclear fuel (SNF) with an inventory of residual water post-dryout. The radiolytic hydrogen generation rates from residual waters in the SNF-incanister system are important for predicting the in-canister environment for sealed SNF dry storage canisters over time and the impact to continued safe dry storage.Under gamma radiation, radiolytic breakdown of water remaining in a canister (free, physisorbed, or chemisorbed) causes the generation of hydrogen gas (H2). SNF assemblies, clad in zirconium alloys, provide a large surface area to host surface-adsorbed water (physisorbed water). Other components in the cask, including stainless steel and aluminum structural components and aluminum neutron absorbers, also contribute to the total water inventory and radiolytic H2 generation in an SNF canister.Water adsorbed to the ZrO2 on the cladding surface may experience accelerated radiolysis compared to free water due to energy exchange with the oxide. In addition, surface water decomposed by radiolysis may be replenished by water vapor in the canister gas, providing a mechanism for accelerated radiolysis of the free water as well. The previous simplified analysis [d'Entremont et al., 2020] predicted that radiolysis of physisorbed water on the Zr-alloy components would dominate the short-term H2 generation due to these factors. Therefore, the yield associated with water radiolysis on the Zr surfaces (physisorbed water, with potential replenishment from water vapor) is the focus of the current testing.The lab-scale testing is conducted on non-radioactive surrogates, namely assemblies of zirconium coupons, irradiated inside a miniature steel canister ("mini-canister") designed to allow intermittent, insitu sampling of the canister gas during irradiation. The mini-canister approach for irradiation with in-situ monitoring was used in recent and on-going studies [Verst and d'Entremont, 2021] to measure radiolytic hydrogen generation from aluminum SNF cladding surrogate materials. This proposed testing forms part of the overall materials performance evaluation of the commercial SNF-in-canister system and is part of the technical bases for their continued safe dry storage.The test plan draws on the previous radiolysis testing on aluminum as well as the previous analysis, "Evaluation of Hydrogen Generation in High Burnup Demonstration Dry Storage Cask" [d'Entremont et al., 2020], which provided a best-estimate evaluation of residual water content (post-dryout) in the High Burnup (HBU) LWR Spent Fuel Demonstration project TN-32 cask and evaluated the expected radiolysis of the residual water, including free, physisorbed, and chemisorbed water in the sealed cask, based on literature data and models.The experiments focus on the contribution associated with the Zr-alloy components, i.e., surface-adsorbed water as well as interactions with free water vapor present in the gas p...

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“…The key findings of the conducted work to close the associated technical gap are:  H2 generation can be directly attributed to the presence of corroded aluminum and adsorbed water, and the H2 yields are directly dependent on the absorbed gamma dose, relative humidity, and cover gas composition. 20,21 Further, H2 generation increases with the increasing availability of corrosion products. A positive correlation between the (oxy)hydroxide surface area and H2 generation is suspected, although it could not be confirmed empirically.…”

Section: Resolution Of Radiolytic Gas Generation Data For Asnfmentioning

confidence: 99%

Technical Basis for Extended Dry Storage of Aluminum-Clad Spent Nuclear Fuel

Eidelpes

Sindelar

Jarrell

2021

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The Department of Energy owns a large inventory (~14 MTHM or ~19,000 assemblies) of aluminum-clad spent nuclear fuel (ASNF) that is presently in interim storage, and continued, safe storage of ASNF must be provided over extended periods of time (>50 years) pending ultimate disposition. To support active reactor operations and ensure safe ASNF management practices, several research activities were initiated to formulate the technical basis for extended dry storage. Within the scope of these activities, technical understanding was developed to answer whether ASNF can remain in its existing (vented) dry storage and whether it can be placed in a system for sealed dry storage for extended periods. That is, the research presented in this report completes existing subject matter literature listed in DOE-ID/RPT-1575 "Aluminum-Clad Spent Nuclear Fuel: Technical Considerations and Challenges for Extended (>50 Years) Dry Storage." The activities were conducted under the sponsorship of the

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Radiation-induced molecular hydrogen gas generation in the presence of aluminum alloy 1100

Cited by 18 publications

References 38 publications

Measurement of radiolytic hydrogen generation and impact of drying treatments on reactor exposed and surrogate aluminum materials

Measurement of radiolytic hydrogen generation and impact of drying treatments on reactor exposed and surrogate aluminum materials

Measurement of radiolytic hydrogen generation from surrogate zr-based materials in a "mini-canister"

Technical Basis for Extended Dry Storage of Aluminum-Clad Spent Nuclear Fuel

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