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Irradiation-enhanced Interactions at UO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub>/Al Interfaces

journal contribution
posted on 2024-01-09, 20:48 authored by Stefania Dede, Khachatur V. Manukyan, Jordan M. Roach, Daniel Robertson, Peter. C. Burns, Ani Aprahamian
<p dir="ltr">Combustion synthesis is used to prepare thin UO<sub>2</sub> films on aluminum alloy substrates. This simple preparation method involves electrospraying <i>uranyl nitrate</i> + <i>acetylacetone</i> + <i>2-methoxyethanol</i> solution on the substrate, followed by a short annealing at 350 or 550 °C. The irradiation of films with a <sup>40</sup>Ar<sup>2+</sup> ion beam (energy of 1.7 MeV and fluences of 7.7 × 10<sup>16</sup> and 1.3 × 10<sup>17</sup> ions/cm<sup>2</sup>) is conducted to investigate irradiation-induced restructuring processes. High-resolution transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) investigations show that the annealing temperature significantly influences the crystallinity and stability of materials during irradiation. A small amount of Mg in the alloy substrate diffuses into the amorphous Al<sub>2</sub>O<sub>3</sub> interfacial layer between the film and the substrate. Local thermal spikes from the incoming ions facilitate the irradiation-induced mixing of immiscible Al<sub>2</sub>O<sub>3</sub> and UO<sub>2</sub> for the materials prepared at 350 °C. This mass diffusion produces relatively large cavities at the interface. Selective diffusion of a more significant amount of Mg for the materials prepared at 550 °C suppresses the mixing of the Al<sub>2</sub>O<sub>3</sub> interlayer with the film but forms Mg<sub><em>y</em></sub>U<sub>1–</sub><sub><em>y</em></sub>O<sub>2±x</sub> solid solutions during irradiation. Local thermal heating triggers the precipitation of a discontinuous crystalline MgO layer close to the film surface. The enhanced and selective diffusion of Mg into the film makes the materials prepared at 550 °C more robust and mechanically stable than those prepared at 350 °C.</p>

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J. Phys. Chem. C 2023, 127, 20, 9850–9857

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