Impact of Corrosion Layer Composition and Thermal Pretreatment on the Radiolytic Generation of Molecular Hydrogen from Aluminum Alloys

To fully evaluate the feasibility of extending the dry storage of aluminum-clad spent nuclear fuel (ASNF) in helium-backfilled cannisters, the amount of radiation-induced molecular hydrogen (H2) generated and the impact of absorbed radiation dose on the ASNF corrosion layer composition must be accurately assessed. Here, we report a slowing in the rate of radiolytic H2 […]

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, […]

Radiation-Induced Chemical Yields of Carbon-Centered Radicals and Hydrogen Atoms from the Gamma Irradiation of n-Dodecane

This study investigates the radiolytic yields of carbon-centered radicals and hydrogen atoms in n-dodecane under gamma irradiation. Utilizing molecular iodine (I2) and 2,4,6-tri-tert-butylnitrosobenzene (3tBNB) as radical scavengers, we quantified the yields of molecular hydrogen and various carbon-centered radicals formed from bond scission of the solvent excited states. The yield of primary alkyl radicals was significantly […]

Gamma Radiation-Induced Degradation of Acetohydroxamic Acid (AHA) in Aqueous Nitrate and Nitric Acid Solutions Evaluated by Multiscale Modelling

Acetohydroxamic acid (AHA) has been proposed for inclusion in advanced, single-cycle, used nuclear fuel reprocessing solvent systems for the reduction and complexation of plutonium and neptunium ions. For this application, a detailed description of the degradation of AHA in dilute aqueous nitric acid is required. To this end, we present a comprehensive, multiscale computer model […]

Multiscale Modelling of the Radical-Induced Chemistry of Acetohydroxamic Acid in Aqueous Solution

Acetohydroxamic acid (AHA) is a small organic acid with a wide variety of industrial, biological, and pharmacological applications. The ability to predict and control the radical-induced behavior of AHA in these environments necessitates a deep fundamental molecular level understanding of the mechanisms responsible, and their interplay with other attendant chemical species, for example, the oxidative […]

Multiscale modelling of the radical-induced chemistry of acetohydroxamic acid in aqueous solution

Acetohydroxamic acid (AHA) is a small organic acid with a wide variety of industrial, biological, and pharmacological applications. A deep fundamental molecular level understanding of the mechanisms responsible for the radical-induced reactions of AHA in these environments is necessary to predict and control their behaviour and elucidate their interplay with other attendant chemical species, for […]

Milestone 1.2.14: Surface Characterization of Irradiated Surrogate Non-Native Corrosion Plumes on Aluminum 6061-T6 Specimens

The United States Department of Energy is seeking to evaluate the feasibility of extended dry storage of aluminum-clad spent nuclear fuel (ASNF) in helium-backfilled cannisters. A significant research effort has been devoted to determining the amount of radiation-induced molecular hydrogen generation from corrosion layers that would be present on the fuel assembly surfaces. However, to […]

Milestone 1.2.10: Steady-state H2 “roll over” point data for aluminum alloys 1100 and 6061

Extended (> 50 years) dry storage is being evaluated by the U.S. Department of Energy (DOE) for the disposition of ~ 18 metric tons of aluminum-clad spent nuclear fuel (ASNF). Transition of the current ASNF inventory into dry storage—using the standard DOE canister—necessitates a rigorous, predictive understanding of the long-term physical and chemical factors that […]

Milestone 1.2.11: H2 Production from Surrogate Non-Native Corrosion Plumes on Aluminum 6061-T6 Fuel Cladding Surrogates

Thick, localized, “non-native” corrosion plumes have been identified on Advanced Test Reactor fuel elements, raising concern on their impact on the radiolytic formation of molecular hydrogen gas (H2) from aluminum-clad spent nuclear fuel (ASNF) under proposed extended (> 50 years) dry storage conditions. Here, we report our findings on H2 generation from the gamma irradiation […]

Radiolytic Gas Production from Aluminum Coupons (Alloy 1100 and 6061) in Helium Environments—Assessing the Extended Storage of Aluminum Clad Spent Nuclear Fuel

Corrosion of aluminium alloy clad nuclear fuel, during reactor operation and under subsequent wet storage conditions, promotes the formation of aluminium hydroxide and oxyhydroxide layers. These hydrated mineral phases and the chemisorbed and physisorbed waters on their surfaces are susceptible to radiation-induced processes that yield molecular hydrogen gas (H2), which has the potential to complicate […]